Condensed Matter Nuclear Science: Proceedings of the 12th International Conference on Cold Fusion, Yokohama, Japan 27 November-2 December 2005

clondensed mlatter nluclear slcience

i to takahashi ken-ichiro ota yasuhiro iwamura

ondensed m otter n"uclear science proceedings of the 12th international conference on cold fusion

This page is intentionally left blank

ondensed m after n uclear cience proceedings of the 12th international conference on cold fusion

Yokohama, Japan 27 November - 2 December 2005

Editors

Akito Takahashi Osaka University, Japan

Ken-ichiro Ota Yokohama National University, Japan

Yasuhiro Iwamura Mitsubishi Heavy Industries, Japan

\[p World Scientific NEW JERSEY • LONDON

• SINGAPORE

• BEIJING

• SHANGHAI

• HONG KONG • T A I P E I •

CHENNAI

Published by World Scientific Publishing Co. Pte. Ltd. 5 Toh Tuck Link, Singapore 596224 USA office: 27 Warren Street, Suite 401-402, Hackensack, NJ 07601 UK office: 57 Shelton Street, Covent Garden, London WC2H 9HE

British Library Cataloguing-in-Publication Data A catalogue record for this book is available from the British Library.

CONDENSED MATTER NUCLEAR SCIENCE Proceedings of the Twelveth International Conference on Cold Fusion Copyright © 2006 by World Scientific Publishing Co. Pte. Ltd. All rights reserved. This book, or parts thereof, may not be reproduced in any form or by any means, electronic or mechanical, including photocopying, recording or any information storage and retrieval system now known or to be invented, without written permission from the Publisher.

For photocopying of material in this volume, please pay a copying fee through the Copyright Clearance Center, Inc., 222 Rosewood Drive, Danvers, MA 01923, USA. In this case permission to photocopy is not required from the publisher.

ISBN 981-256-901-4

Printed by Mainland Press Pte Ltd

PREFACE The study of Condensed Matter Nuclear Science (CMNS) has continued to advance through 11 past conferences (ICCF1 at Utah, USA in 1989 to ICCF11 at Marseilles, France in 2004) and many new compelling scientific findings are becoming known. The historical 1989 claim of "cold fusion" had renewed hope of a portable clean nuclear reactor. The subsequent great wave of denial and hostility forced the claim and further research efforts out of mainstream science. Nevertheless, due to misconceptions and misinformation, very few people know that several hundred researchers from around the world have continued this research during the past 16 years. The efforts by this faint stream of research have now revealed that there exist new kinds of nuclear effects directly related to the nature of condensed matter. The nuclear effects in condensed matter are much more than real "cold fusion"; they include important nuclear effects such as transmutations and resulting release of energy as significant heat with minimal and safe radiation. Low levels of radiation are found in at least some reactions, but are usually absorbed within the cell itself so the system is categorically safe. Through discussions at international conferences (ICCF1-ICCF11), a majority of researchers agreed that the name "cold fusion" was misleading. A new name, closer to the exact phenomenon, Condensed Matter Nuclear Science, is most appropriate. This emerging field, CMNS, treats nuclear effects in and/or on condensed matter, targeting its application for portable clean nuclear sources. This is an interand multi-disciplinary academic field, including nuclear physics, condensed matter physics, surface physics, and chemistry and electrochemistry. CMNS applications involve many other fields of science and technology (nuclear engineering, mechanical engineering, electrical engineering, laser science and engineering, material science, nano-technology, biotechnology, energy politics, etc. To promote the development of CMNS and establish the academic field of CMNS, the field needs highly efficient, cooperative efforts of researchers, and related people working in different fields. International linkage and collaborations are also needed. The full name of this conference is the 12th International Conference on Condensed Matter Nuclear Science. However, we decided to keep the acronym ICCF12 for the Conference, considering our original standpoint and tradition. The International Society for Condensed Matter Nuclear Science (ISCMNS) made a start in 2004 to promote the understanding, development and application of CMNS and has become a main supporting body of the ICCF series conferences till ICCF11. However, ICCF12 is sponsored by other societies like JCF (Japan-CF Research Society) and supported also by non-ISCMNS members. ICCF12 will provide an international scientific forum for direct interaction and stimulation among many scientists working in the CMNS field and participation and presentation of newcomers will be welcome. V

vi

The Conference site and date were: Shin-Yokohama Prince Hotel, Yokohamacity, Japan on 27 November-2 December 2005. The following topics were discussed in the conference: • • • • • • •

Excess Heat and Related Nuclear Products. Nuclear Processes and Transmutations. Materials and Condensed Matter Conditions. Analyses and Diagnoses Techniques. Innovative Approaches. Theories on Condensed Matter Nuclear Effects. Engineering, Industrial, Political, and Philosophical Issues.

For organizing and preparing ICCF12, the following members of LOC (Local Organizing Committee) and IAC (International Advisory Committee) have made contributions. Local Organizing Committee Akito Takahashi, Chairman, Osaka University, Japan. Ken-ichiro Ota, Co-chairman, Yokohama National University, Japan. Yasuhiro Iwamura, Co-chairman, Mitsubishi Heavy Industries, Japan. Shigenori Mitsushima, Secretary, Yokohama, National University, Japan. Shinya Narita, Secretary, Iwate University, Japan. Hiroshi Yamada, Iwate University, Japan. Tadahiko Mizuno, Hokkaido University, Japan. Akira Kitamura, Kobe University, Japan. Kazuaki Matsui, Institute of Applied Energy, Japan. Koichi Tomimura, The Thermal and Electric Energy Technology Foundation, Japan. International Advisory Committee Tullio Bressani, Department of di Fisica Sperimentale, Universita di Torino, Italy. Francesco Celani, INFN, Frascati, Italy. Antonella De Ninno, ENEA, Frascati, Italy. Peter Hagelstein, MIT, USA. Akito Takahashi, Osaka University, Japan. Ken-ichiro Ota, Department of Energy and Safety Engineering, Yokohama, National University, Japan. Jirohta Kasagi, Laboratory for Nuclear Science, Tohoku University, Japan. Yasuhiro Iwamura, Mitsubishi Heavy Industries, Japan. Xing Zhong Li, Tsinghua University, China. Andrei Lipson, Institute of Physical Chemistry, The Russian Academy of Sciences, Moscow, Russia.

vii

Michael McKubre, SRI International, USA. George Miley, Fusion Studies Laboratory, University of Illinois, USA. Nikolai Samsonenko, People Friendship University, Russia. Francesco Scaramuzzi, ENEA, Frascati (retired), Italy. Mahadeva Srinavasan, BARC (retired), India. Edmund Storms, Lattice Energy, LLC, USA. William Collis, ISCMNS. Jean Paul Biberian, University of Marseilles Luminy, France (Chairman, ICCFll). Yuri Bazhutov, Institute of Terrestrial Magnet, Russia (Chairman, ICCF13). Sponsors of ICCF12 ISCMNS: International Society for Condensed Matter Nuclear Science. TEET: Thermal and Electric Energy Technology Foundation. JCF: Japan CF-Research Society. All the full papers submitted for Proceedings book were peer-reviewed by the specialists from Japan. Revised drafts were edited, converted into LaTeX format and send to the publisher (World Scientific Publishing Co. Pte. Ltd., Singapore). For some of the presentations at the meeting of ICCF12, authors did not submit full papers and those papers are not included in the Proceedings book. Due to trivial mistake, a few papers submitted to ICCFll (Marseilles) Proceedings could not be included in the Proceedings of ICCFll (published by World Scientific Co, 2006). These missing papers by Dr. V. Violante group are included in the present book for compensation. Editors Akito Takahashi, Ken-ichiro Ota, and Yasuhiro Iwamura 30 June 2006

CONTENTS Preface

v 1. G E N E R A L

Progress in condensed matter nuclear science A. Takahashi

1

Summary of ICCF-12 X. Z. Li

26

Overview of light water/hydrogen-based low-energy nuclear reactions G. H. Miley and P. J. Shrestha

34

2. EXCESS HEAT A N D He D E T E C T I O N Development of "DS-reactor" as the practical reactor of "cold fusion" based on the "DS-cell" with "DS-cathode" Y. Arata and Y.-C. Zhang Progress in excess of power experiments with electrochemical loading of deuterium in palladium V. Violante, S. Moretti, M. Bertolotti, E. Castagna, C. Sibilia, F. Sarto, M. McKubre, F. Tanzella, I. Dardik, S. Lesin and T. Zilov

44

55

Anomalous energy generation during conventional electrolysis T. Mizuno and Y. Toriyabe

65

"Excess heat" induced by deuterium flux in palladium film B. Liu, X. Z. Li, Q. M. Wei, N. Mueller, P. Schoch and H. Oehre

75

Abnormal excess heat observed during Mizuno-type experiments J.-F. Fauvarque, P. P. Clauzon and G. J.-M. Lalleve

80

Seebeck envelope calorimetry with a Pd|D20 + H2SO4 electrolytic cell W.-S. Zhang, J. Dash and Q. Wang

86

Observation and investigation of nuclear fusion and self-induced electric discharges in liquids A. I. Koldamasov, H. I. Yang, D. B. McConnell, A. A. Kornilova, V. I. Vysotskii and A. V. Desyatov

97

Description of a sensitive seebeck calorimeter used for cold fusion studies E. Storms

108

Some recent results at ENEA M. Apicella, E. Castagna, L. Capobianco, L. D'Aulerio, G. Mazzitelli, F. Sarto, A. Rosada, E. Santoro, V. Violante, M. McKubre, F. Tanzella and C. Sibilia

117

Heat measurement during plasma electrolysis K. Iizumi, M. Fujii, S. Mitsushima, N. Kamiya and K.-I. Ota

133

Effect of an additive on thermal output during electrolysis of heavy water with a palladium cathode Q. Wang and J. Dash

140

Thermal analysis of calorimetric systems L. D'Aulerio, V. Violante, E. Castagna, R. Fiore, L. Capobianco, PR. Del Prete, F. Tanzella and M. McKubre

145

Surface plasmons and low-energy nuclear reactions triggering E. Castagna, C. Sibilia, S. Paoloni, V. Violante and F. Sarto

156

Production method for violent TCB jet plasma from cavity F. Amini

163

New results and an ongoing excess heat controversy L. Kowalski, G. Luce, S. Little and R. Slaughter

171

3. T R A N S M U T A T I O N Observation of surface distribution of products by X-ray fluorescence spectrometry during Z>2 gas permeation through Pd Complexes Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada and T. Lshikawa Discharge experiment using P d / C a O / P d multi-layered cathode S. Narita, H. Yamada, D. Takahashi, Y. Wagatsuma, S. Taniguchi and M. Itagaki Producing transmutation element on multi-layered Pd sample by deuterium permeation H. Yamada, S. Narita, S. Taniguchi, T. Ushirozawa, S. Kurihara, M. Higashizawa, H. Sawada, M. Itagaki and T. Odashima

178

188

196

Experimental observation and combined investigation of high-performance fusion of iron-region isotopes in optimal growing microbiological associations V. I. Vysotskii, A. A. Kornilova, A. B. Tashirev and J. Kornilova Research into low-energy nuclear reactions in cathode sample solid with production of excess heat, stable and radioactive impurity nuclides A. B. Karabut

206

214

Influence of parameters of the glow discharge on change of structure and the isotope composition of the cathode materials /. B. Savvatimova and D. V. Gavritenkov

231

Elemental analysis of palladium electrodes after P d / P d light water critical electrolysis Y. Toriyabe, T. Mizuno, T. Ohmori and Y. Aoki

253

Progress on the study of isotopic composition in metallic thin films undergone to electrochemical loading of hydrogen M. Apicella, V. Violante, F. Sarto, A. Rosada, E. Santoro, E. Castagna, C. Sibilia, M. McKubre, F. Tanzella and G. Hubler In situ accelerator analyses of palladium complex under deuterium permeation A. Kitamura, R. Nishio, H. Iwai, R. Satoh, A. Taniike and Y. Furuyama High-resolution mass spectrum for deuterium (hydrogen) gas permeating palladium film Q. M. Wei, X. Z. Li, B. Liu, N. Mueller, P. Schoch and H. Oehre ICP-MS analysis of electrodes and electrolytes after HNO3/H2O electrolysis S. Taniguchi, S. Shimadu, H. Yamada, S. Narita, T. Odashima, N. Teshima and T. Ohmori The Italy-Japan project — Fundamental research on cold transmutation process for treatment of nuclear wastes A. Takahashi, F. Celani and Y. Iwamura

264

272

278

284

289

4. N U C L E A R PHYSICS A P P R O A C H Reproducible nuclear emissions from Pd/PdO:Dx heterostructure during controlled exothermic deuterium desorption A. G. Lipson, G. H. Miley, A. S. Roussetski, B. F. Lyakhov and E. I. Saunin Correct identification of energetic alpha and proton tracks in experiments on CR-39 charged particle detection during hydrogen desorption from Pd/PdChH^ heterostructure A. S. Roussetski, A. G. Lipson, B. F. Lyakhov and E. I. Saunin

293

304

Intense non-linear soft X-ray emission from a hydride target during pulsed D bombardment G. H. Miley, Y. Yang, A. Lipson, M. Haque, I. Percel and M. Romer

314

Enhancement of first wall damage in ITER type TOKAMAK due to LENR effects A. G. Lipson, G. H. Miley and H. Momota

325

Generation of DD-reactions in a ferroelectric KD2PO4 single crystal during transition through curie point (Tc = 220 K) A. G. Lipson, G. H. Miley, A. S. Roussetski and E. I. Saunin

336

Study of energetic and temporal characteristics of X-ray emission from solid-state cathode medium of high-current glow discharge A. B. Karabut

344

A novel LiF-based detector for X-ray imaging in hydrogen loaded Ni films under laser irradiation R. M. Montereali, S. Almaviva, T. Marolo, M. A. Vincenti, F. Sarto, C. Sibilia, E. Castagna and V. Violante Observation and modeling of the ordered motion of hypothetical magnetically charged particles on the multilayer surface and the problem of low-energy fusion S. V. Adamenko and V. I. Vysotskii

351

356

5. MATERIAL SCIENCE Evidence of superstoichiometric H/D lenr active sites and high-temperature superconductivity in a hydrogen-cycled Pd/PdO A. G. Lipson, C. H. Castano, G. H. Miley, B. F. Lyakhov, A. Yu. Tsivadze and A. V. Mitin

367

New procedures to make active, fractal-like surfaces on thin Pd wires F. Celani, A. Spallone, E. Righi, G. Trenta, G. D'Agostaro, P. Querela, V. Andreassi, 0. Giacinti, P. Marini, V. Di Stefano, M. Nakamura, F. Todarello, E. Purchi, A. Mancini, P. G. Sona, F. Fontana, L. Gamberale, D. Garbelli, E. Celia, F. Falcioni, M. Marchesini, E. Novaro and U. Mastromatteo

377

Using resistivity to measure H/Pd and D/Pd loading: Method and significance M. C. H. McKubre and F. L. Tanzella

392

Measurements of the temperature coefficient of electric resistivity of hydrogen overloaded Pd A. Spallone, F. Celani, P. Marini and V. Di Stefano

404

Magnetic interaction of hypothetical particles moving beneath the electrode/electrolyte interface to elucidate evolution mechanism of vortex appeared on Pd surface after long-term evolution of deuterium in 0.1 m LiOD H. Numata and M. Ban Unusual structures on the material surfaces irradiated by low-energy ions B. Rodionov and I. Savvatimova

411

421

6. THEORY Context for understanding why particular nanoscale crystals turn-on faster and other LENR effects S. R. Chubb

430

Models for anomalies in condensed matter deuterides P. L. Hagelstein

441

Time-dependent EQPET analysis of TSC A. Takahashi

454

Unifying theory of low-energy nuclear reaction and transmutation processes in deuterated/hydrogenated metals, acoustic cavitation, glow discharge, and deuteron beam experiments Y. E. Kim and A. L. Zubarev

462

Catalytic fusion and the interface between insulators and transition metals T. A. Chubb

473

Multiple scattering of deuterium wave function near surface of palladium lattice X. Z. Li, Q. M. Wei, B. Liu, N. N. Cai, S. X. Zheng and D. X. Cao

482

Theoretical comparison between semi-classical and quantum tunneling effect F. Frisone

494

New cooperative mechanisms of low-energy nuclear reactions using super low-energy external field F. A. Gareev and I. E. Zhidkova

504

Polyneutron theory of transmutation J. C Fisher The thermal conduction from the centers of the nuclear reactions in solids K.-I. Tsuchiya Four-body RST general nuclear wavefunctions and matrix elements /. Chaudhary and P. L. Hagelstein

516

521

527

Study on formation of tetrahedral or octahedral symmetric condensation by hopping of alkali or alkaline-earth metal ion H. Miura

536

Calculations of nuclear reactions probability in a crystal lattice of lanthanum deuteride V. A. Kirkinskii and Yu. A. Novikov

542

Possible coupled electron and electron neutrino in nucleus and its physical catalysis effect on D-D cold fusion into helium in Pd M. Fukuhara

547

Tunnel resonance of electron wave and force of fluctuation M. Ban

555

Types of nuclear fusion in solids N. Yabuuchi

564

XV

Neutrino-dineutron reactions (low-energy nuclear reactions induced by D2 gas permeation through Pd complexes — Y. Iwamura effect) V. Muromtsev, V. Platonov and I. Savvatimova

571

An explanation of earthquakes by the blacklight process and hydrogen fusion H. Yamamoto

577

Theoretical modeling of electron flow action on probability of nuclear fusion of deuterons A. I. Goncharov and V. A. Kirkinskii

582

Author Index

589

This page is intentionally left blank

P R O G R E S S IN C O N D E N S E D M A T T E R N U C L E A R SCIENCE

A K I T O TAKAHASfflt Osaka

University,

Yamadaoka E-mail:

2-1, Suita, Osaka 565-0871, [email protected]

Japan

Recent studies of condensed matter nuclear science (CMNS) including cold fusion have accumulated some convincing data and theoretical modeling, and we are about to conclude that (1) deuteron-related clean fusion reactions and (2) cold and special transmutations may take place in the environment of condensed matter containing deuterons and protons. This emerging field of CMNS is expected to give us strong impact on the future of basic sciences for energy-application, fundamental nuclear science, and condensed matter sciences.

1. Introduction Condensed matter nuclear science (CMNS) was born as a descendant research field of Cold Fusion. In March 1989, S. Pons and M. Fleischmann at University of Utah announced "cold fusion" by D 2 0 / P d electrolysis in test tube. The experimental system looked very simple. So many people in the world were involved in hurried trials of replication-experiments. In most trials, however, huge excess heat as claimed by Pons-Fleischmann was not observed. Parallel replication trials for the Nature paper by S. Jones on weak 2.45 MeV DD neutron emission from D20/Ti electrolysis cell were not either successful. Very negative mood was seen in almost all scientific communities in the world. 1 In 1990-1992, some hopeful data on excess heat in D 2 0 / P d cells were reported from research teams in USA, Japan, and Italy. Although reproducibility was yet to be attained, great expectation was come back for the clean energy application based on "new nuclear energy process". In Japan, the New Hydrogen Energy (NHE) project was implemented in 1994-1998, at Shin-Sapporo Laboratory, where about 20 researchers from major Japanese industries and several foreign scientists worked together to verify the excess heat effect in Fleischmann-Pons type systems. The NHE effort was concentrated in D/H absorption data in metal-samples and excess heat detection. In spite of energetic efforts by the NHE team, they made final report that excess heat effect was not confirmed. Few positive data on excess heat from foreign researchers and some positive data on nuclear products from Japanese University teams were unfortunately not meaningfully evaluated by the NHE evaluation committee. The NHE project was terminated in 1998. tSubmitted for keynote paper in ICCF12, November 2005. 1

2

In 1999, Japan CF-Research Society (JCF) was founded for minimumsupporting of research activities in Japan. JCF meetings (JCF1-6) held annually have provided opportunities of exchanging hottest results and accumulating reports in its Proceedings. A faint but steady stream of CF researches has continued in the world after 1990. ICCF-series conferences have counted 11 meetings (ICCF1-ICCF11). The last ICCF conference (ICCF11) was held in Marseilles, November 2004. Other smaller international meetings have been held as Asti-series workshops, Russian cold transmutation conferences, sessions at ANS and APS, and so on. It is thought with rough statistics that about 300 researchers in the world have been continuing CMNS/CF studies. Accumulated research reports are piling up high, as published in ICCF Proceedings, 2-4 Asti-Proceedings, 5,6 and so on. Unfortunately, publication of papers on CMNS/CF works has been rejected by many of highly ranked magazines and journals as Nature, Science and Physical Review Letters, but many peer-reviewed papers have been published in Fusion Technology, Japanese J. Applied Physics (JJAP), Physics Letters A, J. Electro-analytical Chemistry, II Nuovo Cimento, and so on. In the end of 2003, re-evaluation of CF works was done by US DoE, 8 based on the report by Hagelstein et al.7 The DoE report concluded that excess heat effect was not confirmed although the continuation of research was necessary. Latest progress by research reports in 2001-2005 takes over the summary report, 7 and convincing results are given for concluding the existence of excess heat effect with 4 He generation and selected nuclear transmutations. In March 2004, CMNS/CF researchers have at last founded the International Society for Condensed Matter Nuclear Science (ISCMNS) registered in England. This is the first international society for CMNS/CF researchers, which will play a role as host society of international meetings as ICCF and Asti-series workshops and exchange information through its web-site http://www.iscmns.org/ for ISCMNS members and related people. The sustainable development is now widely regarded to be a way of human beings in the 21st century. To solve the energy problem, the idea of best mixing of various available energy sources may be a compromised solution. To mitigate the pollution of environment, cleaner energy resources are being looked for. Solar energy and windmills can merely cover a small portion of energy needs. Extension of nuclear power plants is on the dead lock due to accidents and expensive processing of wastes. Development of thermo-nuclear fusion reactors is also on the dead lock due to the monstrous expensive machine. Some (and probably many) people are seriously dreaming the realization of portably small clean power sources based on some new principles, especially the idea of clean and small-scale source of nuclear energy which can be distributed in private houses and with vehicles (see Slide 1). The emerging field of CMNS including cold fusion is therefore of great potential importance.

3

Energy is key for sustainable development of world Oil: 50-60 years (COa global warning) Solar-E, wind: ca. 10% of E-needs is limit U (235) fission: 50-60 years for LWRs FBR (Pu): ca. 500 years or more (Rapid development of China and India) (Problem in remediation of nuclear wastes) DT fusion: not available PRs in 50 years Distrlbuted-type clean nuclear energy devices are ideal

Slide 1 Slide 2 shows the known fusion reactions by hydrogen isotopes. DD reaction was originally considered as fundamental reaction in cold fusion, but claimed experimental results have revealed that condensed matter nuclear effects (CMNE) are quite different.

Fusion reactions are E-source in universe H + H

D + p+ + y : weak interaction, star

H + D

3

He + y + 5 . 5 MeV:star

D+ D

4

He + y + 2 3 . 8 M e V ; 1 C r 5 %

p + t + 4.02MeV;50%

•

D+T

n + 3 He + 3.25 MeV; 50% n + 4 He + 17.6 MeV: hot fusion

D + Li, P + Li, P + B, etc.

Slide 2 An amount of 1 W excess power by DD reaction corresponds to 10 12 f/s reaction rate. Therefore, if excess heat by CMNS experiments were by DD reactions, experimenters should have died 1 by high dose irradiation of 2.45 MeV neutrons. On the contrary, we could have found only very weak level of neutrons in CF experiments. 2-4 We have had to consider new class of nuclear reactions, probably

4

related to deuterons, in the environment of condensed matter. Some of theoretical models recently developed have proposed mechanisms to produce cleanly 4 He main ash and selected transmutations in metal-D/H systems as discussed later in this report. In frontiers of science pursuing new phenomena, combined actions between Experimentalism, Rationalism, and Skepticism should support the progress. Aspects to application of the phenomena are also important. 1. Experimentalism: The effect should be reproducible with same conditions, qualitatively and quantitatively. Qualitative repeatability of phenomena by other methods and/or other groups is "broadened" reproducibility; the phenomenon with excess heat with 4 He production has cleared this criterion. To be perfect, quantitative reproducibility is required: The technological application is only possible by clearing this criterion. 2. Rationalism: Theoretical models should be created with original ideas. New theories should be compatible to established theories and should be selfconsistent within own theoretical model. All contradictions should be cleared. 3. Skepticism: Defects and contradictions in experiments should be attacked. Mutual consistency between experimental results, new models and established theories should be checked to find contradictions. 4. Applicability: Feasibility for R&D to distributed clean nuclear energy devices should be critically discussed. Remediation of radioactive wastes from nuclear plants should be also discussed. Most essential consequences of latest CMNS studies may be summarized into the following three items: 1. Occurrence of deuteron-related clean fusion producing excess heat and 4 He. 2. Occurrence of selective transmutations of host metal nuclei and fission-like foreign elements. 3. New theoretical models to interpret qualitatively and quantitatively above results. Major experimental results and representative authors are summarized in Slide 3. Major results after 1998 are considered in Slide 3. Items (1) and (2) are independent of known DD reaction and should be new kind of nuclear reactions, but items (3) and (4) are closely related to the occurrence of cold fusion phenomena. 2. Generation of Excess Heat and 4 H e in Metal-D Systems Processed metal (mostly Pd) test samples with nano-technology have recently been used for heavy-water electrolysis, D2-gas permeation and gas-discharge experiments. Experiments with heavy water are no longer simple test tube-type, but various kinds of stimulation techniques have been tried as slow and fast pulsed electrolysis-current supply, ultra-sonic wave supply, laser-beam supply, plasma-mode-electrolysis, and so on.

5

Major experiments (green; after 2001)

1) Excess heat with He-4 Miles,

, McKubre, Gozzi, Isobe, , and so on , Mizuno, Miley, Ohmori, , and so on

3) Weak neutron emission , Takahashi, Mizuno, and so on

4) Anomalous DD enhancement , Takahashi, Huke, and so on Slide 3 The nano-modification of sample, especially surface modification is of current trend of experimental innovations as well as nano-particles, complex multi-layers, micron-size long wires, and so on. Positive and convincing data have been reported from Israel + SRI + ENEA group, 9 ' 10 Arata, 1 1 - 1 5 McKubre, 16,17 de Ninno, Celani, NRL-San-Diego, Li, Case, Cravens, Isobe, 18 and so on. Key issues in experiments are calorimetry, massanalysis, nano-size-condition of sample, stimulation and triggering, diagnostics, and detection. El Boher et al.9'10 have reported clear excess heat data with 25 times out put lasting long time (17 h typically) using super-wave electrolysis (see Fig. 1). They processed surfaces of sample Pd-cathodes by argon or hydrogen plasma etching. Photograph images by SEM showed finer grain sizes for argon plasma etching. They suggest condition of surface processing relating to success of excess heat. Superwave for ultrasonic wave was modulated with special wave forms programmed by computer (PC). Averaged frequency was about 20 kHz. Arata and George are doing irradiation of ultrasonic waves to Pd samples in heavy water, with simple sinusoidal function of about 20 kHz. It is interesting how the highly fractal wave form by El Boher et al. may effect on dynamic behavior of deuterons in PdDx lattice systems. One of their collaborators is asserting that superposition of superwaves in microscopic limit can induce microscopic ordering of condensed matter and bio-systems and induce nuclear reactions. Effect on ordering in atomic or molecular size level should be interesting, but phonon or electromagnetic wave should not so easily induce directly nuclear reactions.

In series of their experiments they reported large excess power reaching more than 10 times of input power for time-spans of more than several hours. Reproducibility is in 20-30%. Best data are shown in Fig. 1, where 20 W averaged output with 0.74 W input lasted for 17 h. Gain was 25! This excess power level is corresponding to 24.8 keV per Pd-atom-in-lattice, and is far greater (more than 1000 times) than chemical heat source level.

Excess power; Exp. #84a; EI-Boher, ICCF11 fc.aai^iassafai!j.m

PBB l»1

-mi 0/00:00:00

TM>3

.000

a-Jr:

W>i

JS>5 I

Tub 6 » 7 0/09:58:40

„

•

THUS

.

Ware

17

HF

" f «•?«» !'" 0/19:57:21

H

»•« COPE = (Pout-Pinet): Pim - (20-0.74):0.74 » 25 34,000 32,000

Average PouS -20 W

26,000 24,000

j

I

,

^

ft K.

22,000 £20,000

w.

118,000 ^ 16,000 14,000

\r*\'

6,000 4,000

Average P inet -0.74 W

2,000 llfcliilliHiTt lit

0,000 f

<m WyfliWOfc^

t u l i l i f t ' i U i M l 11 iin UK i m i ^ '

;

Mil liW HI

*: ••- j 4 f ] 5000

10000 15000 20000 25000 30000 35000 40000 45000 50000 55000 00000 S5000

71S24 *

Excess power up to 34 W; average -20 W for 17 h Figure 1.

Best output-power data obtained by El Boher et al.

This group is trying superposed stimulation with laser beam and ultrasonic wave. This is interesting trial. The group has obtained data for 4 He production in correlation with excess heat generation. An example of data is shown in Fig. 2. When we irradiate laser on surface of Pd cathode, we can choose laser wavelength in ultraviolet and EUV region due to the classical Drude formula for frequency dependence of dielectric constant of metal. They used He-Ne laser (632 nm wavelength). Also they observed increase of excess power of several times of laser input power (33 mW). On the right-hand side figure of Fig. 2, time-dependent data of relative resistance ratio of PdDx are drawn. During the laser irradiation and excess power episode, D/Pd ratio kept more than 0.9. However, continuation of laser irradiation induced no excess power and decrease of D/Pd ratio (increase of resistance ratio). This is very interesting data showing relation between excess power and D/Pd ratio under laser stimulation. Arata et al.11^15 have made significant contribution to provide clear experimental data of 4 He production from their own double structure cathode of Pd in heavy water electrolysis cell and from D-gas-phase absorption system of Pd nano-particles

7

under laser or ultrasonic wave irradiation. Their 4 He analysis by QMAS is reliable. Detection of neutron emission was tried in-situ, but could not observe meaningful events. Tritium production in electrolyte liquid was checked periodically for sampled heavy-water by LSC to observe no significant increase of tritium level compared with BG sample. They observed great amount of 4 He from Pd powder by heating. Arata et al. also tried laser irradiation experiment on Pd nano-particles (5 nm in diameter) in ZrO substrate, and observed clear 4 He generation. 11,15 This experiment gave important hint to theoretical modeling 57 of CMNE in finite size PdDx lattice system. Violante: SIENA 2005

3.4 kJ of produced energy: 2.5 MJ/mol Pd 632 nm (He Ne), 33 mW Laser-off

Excess of power under laser triggering

Loading evolution

(laser off effect). Hi-Lo current mode

(normalized resistance)

Figure 2. Excess power data triggered by laser (left figure) and variation of resistance ratios (right figure), after Violante et al.

McKubre et al. in S R I 1 9 - 2 1 have made great efforts in replicating experiments by Arata and Case. 19 They were also involved in their own systems of closedtype heavy-water/Pd electrolysis to detect excess power and 4 He and their mutual correlation. Data shown in Fig. 3 were taken in Case-type cell, which employed PVC-deposited Pd layer on carbon. Produced 4 He goes out partially into gas-phase of cell, and other portion will be remained in Pd cathode. They collected both components and made He analysis. They obtained correlation data as 31 MeV per He-atom with 13 MeV error bar. This is important data indicating that ash of excess heat events was 4He-nuclei. George et al.23 have been studying the effect of excess heat with 4 He production using the ultra-sonic wave irradiation into Pd-plate in heavy-water, and reported

8

that the effect is real. It was observed that Pd-plate was destroyed into small powders during the experiment. Stringham 24 has been studying the similar method with higher frequency (in MHz range) ultrasonic wave. We have other reports on 4 He production by de Ninno, Isobe, 18 and so on. We can say that the phenomenon of excess heat with 4 He generation is "qualitatively" reproducible. However, conditions for 100% reproducible protocols are yet to be established. To find quantitatively reproducible conditions, we need investigations on nanomodification of samples, procedures to keep high D/Pd ratios and dynamic D-flux through samples and external stimulation methods (electrolysis patterns, laser and ultra-sonic wave irradiations, and so on).

150 Gradient

)'=18.36X

it = 0,99 Differential

y = 18.36x f? = 0.99

100

4=

Gradient Q = 31 ± 13 MeV/atom Differential 0= 32 ± 13 MeV/atom ! ^-'

50

0 <3^H ^—

0

2

3

4

5

6

Helium increase (ppmV/V)

Figure 3.

Case: "Q"-value-energy versus 4 He (after M. McKubre, ICCF11, 2004).

Many researchers have been asserting the working hypothesis: D + D ->• 4 He + Lattice-energy (23.8 MeV).

(1)

However, this hypothesis has no support from nuclear physics theory as we discuss in the theory section. 3. Nuclear Transmutations in Metal-D Systems Reports claiming nuclear transmutations in CF experiments using metal-D systems have gradually increased 2-4 since around 1992. People have looked the claims of transmutations with doubtful views since transmutation should overcome very high Coulomb repulsion of two-body nuclear interactions and even cold DD reaction with milder Coulomb repulsion condition looks impossible. Nevertheless, from the latest experimental results, we have to take seriously the case of "special kinds of nuclear transmutations in the environment of condensed matter of metal-D systems".

9

Major reports 2 " 6 are from Iwamura, Mizuno, Celani, Yamada, Karabut, Violante, Miley, Mastromatteo, Savvatimova, Passel, Szpak, and so on. Key issues in experiments are mass-analysis, isotopic-ratio analysis, spectroscopic detection of particles (including X-rays and gamma-rays), nano-modification of samples, and external stimulation (or triggering). Most remarkable and reproducible transmutation experiments have been reported by MHI Iwamura group. 2 5 " 2 9 They are using Pd-complex samples which have multi-layered structure of about 100 nm surface Pd layer and following four layers of alternative CaO/Pd composition (see Fig. 4) on 0.1 mm thick Pd substrate plate. They put small amount of test elements (Cs or Sr) on surface. They set a sample in a chamber filled with 1-atom D2 gas and evacuate the volume rear sample plate. D-atoms permeate through sample by keeping permeation rate higher than 1 seem. They have made in situ analyses of surface elements by Xray-induced Photoelectron Spectroscopy (XPS) or X-ray Fluorescence Spectroscopy (XFS). Amazingly, they observed transmutations of 133 Cs -^ 1 4 1 Pr, 88 Sr -^ 96 Mo for the cases of D-permeation, but did not at all for H-permeation.

Cross section of Pd complex D permeation Cs, Ba, etc.

i..rT-"-;>T j.

Dflux Vacuum

Figure 4.

D2 gas permeation through the Pd complex.

The claimed transmutation channel is strangely selective as M{A, Z) + 4D (or 2 4 He) -> M(A + 8,Z + 4) + Q.

(2)

People have checked if there are misunderstandings in experimental procedure, contamination of impurity elements, mistakes in element and mass analyses, and others to find nothing wrong as far as they have checked through. People have started to take this result of "selective transmutation" seriously. Takahashi-group of Osaka University tried replication 30 of Iwamura experiments to result in observation of Pr production from Cs, three times out of three runs. Iwamura group has been doing separate series of experiments at Spring8 setting

10

up new chamber with incidence of strong SOR X-ray beam to make in situ FXS analysis of surface elements of Pd-complex under D-permeation. They have repeatedly observed transmutation from 133 Cs to 1 4 1 Pr (see Fig. 5). They have made sample analysis after experiments by Time-of-Flight Secondary Ionization Mass Spectroscopy (TOF-SIMS) to find that transmuted Pr distributed within about 10 nm depth from surface of Pd-complex sample (see Fig. 6). The data in Fig. 6 give insight that the transmutation reaction should have taken place in near surface region.

.....a...... 35 Cs-U;,

™, # ™>36

Iw—s* Br ^.4

Cs-L p1

1

•

4

;

T ,if

I

•

100-

1m -A

i' i

. ^

•,

i

• • i

1

' !-\

i

' V

Cs Lp2

'i*

J

50-

Energy (keV) Figure 5.

An experiment of Pr detection by the experiments at Spring-8 (Imaura, ICCF11).

To explain theoretically the surprising selective transmutation, Takahashi is developing the EQPET/TSC model of bosonized condensates of deuteron clusters under ordered dynamics of PdDx lattice, and T. Chubb-S. Chubb are proposing coherent reaction models by ion-band state of Bloch wave functions of many deuterons in lattice, as we will discuss in Section 5. When this transmutation process also takes place for radio-isotopes as 137 Cs and 90 Sr, the principle can provide a new way for remediation of nuclear wastes. Observations of anomalous production of foreign elements in D 2 0 / P d and Pd/Dgas systems have been reported by Mizuno, Ohmori, Karabut, Szpak 105 and so on. In these cases, they observed also excess heat events. Observed foreign elements are very common among these reports, namely Si, S, Ca, Ti, Cr, Mn, Fe, Cu, Zn, etc. Mizuno 31 reports that production rates of foreign elements were drastically small (several orders of magnitude) when excess heat evolutions were not observed. If these foreign elements, which were distributed in a wide range of mass and atomic number, were generated by some nuclear reaction, some fission process of host metal nuclei should be attributed to the reaction.

11

200

0

400

600

1000

800

Sputtering time (s) Figure 6.

Depth profile of Cs and Pr by TOF-SIMS (Iwamura, ICCF11).

Takahshi et a/. 32-34 have proposed a deterministic fission theory [Selective Channel Scission (SCS) model] based on rotating liquid drop model of excited nucleus. They checked the model successfully for calculating mass and atomic number distributions of fission products (FP) by 2 3 5 U+n fission process 33 to be compared with experimental data. Then they applied the model for predicting FP distributions of lower mass nuclei of A < 200. Mizuno's foreign element data are compared with Takahashi calculation in Fig. 7. Theoretically predicted element distribution looks similar to Mizuno experiment. In the SCS process, isotopic ratios of FP element become very different from natural abundances. For example, 57 Fe exists with 0.3% in natural iron, but both of FP of SCS theory and experiments by Mizuno gave similar values of about 10% in FP iron

« Fission products by theory {MPIF, Takahashi et al.) » Mizuno Exp, by D2Q-Pd/etectrolysis

100

Pd-natural LB-1

.MPIF • MIZUNO-EXP

10

1 t

Sr

0.1

0

5

10

15

20

25

30

35

40

45

50

Atomic number Figure 7. Foreign atom distribution obtained by Mizuno's D2O electrolysis, compared with theoretical prediction of Pd-fission products calculated by SCS theory by Takahashi et al.

12

isotopes. These agreements are quite interesting, and further studies are expected to verify if the phenomenon is really nuclear fission process for lighter nuclei in the environment of metal-D systems. Similar results have been reported for Ni-H systems as discuss below. The SCS theory predicts that fission products for A < 200 nuclei become very much cleaner (less radio-active and very small neutron emission) due to predominant production of stable isotopes. 3 2 - 3 4 4. Metal—Hydrogen Systems Observation of anomalous production of foreign elements and excess heat in metalordinary-water/H systems have been claimed 2 " 6 in reports by Piantelli, Ohmori, Miley, Yamada, Romadanov, Dash, Li, Mizuno, and so on. Key issues of experiments are again calorimetry, mass and isotopic analyses, radiation detection, sample fabrication, and triggering and stimulation techniques. Piantelli et al.36'37oi Siena University has been doing a H-gas absorption and diffusion type experiments using cylindrical Ni samples in chamber with heating device. They have made claim of large excess heat and gamma-ray emission with production of foreign elements. Figure 8 shows one of their typical data for observation of gamma-ray emission. They set up a standard 137 Cs gamma-ray (661 keV peak) source for calibration. The observed peak at around 744 keV is a surprise, which they say the gammaline from Mn isotope. A theoretical prediction by Takahashi's 4p/TSC-induced fission35interpret that 52 Mn and 56 Ni as FPs of Ni + 4p fission process can be sources of 744 keV line. It is well known that Miley-Patterson 38 reported distributed production of transmuted elements and excess heat in their Ni-ordinary-water electrolysis experiments.

Piantelli; SIENA 2005

Photo emission Cell with cylindrical smples

Cs source 661 keV

TARATURAconCs-137

Comment by A. T. 400.00 Mn (EC) (90%) 744.2 keV y 200.00 Ni-fl-4p-> C + "Fs(EC)"Mn(ECi"cr(EC) 0.00

1

0.00

Figure 8.

1 200.00

'

1 400.00

'

1 600-00

'

1 Canal! 800.00

Gamma-ray spectrum obtained in Ni-H-gas experiment by Piantelli et al.

13

Data from Miley'96 t

1 t.

<

i

»NA»

<

1 1 2

-

Atomic number

S

5 10 15 20 25 30 35 40 45 50

Yield (%)

1

, >

Ni + 4p/TSC to fission

3

10

calculated by selective channel fission model

Figure 9.

20

30

40

50

Atomic number

F P elements by SCS versus Miley experiment

(G. Miley and J. Patterson J. New

Energy, 1996, 1, p. 5).

Specially nano-fabricated multi-layered test samples were used in these experiments. Dominant foreign elements observed are compared with the SCS prediction for Ni + 4p/TSC fission process, 3 ' 39 in Fig. 9. Agreement has to be said surprising. For two peaks near at atomic number 25 and 15, we see almost same distributions. The third peak including C and O in theory is considered to be difficult to identify in experiments due to contaminants. Predominant fission products from Ni + 4p fission come from 60 Ni + 4p, and contribution of 58 Ni is very small. And FPs are almost stable isotopes (Slide 4).

Major fission channels from Ni + 4p (1) °°Ni (68%) + 4p -> ° Ge (Ex = 11.2 MeV) * 8.8 MeV -t • 8.8 MeV +

58

(3) °'Ni (1.1%) + 4p -» 0 0 Ge (Ex = 21.3 MeV)

s8

61 81 -»18.9MeV + • + Zn (EC) Cu (EC) + 68 Fe(EC) 68 Mn(3.7x10 8 y) ^15.9 MeV+

t- Zn (EC) Cu (EC) v M Ar (EC) MCI (EC)

4! ^11.0 MeV + ! + Ti (EC) 37 —17.4 MeV + • + Ar(EC)

!(2) °°Ni (26.2%) + 4p - * " G e (Ex = 19.1 MeV) - . 16.4 MeV + He + 80Zn (EC) 60Cu (EC) - t 13.6 MeV + "Be + "TN|I (EC) 56Co (EC) ; - . 13.0 MeV + 12C + 52Fe (EC) MMn (EC) ' . 48 48 -»12.2 MeV + " 0 + Cr (EC) V (EC) -»13.5 MeV + + ^ 1 6 . 4 MeV + + -.16.7 MeV + + -.6.5 MeV + + 26 Sl(EC)AI(10 5 y)

!7 -,12.0 MeV + Si(EC)

..

+ •

-*17.5MeV +

Note:

• Average kinetic energy of fission product = 9.7 MeV for Ni-natural

Takahashi;ICCF11

Slide 4

14

The plasma-discharge type experiments 40 using ordinary-water/W-cathode electrolysis is currently of interest. Anomalously large generation of HVgas was reported by Mizuno. 40 Amount of Hj-gas production rate reached at the level of 80 times exceeding the Faraday law of electrochemical dissociation of H2O. Even if this anomalous amount of H2 production can be attributed to pyrolysis, there should be a great amount of energy source than electrolysis. They reported transmutation-like foreign elements 41 in this experiments, too. Reproducibility of CMNS experiments is of key issue for convincing the CMN effects and applying to technological devices for energy production and NWremediation. Few approaches look establishing the qualitative reproducibility, but we need further efforts to meet the 100% (quantitative) reproducibility. We may rank up hopeful methods as follows. 1. D2 gas permeation with Pd-complex. 25-30 Iwamura, Higashiyama, Spring-8 (100% for selective transmutation). 2. Super-wave + laser electrolysis with thin Pd. 9 ' 10 Israel + SRI + ENEA (very high reproducibility for large excess heat). 3. Sono-fusion with plate and nano-particles. 23 ' 24 Stringham, R. George, Arata (very high reproducibility for heat and 4 He). 4. Plasma electrolyses with W. 3 1 ' 4 0 , 4 1 Mizuno, Ohmori (transmutation and excess-H-gas production). 5. Micro-wire-Pd with Th, silica-colloid by pulse-electrolysis. 42-44 Celani, Spallone, and Violante (very high reproducibility for rapid full D-loading). 6. Nano-crystals plus gas plus laser: Arata, 15 Mastromatteo, 45 and Israelgroup. 10 Other methods of gas-glow-discharge by Karabut 46 and Yamada 4 7 - 4 9 should be notified for studying transmutation effects. For more fundamental studies, Low-energy D-beam experiments with metaldeuterides (searching enhancement of d-d and 3d fusion) by Kasagi, 9 0 - 9 4 Huke, 95 ' 96 Kitamura, 97 and Takahashi-Isobe-Ochiai 98 " 101 have made significant contributions to the progress of CMNS. 5. Theories on Nuclear Reactions under Ordering Process (Strong Interaction) Several theoretical models have been proposed and elaborated for interpreting possible mechanisms of "new fusion reactions" by deuteron behaviors under ordered (or equivalently constrained) conditions in the environment of metal-D condensed matter. Typical theories have been proposed as follows. 1. D-cluster fusion models: (Kirkinskii). 59 ' 60

EQPET/TSC (Takahashi), 50 - 58 and EODD

15

2. 3. 4. 5. 6. 7.

Bose-Einstein condensation models: Kim 61 and Tsuchiya. 62,63 Resonance tunneling: X.Z. Li. 6 4 - 6 7 Phonon-coupled gauge theory: Hagelstein. 7 ' 68 ~ 70 Coherent Bloch-state models: S. Chubb 71 - 72 and T. Chubb. 73 - 74 Swimming electron layer model: Hora-Miley. 75 ' 77 SCS fission model: Takahashi-Ohta. 32 " 35

For modeling in every theory, we should treat the new aspect how dynamic ordering or particle-constraint conditions in condensed matter (solid state) physics states can be linked or combined with new nuclear reaction channels. We have to clarify how Coulomb repulsion can be overcome, how new nuclear channels are open. We have to quantify theoretical models to give quantitative predictions for nuclear reaction rates, so as to meet the reaction rate levels from experiments. One practical issue is how 4 He can be major ash without associating intense neutron emission. The scenario D + D —>4 He+ lattice-energy (23.8 MeV) does not have place to stand on, in the view of nuclear physics 57 (see Fig. 10).

Takahashi: SIENA 2005

d + d -> 44He*(23.8 MeV) -> break-up « Branching ratio: Sn(0)/Sp(0)/Sg(0) =

&»s/////////J< 20.577 • 19,814-

r„/r,/rg =

„ 3 © . n + aHe — -*• p +1

0.5/0.5/0.0000001 • r n = r p = 0.2 MeV • r g = 0.2 MeV

Qamma transition

• r, = r n + r p + r g .T = WT,=1E-22S

0.0-

Figure 10.

-4He(gs)

• No forces to change BRs have ever been proposed!

Final state interaction and branching ratios for d-d fusion.

In EQPET/TSC models by Takahashi, 5 0 - 5 8 the idea of bosonized condensates was substantiated. To induce 4 He production without neutron emission, he made the third and fourth hadrons (deuterons or protons) participating into d-d strong interaction. In consequence, he had to treat multi-body fusion (or cluster fusion) reactions under ordered constraint of Tetrahedral Symmetric Condensate (TSC) motion in PdDx lattice. In other ways, Chubb-Chubb 7 1 - 7 4 and Hagelstein 69 ' 70 have proposed some sort of coherent fusion processes for so-many-body systems in PdDx lattice to try to

16

2) Minimum TSC

V

A ^ 4

xr 3) Be* formation

4

He

He

4) Break up

Figure 11. Illustration of TSC squeezed condensation; (a) TSC formation at t = 0, (b) minimum size state of condensed TSC, (c) formation of 8 Be* by strong interaction, and (d) break-up of 8 Be* into two alpha-particles.

reach 4 He production channels. Takahashi treats rather microscopic coherence, while Chubb-Chubb and Hagelstein do rather macroscopic coherence in metaldeuterium lattice systems. In theorizing nuclear effects in CMNS, to point out qualitatively new reaction channels is not enough at all. We have to quantify theoretical models to show quantitative (numerical) predictions that new reaction channels will be feasibly taken place. For example, such reaction channels as D + D —>4 He + 7 (23.8 MeV) or 133 Cs + 4D -^ 1 4 1 Pr + Q (50.49 MeV) look possible from the mass-energy conservation of Einstein relation, because of exothermic reactions, but actually these do Strong F. Bare Coulomb potential

Figure 12. Shielded Coulomb potential for dde* pseudo-molecule under steady-state assumption; relation to screening energy and strong interaction range for d-d reaction is illustrated.

17 Table 1. Screening energy of E Q P E T molecules Us = e2/b0 for V3 (b0) = 0 (Takahashi, SIENA 2005). Us(eV)

e*

(1.1) (2.2) (4,4) (8,8) (208,1)

b0 (pm)

dde*

dde*e*

dde*

dde*e*

36 360 4000 22154 7579

72 411 1108 960 7200

40 4 0.36 0.065 0.19

20 3.5 1.3 1.5 0.20

not happen unless high potential barriers of Coulomb repulsion can be overcome by particular ways that we should theorize. We have to estimate how Coulomb repulsion is overcome in the initial state interaction, how intermediate compound state is and what are branching ratios in the final state interaction. Theoretical modeling should be self-consistent so as to be quantified. The theory of EQPET/TSC by Takahashi 50 " 58 is trying to give quantified predictions. Recently at ICC10, Takahashi proposed TSC of four deuterons and four electrons in PdDx lattice dynamics forming a transient quasi-molecular state of orthogonally coupled two D2 molecules and squeezing semiclassically into central T-site to reach TSC-minimum-size state with about 10 fm diameter as charge neutral pseudo-particle. The TSC-minimum state for 4D/TSC causes self-fusion of 4D to 4 He + 4 He + 47.6 MeV, or capture reaction (selective transmutation) with host metal nucleus. This scenario is shown in Fig. 11. Takahashi treats transiently bosonized states of electron pairs with anti-parallel spins and quadruplet coupling e*(4,4) by Electronic Quasi-Particle Expansion Theory (EQPET). 5 1 - 5 5 He treats virtual pseudo-molecule dde* as illustrated in Fig. 12. He calculated screened potentials for dde* molecules and estimated screen energies and other potential parameters as given in Table 1. Nuclear strong force for fusion is estimated based on the concept of optical potential (see Fig. 13) and effective surface sticking force P E F 5 2 - 5 8 for multi-body (4D) fusion by TSC. • U ( r ) = V(r) + ilV(r} . l/(r) - -2.5 to -50 MeV . W(r) .0.1 to 5 MeV WW

J •4

» For fusion by surface sticking force: IV(r) - W „ 8 ( r - r 0 )

• Vs (r): screened Coulomb potential -"0

Figure 13.

Optical potential for strong interaction

18

Fusion rate in general is given for collision-like process as shown in Slide 5. ^—iment b\ A T

Fusion rate for collision process dynamic or transient process• 7= OF, |Hint| ¥i> = (Initial state interaction) x (Intermediate compound state) x (Final state interaction) • Cross-section - T2 p (E') • p (E'): final state density - Reaction-rate (ov): (4TCS//I)V72 p (E')

• (Initial) = (El. EM int) (strong int) • (Final) = BRs to irreversible decays

Slide 5 Practical formulas are given in Fig. 14. Time averaged cluster fusion rates for the TSC squeezing motion is given in Table 2. He reports some of key issues in CMNE can be explained by these EQPET/TSC models as shown in Table 3. Kim 61 ' 62 is studying CMN effects in Bose-Einstein condensation (BEC) process. He assumes that many deuterons, metal ions like Li + and electrons are confined in a void cavity in metal lattice and they are behaving as plasma. Superposition of many-body wave functions by BEC is supposed to play role for strong enhancement of dd fusion and d-6Li fusion (source of 4 He generation). Deuteron is a boson. To

F l J S i O n T a t e Of D - C l U S t e r |Takahasni:racemRes.Devel.Physics,6(2005) 1

© D-cluster formation process:

U0 = e2/r

FnD = 0F12>(4'22>Cl'32>-vI'„2> © Barrier penetration process: PB = exp (-nr„) Screened potential

® Nuclear fusion process: a = SnD/Ed !_ = av* PB* FnD D •!• (D +• {D -i- D)) =* 4D

For T-matrix elements: (1) and (2): EM interaction, (3): strong interaction Figure 14. Three-step Born-Oppenheimer treatments in formulating D-cluster fusion rates in condensed matter.

19 Table 2. e* (m, Z) (1,1) (2,2) (4,4)

T D E Q P E T calculation for E Q P E T molecules (Takahashi, ICCF12).

(A 2d) (f/s/cl.) 44

4.3 x 1 0 2.9 x 1 0 " 2 5 2.1 x 10~ 1 7 *

(A Ad) (f/s/cl.) 7.8 x 10" 2.5 x 10" 5.5 x 10"

A 2d (0) (f/s/cl.) 60

1.9 x 1 0 " 2.4 x 1 0 ~ 3 7 5.5 x 10" 2 2 *

A 4d (0) (f/s/cl.) 7.3 x 1 0 ~ 9 3 1.1 x 10~ 5 0 5.9 x 1 0 " 2 0

*Virtual value.

minimize system Coulomb energy of particles in the cavity should, however, lead to charge neutralization between deuterons and electrons to form D-atoms for dilute gas (or D2 molecules after collision process for dense gas). Plasma state at room temperature looks no good idea. And D-atoms are fermions due to odd (non-integer) spin for electron. Models by Kim and Tsuchiya need further elaboration. Takahashi's EQPET/TSC models are kind of bosonized condensate models. However, TSC is bosonized condensate under strong constraint (namely ordering process in lattice), different from BEC of dilute gas at near zero temperature but similar to bosonization of fermions (formation of Cooper pair) for super-conductivity and super-fluid. New aspect as CMNS is "Bosonization in Ordering Process". X. Z. Li has studied Resonant Tunneling Model. 64 ' 65 Intermediate compound state of fusion reactions in CM may have, he proposes, excited state with very long (as 104 s) life time to select resonating decay channel for final state interaction. During his study he has made nice progress to fit fusion cross sections for DD, DT, and D 3 He reactions using revised formulas of elementary phase-shift analysis of scattering matrix and optical potential. This is good progress. However, his model cannot change the situation of Fig. 10, namely for drastically increase branching ratio to 4 He channel since longer life time makes the gamma-transition branching ratio smaller. Hagelstein has been studying a kind of coherent fusion model to explain neutronless 4 He generation and excess heat. His models do not reach the stage of quantified theory, but are trying to approach to quantification. Recently he is proposing the phonon-coupled gauge models, assuming 'compact' intermediate state of (n-3He) to evaluate gauge transform between (d-d) state, (n-3He) state, and irreversible Table 3.

Major results: experiments versus theory.

Item

Experiment Author/Method/Results

E Q P E T / T S C model

Screening

Kasag/beam/310 eV Takahashi/3D/10 9 (dd) McKubre/electrolysis/ 30±13MeV/4H El Boher/EI/24.8 keV/Pd, Gain = 25 Iwamura/Perm/Cs —> Pr Miley/NiH/Fission-like Pro.

360 eV by dde* (2,2) (10 1 3 ) r (0.1 ms)

He production Maximum heat Transmutation

23.8 MeV/ 4 He by 4D - • Hex2 + 47.6 MeV 23 keV/Pd 46 MeV/cc by 4d/TSC 4d/TSC + M 4p/TSC + M reaction 4

20

out-going channel to 4 He. This is an elegant approach. However, there are some fundamental problems. First, (n-3He) state may not exist with meaningfully large life time to be prohibited to going out to the n + 3 He + 3.25 MeV channel with very short life time (on the order of 10~ 22 s) from the intermediate compound state 4 He* as shown in Fig. 10. He estimates that the transform strength (QM flow) between states by phonon exchange is on the order of 1 0 - 4 , which is right but is much smaller than field coupling between strong interactions (see Slide 6, accordingly). Branching ratio to electromagnetic transition (decay channel to 4 He) cannot be increased by more than 10~ 4 of those (0.5) for n + 3 He or p + t channels. Chubb-Chubb 7 1 - 7 4 have proposed a kind of coherent fusion model through the D-ion-band state in PdDx lattice Bloch potential. They assume that QM waves of many deuterons inside a well of many-body (more than 10,000 Ds) potential can link widely and, due to the double Bloch symmetry conditions, Coulomb repulsions between deuterons eliminate in scale of 1/Nwell for Nwell more than 10,000. They also assume this coherent condition should change the intermediate compound state (4He*) of DD interaction to form 4 He-ion-band state with long life time, for which we can use wave-function form of 4 He. This is another elegant theory. To reach quantified predictions by this theory, we need to substantiate many things; to prove definitely the 1/Nwell law, to Relative strength of interactions Comment by AT.

• Nuclear strong interaction: f/hc = 1 • Electro-magnetic interact: eVhc = 7.3E-3 • Weak nuclear interaction: (ghc)2 (mc/h)4 = 5E-14 • Gravity: GM2/hc = 2E-39 . Sdd = 1.1E2 keVb versus Spp = 1E-22 keVb a ~ (T-matrix)2

Slide 6 quantify ion-band state excitation functions, to evaluate life time of 4 He-ion-band state if at all, to propose an intermediate compound state (4He*) with quite different spin-parity state through the interaction with electromagnetic Bloch potential (actually phonons by lattice vibration, harmonic oscillators, for example) to avoid final state irreversible decays to n and t channels in Fig. 10. Elaboration will be tough. We summarize elaborations for quantification of theories in Slide 7, including other models by Hora's 76 swimming electron layer model, Fisher's poly-neutron model and Kozima's neutron-catalyzed reaction model.

21

We need quantification of models (difficult) by improving » Chubb-Chubb: is 1/N well screening by variational principle correct? We need quantitative estimations of T-matrix-components, for intermediate and final states. Can 4He-ion-band have life GT. 1E-22 s of 4He* (23.8 MeV) * Hageistein: branchinh ratio (1E-4) in competition of EM-force and Strong force is ignored? Does the compact n-3He state exist with meaningful life time? * Li: theory only treats S-matrix 9 (phase-shift analysis), hence total reaction cross-section improved. Others are speculations for final state interactions. * Fisher: no reason for polyneutron binding force found? * Hora: usage of reaction rates for random plasma is wrong * Kozima; no neutrons exist, neglect phonon-n inelastic scattering which escapes Bragg condition, wrong formula for secondary charged particle reactions, etc.

Slide 7 6. Theories with Weak Interactions and Others Interesting theoretical models are as follows: 1. Mini-H-atom (by heavy electron) formation to zero-momentum neutron model: Widom. 78 2. Mini-H-atom (by suborbital QM state): Mils,79 Yamamoto, 80 and 81 Filimonov. 3. Poly-neutron reaction model: Fisher 82 and Kozima. 83 Here key issue will be how reaction rates via weak interactions can be enhanced. Quantitative predictability is the key. Brief scenario of Widom's theory is; on the flat surface of metal-hydride, coherent coupling between many-body electron oscillations and proton oscillations makes effective electron mass significantly heavy. Mini-atom orbit of H-atom with heavy electron forms. Electron capture process into proton may be very strongly enhanced to generate near-zero-momentum neutrons. These very low-energy neutrons will be absorbed within very short range near surface to induce neutron-induced reactions. This kind of theory has many fundamental problems as: (1) Production cross section of "heavy electron" e* is not given, so that we cannot argue on density of very-low-momentum-neutron (VLMN) available in matter, taking into account of 10 min beta-decay of neutrons and assumed neutron-conversion cross section (see 3). If neutron density were greater than 1016 per cm 2 on surface, neutron reaction rate with H and host metal-nuclei were realistic level as experiments claim. According to neutron decay and

22

(2)

(3)

(4)

(5)

(6)

(7)

inelastic phonon-scattering with lattice vibration, which is up-scattering to higher neutron energy, we need to estimate mean existing time of VLMN on surface. (The author guesses that VLMNs get phonon energy with several barns of cross-section and very rapidly - in less than one micro-second-leak out from system.) Proton (deuteron) on metal surface lattice vibrates with (l/2ir) hu, as Einstein oscillator, and has "recoil energy" of about 30 meV. VLMN converted from proton should conserve this 30 meV as kinetic energy which is a little more than averaged (thermal equilibrium) energy of 25 meV in media at room temperature. (Einstein oscillator can have higher zero-point energy than Debye oscillators of metal atoms.) Cross section for p + e* to n+neutrino is not given. The author thinks this cross-section (over threshold energy of reaction) should be very much small, of the order of 1 0 - 2 6 of usual strong interactions. And neutrino here is different from electron-neutrino and muon-neutrino, and deviates from the three generations scenario of leptons. This cross-section (or transition matrix) estimation is key problem for making their theory realistic! 6 Li + n to 4 He + 1 + 4.8 MeV channel has about 1000 barn at En = 25 meV, compared with very small cross section 4 x 10~ 2 barn for n-capture, 6 Li + n to 7 Li + gamma. And 7 Li + n to 8 Li to 8 Be + beta to 4 He + 4 He + e process has 4 x 10~ 2 barn at En = 25meV, only. So, it is well known that 6 Li + n to 4 He + t + 4.8 MeV is predominant channel! Since reaction rate per neutron flux is (cross-section) x (velocity) and cross-section at lower energy than 30 meV has 1/v law, all reaction rates keep constant according to the change of momentum or kinetic energy. So that, even at very much low energy, reaction rate does not increase so. Widom-Larson might misunderstand these points. If p + e* state exists, it should have transition to mini-atom orbit which should emit photons greater than 13.6 eV of H-atom ground state. (This has some sort of relation to Randi Mill's sub-orbital quantum state, hydrino!) We need to estimate life time of e* becoming heavy by Widom's oscillating electro-magnetic plasmon (surface polariton) interaction on surface. If hard gamma-rays were totally absorbed by e*, we can do easily test using a standard gamma-ray source to measure gamma-peak attenuation through the sample metal-hydride surface. We have no data for Compton scattering with e*, which he assumes very much large to neglect gamma-electron processes with metal-atoms having usually much larger photoelectric, Compton and pair-creation cross sections compared with those for hydrogen atom. We know, dde*(mass = 208m-electron), namely muonic dd-molecule does not emit low-energy neutrons (but 2.45 MeV neutron by d-d fusion), although Widom theory suggests dde* to d + n + n break-up.

23

We can make such skeptical critics easily for other models also. By making clear every question, one by one, one can improve m o d e l s 8 4 - 8 9 and approach t o the target. We need tough efforts of elaborations. 7. C o n c l u s i o n s 1. Recent results of CMNS studies show very important consequences of Clean Fusion and Cold Transmutation. 2. We are in Turning Point for studying deeper and establishing new field of Condensed M a t t e r Nuclear Science (CMNS). 3. New progress is expected at this conference of ICCF12. References 1. J. R. Huizenga, Cold Fusion, The Scientific Fiasco of the Century (University of Rochester Press, USA, 1992). 2. Proceedings of ICCF9, Tsinhua University Pub. (2003). 3. Proceedings of ICCF10, World Scientific Pub., to be published, see also internet version at http://www.lenr-cana.org/ 4. Proceedings of ICCFU : World Scientific Pub., to be published, see also internet site http://www.iscmns.org/ 5. Proceedings of ASTI5 Meeting, see internet site http://www.iscmns.org/ 6. Proceedings of SIENA2005 Workshop, see ibid. 7. P. Hagelstein, M. McKubre, D. Nagel, T. Chubb, and R. Heckman, New Physical Effects in Metal Deuterons, Reprot to US-DoE (2003). 8. US-DoE: Report of the Review of Low Energy Nuclear Reactions, December 1, 2003, see to find paper at http://www.newenergytimes.com/ 9. El Boher et al, Proceedings of ICCF11, see Ref. 4. 10. V. Violante et al, Proceedings of SIENA 2005 Workshop, see Ref. 6. 11. Y. Arata et al, II Nuevo Saggitore 20, 66-71 (2004). 12. Y. Arata et al, JJAP 37 (11), L1274 (1998). 13. Y. Arata et al, JJAP 38 (7), L774 (1999). 14. Y. Arata et al, JJAP 39 (7), L4198 (2000). 15. Y. Arata et al, J. High Temp. Soc. Japan 29, 1-40 (2003). 16. M. McKubre et al, Proceedings of ICCF10, see Ref. 3 17. M. McKubre et al, Proceedings of ICCF11, see Ref. 4 18. Y. Isobe et al, JJAP 4 1 , 1546 (2002). 19. L. Case, Catalytic fusion of deuterium into helium-4, Proc. ICCF7, Vancouver (1998). 20. M. McKubre et al, Excess power observations in electrochemical studies of the D / P d system, Frontiers of Cold Fusion, Proc. ICCF3, Nagoya (1992), see http://www.lenrcanr.org/ Library. 21. M. McKubre et al, Development of advanced concepts for nuclear processes in deuterated metals, EPRI-Report (1994), see http://www.lenr-canr.org/ Library. 22. Y. Isobe et al, JJAP 4 1 , 866-870 (2002). 23. R. George, see Ref. 6. 24. R. Stringham, 1.6 MHz sonofusion device, Proc. ICCF11, see Ref. 4. 25. Y. Iwamura et al JJAP 4 1 , 4642 (2002). 26. Y. Iwamura et al, Proc. ICCF10, see Ref. 3. 27. Y. Iwamura et al, Proc. ICCF11, see Ref. 4.

24

28. M. Sakano et al, Confirmation of transmuted elements on Pd complexes using D2 gas permeation method, Proc. JCF-5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 29. Y. Iwamura et al, Correlation between deuterium flux through Pd complexes and quantity of nuclear products using D2 gas permeation method, ibid. 30. T. Higashiyama et al, Proc. ICCF10, see Ref. 3. 31. T. Mizuno, Nuclear Reactions in Solid, No.l, Chapter 8 (Kokakusha, 1999). 32. A. Takahshi et al., JJAP 4 1 , 7031-7046 (2001). 33. M. Ohta and A. Takahashi, JJAP 42, 645-649 (2002). 34. M. Ohata and A. Takahashi, Proc. ICCF10, see Ref. 3. 35. A. Takahashi, Theoretical backgrounds for transmutation reactions, ppt slides for Sunday School of ICCF10, see http://www.lenr-canr.org/ Special Collection for ICCF10. 36. F. Piantelli, Hydrogen loading of Ni and related phenomena, Proc. Siena2005 Workshop, see Ref. 6. 37. V. Montalbano et al, Evidence of radiation from Ni-H system, Proc. ICCF11, see Ref. 4. 38. G. Miley and J. Patterson, J. New Energy 1, 5 (1996). 39. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Proc. Siena2005 Workshop, see Ref. 6. 40. T. Mizuno et al., Hydrogen evolution by plasma electrolysis in aqueous solution, JJAP ±A, 396-401 (2005). 41. T. Mizuno et al, Proc. JCF6, Tokyo (2005), see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 42. F. Celani et al, Proc. ICCF11, see Ref. 4. 43. F. Celani et al, Proc. JCF5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 44. F. Celani et al, Proc. JCF6, see ibid. 45. V. Masteromatteo et al, Proc. Siena2005 Workshop, see Ref. 6. 46. A. Karabut et al, Proc. ICCF10, see Ref.3. 47. H. Yamada et al, Proc. ICCF10, see Ref. 3. 48. H. Yamada et al., Proc. JCF5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 49. S. Narita et al., ibid. 50. A. Takahashi, Condensed matter nuclear effects, Proc. Int. Meet. Frontiers of Physics, Kuala Lumpur, 25-29 July 2005, Malaysian J. Physics, to be published. 51. A. Takahashi, Deuteron cluster fusion and related nuclear reactions in metaldeuterium/hydrogen systems, Recent Res. Devel. Phy. 6, 1-28 (2005), ISBN: 817895-171-1. 52. A. Takahashi, Proc. ICCF9, pp. 343-348, see Ref. 2. 53. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Proc. ICCF10, see Ref. 3. 54. A. Takahashi, Proc. JCF5 and 6, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 55. A. Takahashi, Proc. ICCF11, see Ref. 4. 56. A. Takahashi, Deuteron cluster fusion and ash, Proc. ASTI5 Meeting, see Ref. 5. 57. A. Takahashi, A theoretical summary of condensed matter nuclear effects, Proc. Siena2005 Workshop, see Ref. 6. 58. A. Takahashi, Time-dependent EQPET analysis of TSC, Proc. ICCF12, Yokohama (2005). 59. V. Kirkinskii and Y. Novikov, Proc. ICCF9, pp. 162-165, see Ref. 2. 60. V. Kirkinskii and Y. Novikov, Numerical Calculations of Cold Fusion in Metal (Novosivirsk University Press, 2002). 61. Y. Kim, Proc. ICCF11, see Ref. 4. 62. K. Tsuchiya, ibid.

25 63. 64. 65. 66. 67. 68. 69. 70. 71. 72. 73. 74. 75. 76. 77. 78.

79. 80. 81. 82. 83. 84. 85. 86. 87. 88. 89. 90. 91. 92. 93. 94. 95. 96. 97. 98. 99. 100. 101. 102.

K. Ttsuchiya, Proc. JCF5 and 6, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ X. Z. Li et al., Proc. ICCF9, pp. 197-201, see Ref. 2 X. Z. Li et al, Phys. Rev. C 6 1 , 24610 (2000). X. Z. Li et al, Laser and Particle Beams 22 (4) (2004). X. Z. Li, Lecture at Sunday School of ICCF11, see Ref. 4. P. Hagelstein, Proc. ICCF9, see Ref. 2. P. Hagelstein, Proc. ICCF10, see Ref. 3. P. Hagelstein, Proc. ICCF11, see Ref. 4. S. Chubb, Proc. ICCF10, see Ref. 3. S. Chubb, Proc. ICCF11, see Ref. 4. T. Chubb, Proc. ICCF10, see Ref. 3. T. Chubb, Proc. ICCF11, two papers, see Ref. 4. H. Hora et al, Proc. ICCF9, p.135, see Ref. 2. H. Hora et al, Proc. ICCF10, see Ref. 3. H. Hora et al, Proc. ICCF11, see Ref. 4. A. Widom and A. Larson, Ultra low momentum neutron catalyzed nuclear reactions on metallic hydride surfaces, private communication (2005), see http://arxiv.org/abs/cond-mat/0505026 R. Mills et al, IEEE Trans. Plasma Set. 3 1 , 338-355 (2003). H. Yamamoto, Proc. JCF5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ B. Filimonv, Proc. Siena2005 Workshop, see Ref. 6. J. Fisher, ibid. H. Kozima, Proc. JCF-5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ F. Gareev, Proc. ICCF11, see Ref. 4. F. Gareev, Proc. SIENA2005 Workshop, see Ref. 6. T. Sawada, Proc. ICCF11, see Ref. 4. T. Sawada, Proc. JCF5, http://wwwcf.elc.iwate-u.ac.jp/jcf/ F. Frizone, Proc. ICCF11, see Ref. 4. V. Vysotskii, ibid. J. Kasagi et al, J. Phys. Soc. Jpn. 7 1 , 2881-2885 (2002). J. Kasagi and H. Yuki, JPSJ 58(3), 190-194 (2003). J. Kasagi et al, Proc. ICCF10, see Ref. 3. J. Kasagi et al, Proc. ICCF11, see Ref. 4. J. Kasagi, Abstract for JCF5, http://wwwcf.elc.iwate-u.ac.jp/jcf/ A. Huke, Ph. D. Thesis, Technical University of Berlin, 2004. A. Huke et al, Proc. ICCF11, see Ref. 4. A. Kitamura et al, Proc. ICCF10, see Ref. 3. A. Takahashi et al, Phys. Lett. A 255, 89 (1999). Y. Isobe ., see Ref. 22. A. Takahashi et al, Studies on 3D fusion reactions in TiDx under ion beam implantation, Proc. ICCF10, see Ref. 3. A. Takahashi et al, Fusion Technol 34, 256-272 (1998). S. Szpak et al, Evidence of nuclear reactions in the Pd lattice, Naturwissenschaften 00:1-4 (2005).

S U M M A R Y OF ICCF-12

X I N G Z. LI Department

of Physics, Tsinghua University, Beijing E-mail: [email protected]

100084,

China

The progress of the Condensed Matter Nuclear Science reported during ICCF-12 is summarized with emphasis on reply to the DOE review in 1989 and in 2004. The 18 reviewers might not be aware of the new achievement in the Advanced Technology Research Center, Mitsubishi Heavy Industries; hence, their conclusion should have been more positive toward this research. Arata's DS-reactor and the "heat after death" experiment should change the conclusion about the "excess heat" and its prospect. Various fundamental researches have shown the consistent nature in understanding. A cost effective and comprehensive study is mentioned.

1. From 1989 DOE Review to 2004 DOE Review ICCF-12 is a good chance to check the progress in the past 16 years. DOE reviews in 1989 and in 2004 represent two milestones. In the Blue Cover Book written by DOE 1989 ERAB, 1 the fifth point in conclusion was "Nuclear fusion at room temperature, of the type discussed in this report, would be contrary to all understanding gained of nuclear reactions in the last half century; it would require the invention of an entirely new nuclear process." It is true that 16 years study has confirmed that there is an entirely new nuclear process. The title of Mckubre and Hagelstein's report was just "New Physical Effects in Metal Deuterides." 2 Among the 18 reviewers, one-half of them recognized that "evidence for excess power is compelling;"3 however, only one of them recognized that the occurrence of low energy nuclear reactions is demonstrated by the evidence presented. If DOE allowed more time for the reviewers to become acquainted with the nuclear transmutation work, the other 17 reviewers might recognize also that the occurrence of low energy nuclear reactions is demonstrated, because in the past 10 years Dr. Iwamura just did what they recommended, i.e. "the use of state-of-the-art apparatus and techniques to search for fusion events in thin deuterated foils."4 2. Nuclear Transmutation in Super-Lattice Complex Dr. Iwamura's pursuing led to his great success. He started his research when Japanese New Hydrogen Energy (NHE) Project was initiated in 1993; however, he did not stop when NHE project stopped. He did not insist to use neutron as the only one signal for nuclear reaction. He tried tritium, X-rays, and excess heat. He tried both electrolysis and gas-loading method. Eventually, he found that deuterium flux, cesium coating on the surface, and the super-lattice complex were 26

27

the three key elements to reproduce his discovery, i.e., the nuclear transmutation induced by deuterium flux. He found that X-ray photoelectron spectroscopy was the most suitable in-situ diagnostic tool to monitor the nuclear transmutation. His supervisor was so judicious to allow him traveling between Yokohama and Kobe in every week in order to continue his study. Indeed he was so brave to try the high Z element as a candidate to interact with the low energy deuterium gas; and he was so patient to wait for weeks in order to observe the nuclear transmutation. When his methodology was established, he was able to send his sample to France for the SIMS (time-of-flight) analysis; and send his sample to SPring-8 for microbeam analysis. Moreover, professor Takahashi of Osaka university was able to use his method to make sample, and use the Neutron Activation Analysis to verify the product of the nuclear transmutation (Pr). 5 Now Mitsubishi Heavy Industries is collaborating with Naval Research Laboratory (NRL) in US in order to use NRL's Trace Element Analysis Mass Spectroscopy equipments. The Disclose Agreement between MHI and NRL restricted the information flow before the publication; however, we might still learn from Drs. Iwamura, Narita, and Yamada's presentations. 6,7 The unidentified peak was discovered using the microbeam. Possibly, it was lanthanum (La). It was just the element between Cs and Pr. It might imply that Cs was added a deuteron first; then, one more deuteron was added to reach the Pr. Moreover, if we look at the natural abundance of lanthanum, there is only one stable isotope for lanthanum with a little mixture of long life-time isotope (0.09%, 1.05 x 10 11 years). This is very similar to the praseodymium which has only one stable isotope as well. Indeed, terbium (Tb) and thulium (Tm) were discovered in the early Electron Probe MicroAnalysis experiment also when we tried to identify any new elements in the sample of palladium hydride. 8 To my surprise, Tb and Tm have only one stable isotope as well (see Table 1). Table 1. La 99.91

Ce

Pr 100

Nd

Isotope abundance of the rare earth series of elements Pm

Sm

Eu

Gd

Tb

Dy

Ho

100

Er

Tm

Yb

Lu

100

3. Hydrogen-Induced Low-Energy Nuclear Reactions It was a brave decision for Iwamura to select high Z material (Cs, Sr, Ba, etc.) as sample. It was also a brave decision for professor G. Miley to study the hydrogeninduced low-energy nuclear reaction. 9 In the early days, H2 was just selected as a control in comparison with D2, because most of scientists (including the members of ERAB of DOE) were thinking of the d + d fusion reaction only. Even professor M. Fleischmann was not ready to accept such new phenomena. In ICCF-7 (Vancouver, 1998), Miley asked a question during a plenary session. He would like to know what are Martin's comments on nuclear transmutation. Fleischmann

28

replied with humor "I am a conventional chemist." However, the most impressive results are the four peaks in the distribution of nuclear products which appeared in various experiments in the world (Refs. 10-12). The organizer of ICCF-12 made a good program to arrange a minicourse presentation by Miley. It should be emphasized that both Miley and Iwamura used thin film samples and used super-lattice complexes in their experiments. 4. Prom DS-Cathode to DS-Reactor Professor Arata switched from electrolytic cell to gas-loading experiment while keeping his double-structure characteristics of palladium. 13 He is happy with this new structure because "Sauna-bath" is better than the "hot-water-bath." More energy output would be available from the newly designed DS-reactor. It is quite clear qualitatively to show that the temperature reverse (i.e. the temperature of heater is lower than that of the heated object) appeared when the H2 was replaced by D2, and the vacuum vessel was filled with Pd-black or Nano Pd. The most interesting point was the temperature setting. T out = 140°C was just same as that appeared in the early experiment in China, where a correlation between the deuterium flux and abnormal heat flow was found14 (Fig. 1, right-hand side).

Correlation between heat flow and deuterium

J. Phys. D: Appl. Phys. 36 (2003) 3095

Arata "Sauth bath" reactor

140°C-150°C

Figure 1. About 140°C as a characteristic temperature was discovered in both Arata's Sauna bath and an early Chinese correlation experiment where D2 gas was permeating Pd thin wall.

The DOE reviewers in 2004 asked the frequently asked questions in those excess heat experiments: "The reviewers who did not find the production of excess power convincing cite a number of issues including: excess power in the short term is not the same as net energy production over the entire of time of an experiment; all possible chemical and solid state causes of excess heat have not been investigated and eliminated as an explanation; and production of power over a period of time is

29

a few percent of the external power applied and hence calibration and systematic effects could account for the purported net effect." As a supplement to against those criticisms, we may add one more experiment: "Heat after Death" work. 15 M. Fleischmann's "Heat after Death" experiment in 1993 provided a compelling estimate. His electrolytic cell was boiled to dry in 10 min. The vaporization heat was so large (102.5 kJ) that all uncertainties in the other effects might be ignored (22.5 kJ for input from electrolysis, 6.7kJ for heat transfer to ambient). The volume of the palladium cathode was only 0.0392 cm 3 which is about 4.6 x 10~ 3 mol. Hence, the most conservative estimate would be 18.8 MJ per mol of Pd (i.e. 195 eV per Pd atom). Even if this amount of energy had have been stored in the palladium due to some unknown mechanism during the long period of electrolysis, this would have still be an anomalous "chemical" effect (if it is not a nuclear effect). Would the reviewers still say "While significant progress has been made in the sophistication of calorimeters since the review of this subject in 1989, the conclusions reached by the reviewers today are similar to those found in the 1989 review," if they had paid attention to this calculation. 5. N e w Hydrogen Energy Project and Loading Ratio Dr. Matsui kindly appeared in ICCF-12 again. His announcement about NHE project in ICCF-4 was a great impetus to Condensed Matter Nuclear Science research. At that time a program was established to aim at the high loading using electrolysis method. Adding something (e.g. thiourea, etc.) in the electrolyte was found effective to enhance the loading ratio, but the excess heat was not as great as expected. 16 The failure in helium detection and the argument on "excess heat" were partially compensated by the successful nuclear transmutation 17 and the deuterium flux effect.18 Particularly, the deuterium flux effect appeared both in the "excess heat" and in the nuclear transmutation. It turns out to be the key issue to reproduce the effects of the condensed matter nuclear science. If the 18 reviewers had have chance to review this issue, they might not be so pessimistic that "Most reviewers, including those who accepted the evidence and those who did not, stated that the effects are not repeatable,..." 6. Fundamental research in Condensed Matter Nuclear Science "... Use of reasonably well-characterized materials, exchange of materials between groups, and careful estimation of systematic and random errors" was recommended in DOE 1989 review. Then, how to characterize the material? The resistance ratio of palladium sample was widely used as an important characteristic in electrolysis and gas-loading experiment. Mckubre of SRI group, 19 and Spollane and Celani of Frascatti group 20 presented very careful measurement with close collaboration. Eight methods of measurement were summarized to relate this resistance ratio to the loading ratio of the palladium sample. It was found that the relationship between

30

resistance ratio and loading ratio was very complicated because there was no good calibration for the high loading region where the sample was supposed to work, and because the resistance depended on temperature while the temperature coefficient depended on loading ratio also. The recommendation is that resistance ratio might be still a good characteristic if we specified the temperature at which this ratio was measured. The careful study on the temperature coefficient of the resistance of the palladium hydride revealed a possible phase transition in the high loading region which might be just the region of interests for CMNS. 7. Long Life-Time State in Condensed Matter Nuclear Science Three-deuteron reaction was unexpectedly discovered while the branching ratio of the d + d fusion was measured at low energy. It was first discovered in 1993 by professor Kasagi at Tohoku University in terms of d + (d + d) —> p + n + a reaction. 21 Kasagi's experiments at low energy was very reliable that even Dr. Morrison, the famous opponent of the "cold fusion", stood up to praise Kasagi's experiments for screening effect at low energy as the best experiment in ICCF-7 (Vancouver, 1998). Indeed, professor Takahashi tried to verify this three-deuteron reaction in terms of d + (d + d) —> T + 3 He as well at Osaka University.22 This three-deuteron reaction implied that two deuterons were kept in a Long Life- Time State before two deuterons saw the third deuteron. During the ICCF-12, Kasagi proposed further the evidence of the motion of the deuteron before d + d interaction, and Takahashi proposed further the assumption of Bosonized Condensates. 23 If we look at the Bockris' paper in ICCF-11 proceedings 12 about the tritium production and the /3-decay, we may believe that this Long Life- Time State might be essential in order to understand the mechanism of the condensed matter nuclear science. If the reviewers could be aware of those facts; then, they might not say: "The studies were designed to investigate screening effects in materials that would be relevant to fields such as nuclear astrophysics. Those reviewers who commented on these studies generally viewed them favorably, but to many reviewers these studies were somewhat peripheral to the main thrust of this review." 8. Dolan's Comments and Italy—Japan Joint Projects Dr. Thomas Dolan was an officer at International Atomic Energy Agency to coordinate the fusion research in the world for United Nations (1995-2001). He was mainly working for plasma fusion projects; however, he visited some of the "cold fusion" laboratories, and even took part in the ICCF-9 (2002, Beijing) as a retired scientist. He suggested that we should establish an international society, an international journal, and an award in order to enhance the credit of our research, and break the bad cycle to obtain both the credit and the research fund. Now he attended ICCF-12 again. We have the International Society for Condensed Matter Nuclear Science, the International Journal for Condensed Matter Nuclear Science,

31

and the Preparata Medal. Professor Takahashi announced that there would be a Joint Project between Italian and Japanese scientists to explore the possibility of processing the nuclear waste using the nuclear transmutation induced by deuterium flux. The first phase would be supported by 13 million Euros and followed by second phase with 12 million Euros. 9. A Cost-Effective Study Dr. Thomas O. Passell, the Co-Chairman of the ICCF-4, proposed further his results in using discharge tube for excess heat detection. 24 He intended to use the small size gas discharge tube to make a wide-range survey on various materials for electrodes and gases while keeping the sensitivity and efficiency high enough. When the government support is still a long way to go, he used his retirement money to keep the project running. As a retired manager from the Electrical Power Research Institute, he has been optimistic towards the future of the Condensed Matter Nuclear Science. Israel group represents an excellent private company to achieve constant progress in excess heat with the best international collaboration (Mckubre of SRI, Violante of INFN). 25 DOE's recommendation, "Emphasis should be placed on calorimetry with closed systems and total gas recombination, use of alternative calorimetric methods, use of reasonably well characterized materials, exchange of materials between groups, and careful estimation of systematic and random errors. Cooperative experiments are encouraged to resolve some of the claims and counterclaims in calorimetry", has been fully realized already. 10. Prospects The situation is changing gradually towards favorable to Condensed Matter Nuclear Science. The Journal of Fusion Energy, decided to accept the submission from the Condensed Matter Nuclear Science.26 It has been mainly a hot fusion journal edited by the former DOE officer (Dr. Steve Dean), and published by the famous Springer Verlag. Springer Verlag even decided to publish an academic book about the Condensed Matter Nuclear Science as well. This "New Physical Effects in Metal Deuterides" would be disseminated eventually, and lead to a clean and sustainable energy resource for the world. Acknowledgements This work is supported by the Natural Science Foundation of China (#10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds). I would like address that we are grateful to Professor A. Takahashi, Dr. Y. Iwamura, Professor K. Ota, and the local organization committee for a very successful ICCF-12. It was well planned, well organized and well programmed.

32

References 1. Cold Fusion Research, DOE/S-0073, A report of the energy research advisory board to the united states department of energy (1989). 2. Peter L. Hagelstein, Michael C.H. McKubre, David J. Nagel, Talbot A. Chubb, and Randall J. Hekman, New Phys. Eff. Met. Deuterides (2004). 3. U.S. Department of Energy Cold Fusion Review Reviewer Comments, http://www. newenergytimes.com/DOE/DOE.htm (2004). 4. Y. Iwamura et al., Observation of surface distribution of products by X-ray fluorescence spectrometry during D2 gas permeation through Pd complexes, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 5. T. Higashiyama, A. Takahashi et al., Replication of MHI transmutation experiment by D2 gas permeation through Pd complex, in: P. Hagelstein, S.R. Chubb (eds), World Scientific (New Jersey, 2006), Proc. ICCF-10, Cambridge, USA, 24-29 August (2003). 6. S. Narita et al., Discharge experiment using P d / C a o / P d multi-layered cathode, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 7. H. Yamada et al., Producing transmutation element on multi-layered Pd sample by deuterium permeation, Presentation ICCF-12, Yokohama, Japan, November 27December 2 (2005). 8. G.S. Qiao, X.Z. Li et al., Nuclear products in a gas-loading D/Pd and H/Pd system, Proc. ICCF7, Vancouver, Canada, April 19-24, ENECO, Inc., Salt Lake City, UT (1998). 9. G.H. Miley, Overview of light water/hydrogen-based low energy nuclear reactions, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 10. T. Mizuno, T. Ohmori and M. Enyo, Change of isotope distribution deposited on palladium induced by electrochemical reaction, J. New Energy 1(1), 23 (1996). 11. T. Ohmori and M. Enyo, Iron formation in gold and palladium cathodes, J. New Energy 1(1), 15 (1996). 12. J.O-M. Bockris, Histroy of the discovery of transmutation at texas A & M university, in: Jean-Paul Biberian (ed.), World Scientific (New Jersey 2006) Proc. ICCF-11, Marseilles, France, 31 October-5 November (2004), p. 562. 13. Y. Arata and M.J.A.Y.C. Zhang, Development of 'DS-Reactor' as the practical reactor of cold fusion based on the 'DS-CelF with the 'DS-Cathode', Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 14. X.Z. Li, Jian Tian et al., Correlation between abnormal deuterium flux and heat flow in a D/Pd system, J. Phys. D: Appl. Phys. 36, 3095 (2003). 15. M. Fleischmann and S. Pons, Calorimetry of the Pd-D20 system: from simplicity via complications to simplicity, Phys. Lett. A 176, 118 (1993). 16. A. Kubato et al., Development and experiments on a flow calorimetry system, in: M. Okamoto (ed.), Proc ICCF-6, Toya, Japan, 13-18 October (1996), Vol. 1, p. 52. 17. G.H. Miley et al, Quantitative observation of transmutation products occurring in thin-film coated microspheres during electrolysis, in: M. Okamoto (ed.), Proc ICCF6, Toya, Japan, 13-18 October (1996), Vol. 2, p. 629. 18. Y. Iwamura et al., Correlation between behavior of deuterium in palladium and occurrence of nuclear reactions observed by simultaneous measurement of excess heat and nuclear products, in: M. Okamoto (ed.), Proc. ICCF-6, Toya, Japan, 13-18 October (1996), Vol. 1, p. 274. 19. M.C.H. Mckubre et al., Using resistivity to measure H/Pd and D/Pd loading: method and significance, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005).

33

20. A. Spallone, F. Celani et al, Measurements of the temperature coefficient of electric resistivity of hydrogen overloaded Pd, Presentation ICCF-12, Yokohama, Japan Novembew 27-December 2 (2005). 21. J. Kasagi et al., Energetic protons and alpha particles emitted in 150-keV deuteron bombardment on deuterated Ti, J. Phys. Soc. Jpn 64(3), 777 (1995). 22. A. Takahashi et al, Studies on 3D fusion reactions in TiDx under Ion beam implantation, in: P. Hagelstein, S.R. Chubb (eds), World Scientific (New Jersey, 2006), Proc. ICCF-10, Cambridge, USA, 24-29 August (2003) p. 657. 23. A. Takahashi, Time-dependent EQPET analysis of TSC, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 24. T.B. Benson and T.O. Passell, Glow discharge calorimetry, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 25. I. Dardik et al., Progress in electrolysis experiments at energetics technologies, Presentation ICCF-12, Yokohama, Japan, November 27-December 2, (2005). 26. X.Z. Li et al., A Chinese view on summary of condensed matter nuclear science, J. Fusion Energy 23(3), 217 (2004).

OVERVIEW OF LIGHT W A T E R / H Y D R O G E N - B A S E D LOW E N E R G Y N U C L E A R REACTIONS

G E O R G E H. M I L E Y Department

of Nuclear, Plasma and Radiological Engineering, 103 S. Goodwin Avenue, Urbana, IL 61801, E-mail: [email protected]

University USA

of

Illinois,

P R A J A K T I J. S H R E S T H A NPL Associates

Inc.,

912 W. Armory Avenue, Champaign, E-mail: [email protected]

IL 61821,

USA

This paper reviews light water and hydrogen-based low-energy nuclear reactions (LENRs) including the different methodologies used to study these reactions and the results obtained. Reports of excess heat production, transmutation reactions, and nuclear radiation emission are cited. An aim of this review is to present a summary of the present status of light water LENR research and provide some insight into where this research is heading.

1. Introduction This review focuses on the transmutation reactions and excess heat production in experiments using light water electrolysis or hydrogen gas/plasma loading undergoing low-energy nuclear reactions (LENRs). Although most LENR ("cold fusion") research has focused on heavy water, a considerable number of experiments have used light water electrolysis or hydrogen gas loading. A few experiments have attempted to compare the results from light versus heavy water, 1 - 4 but these comparisons remain inconclusive. There are a wide variety of cold fusion nuclear reactions. As shown in Fig. 1, the original Pons-Fleishmann (P-F) reaction involved DD fusion, where unlike in hot fusion, the reaction channel is "interrupted" through deactivation of the excited He4 reaction product by energy transfer to the host lattice, ultimately heating the lattice. Alternately, a number of researchers have reported transmutation reactions that involve interactions between deuterium (or hydrogen) directly with atoms in the host lattice, typically heavy metals. This branch of "cold fusion" is commonly termed LENR, although recently there has been a move to also term P - F type DD reactions as LENRs as well. The observation of nuclear reactions between electrolyte and host metal atoms is quite unexpected due to the very large coulombic barrier involved (much larger than for D-D reactions). Consequently, one purpose of this review is to bring together much of the data accumulated on this striking new phenomenon. The readers are 34

35

left to decide for themselves if the data is adequate to establish the case for such reactions and possibly to formulate new experiments that build on and extend this data base. About 40 publications were included in this review (see references herein). This was intended to be representative but not exhaustive of the field. Researchers wishing to add information to the data base are invited to contact the authors. D-D Reactions T +p

% branching hot fusion "P—F" type 50 < 0.1

D - D - > He-3+ n

50

He-4 + gamma

< 10

< 106 99+

LENRs p + metal —fc- products or "fission" product array Figure 1. Comparison of LENR reactions and DD reactions occurring in hot and "cold" ( P - F type) fusion.

1.1.

Methodology

A summary of various methods employed for this study is given in Table 1. A majority of the researchers cited used electrolysis to study LENR: Pd/Pt, Ni/Pt were commonly used electrodes. K2CO3 is a popular choice as an electrolyte, a trend perhaps started by the Mills and Kneizy's early experiments where extremely large reaction rates were reported. Gas loading is also frequently used while a few researchers have reported using a glow discharge (GD) plasma. 1.2. Early Studies

at

UIUC

Earlier work by one of the authors (Miley) in collaboration with Patterson represents one of the more extensive studies of light water electrolysis relative to reaction products and excess heat. About 1000 microspheres (~0.5cm 3 volume) were used in a packed-bed electrolysis cell. Thin films of Ni and/or Pd were coated on the beads to serve as the cathode. The electrolyte was 1 M Li2S04 light water electrolyte with a flow rate of ^ l l m l / m i n through the packed bed. Voltages across the bed were held at ~2-3 V, with several mA of current, giving an electrical input power of approx. 0.06 W. Significant excess heat and a fission-like reaction product array were reported. A detailed description of the experiment can be found in Ref. 1. 1.3. Reaction

Product

Analysis

Method

Reaction products have been analyzed using a variety of precision mass analysis techniques. For example, Miley et al. used a combination of NAA, SIMS, Energy Dispersive X-ray (EDX) analysis and Auger Electron Spectroscopy (AES). 1 Cirillo

36 Table 1. Summary of various methods employed for light water/H2 LENR studies (data collected for this and following tables and figures use Refs. 1—35) Electrolysis

Total

Electrode Pt/Pd Pt/Ni Pt/W Pt/Au Pt/Sn Pt/Re Pt/Ti Pt/Ag Pt/Pt

14 5 3 4 1 1 2 1 2

Electrolyte K2CO3 H2SO4 Na2C03 Li2S04 KOH Na2S04 CS2SO4 H20

10 3 5 4 1 5 1 2

GD plasma Gas loading

1 5

and Iorio used SEM to study transmutation products. 9 Arapi et al. used TOFSIMS for product analysis. 5 Iwamura et al. used XPS extensively in their studies, although they concentrated on D2 gas experiments (versus H2), so are not included in this survey per se. 36 2. Results 2.1. Transmutation

Products

A quantitative measure of the yield of transmutation products (and isotopic shifts from natural distribution in key products) in four major atomic groups (6-18, 22-35, 44-54, and 75-85) were obtained by Miley et al.1 Others also have reported significant nuclear reaction products and isotopic shifts in light water LENRs. In some cases of the observed elements were from the lanthanide group, including Lu, Tb, Pr, Eu, Sm, Gd, Dy, Ho, Nd, and Yb. It is widely accepted that these rare earth elements are less likely to be found as impurities, strengthening confidence in their results (although most researchers have tried to rule out mistakes due to impurities versus the common "product" elements such as Fe, Cu, Ag, Zn, Au, etc via analysis of cell components, electrodes and electrolyte prior to LENR runs).

37

Isotopic shifts are another key feature often cited against mistaken identification of impurities as reaction products. Violante's study showed that the 6 3 Cu/ 6 5 Cu isotopic ratio shifted.33 In this Ni-hydride film work the most abundant copper isotope was 65 Cu with a shift from natural distribution by f360%. Cirillo and Iorio found Re, Os, Au, Hf, Tl, Er, and Yb on the surface of the cathode, which was not present before the reactions. 9 Ohmori et al. reported finding Hg, Kr, Ni, and Fe with anomalous compositions in Au electrodes during light water electrolysis.29 In addition Si, Mg with other anomalous compositions were also detected in the precipitates separated from the Au electrode after electrolysis at extremely high current densities. They found significant deviations from natural values. Minor product elements such as Os, W, and Ru in particular showed large deviation, whereas elements with larger yields like Pb and Ag rarely showed significant deviations. Yamada et al. also reported a large increase of Cr, Fe, Cu, and Ag in their experiment where Pd was loaded with hydrogen gas. 35 Arapi et al. found Be and Ni in heavy water while in light water LENR they report Li, Ba, and Ni. 5 Dash et al. reported formation of Au and Ag in both light and heavy water LENR; however, the concentrations were somewhat higher in the heavy water experiments. 10 Table 2 summarizes the list of elements observed in light water by the number of times they were reported being produced in their research by different research groups. Fe and Cu were commonly observed. Rare earth elements were reported less frequently. Also note that a majority of the transmutated elements reported have changes in their isotopic composition from the natural abundance. It is interesting that the frequency of observation of light water LENR elements is not significantly different from heavy water LENR (for the latter see Ref. 37). Table 2. The total numbers of reports that state the elements were produced in their experiment Observation frequencies

Transmutation elements

1 2 3 4 5 6 7 8 11

As, Ge, S, Hg, Kr Cd, Rr , Au, Hf, Th, Er, Yb, B, V, Cs Li, Ba, Al, Os, C, Si Mg, Mn, Co, P b Ag, CI, Ti Ni, K Ca, Cr, Zn Cu Fe

One way to evaluate this data is to consider a confidence level of >6 observations. Then Ni, K, Ca, Cr, In, Cu, and Fe meet the criteria (Fig. 2). However, it can be argued that the potential impurity levels for some of the less frequently observed elements are very low, raising the signal/noise confidence level for those observations despite their less frequent observation.

38

Figure 2. This graph shows the frequency of observation for various transmutated elements designated by atomic number.

2.2. Radiation

Emission

Recent experiments using various methods of loading hydrogen have shown significant soft X-ray emission in certain specialized experiments, e.g. see Ref. 38. Also MeV energy charged particles have been reported. Alpha particles and protons have been identified with energies around 11.0-16.0 and 1.7 MeV, respectively. During electrolysis of thin Pd-film cathodes on dielectric substrates as well as from Pd-black electrode surfaces. Only very weak X-ray emission was found in these experiments, the upper dose limit (corresponding to <~5.0 X-ray photon/s x cm 2 with E^ = 10 keV). 39 While there is evidence for energetic charged particles and soft X-ray emission in these studies, it remains to be determined if the mechanism for this emission is directly related to the transmutation/heat effect or is associated with auxiliary EM effects. In a unique experiment to explore possible radioactive waste disposal applications, Dash and Chicea reported that in light water experiment using U electrodes the intensity of the alpha, beta, gamma radioactivity of the electrodes increased after loading hydrogen. 11 The 235 U and 2 3 4 Th isotopic concentrations were also reported to have increased. 2.3. Excess

Heat

Various researchers have reported excess heat generation suggesting that it is also one of the signatures of light water LENRs. Several such reports are mentioned here. Indeed, since the transmutation reactions involve +Q values, some excess heat should be expected. However, the magnitude of the excess heat versus the input power remains an open question. Cirillo and Iorio report a definitive excess energy in their light water experiment even after substracting out energy associated with chemical reactions; energy related to the heating-up and fusion of the tungsten; energy used in expanding gas and

39

steam leaving the cell; energy lost by thermal and electromagnetic radiation; and loss of heat through the insulation. 9 Dash et al. have performed extensive light-water experiments and report that excess heat generated in their light water LENR experiment was only slightly lower than in "equivalent" heavy water experiment. 10 In their pioneering studies Mills and Kneizys reported 130 mW of excess heat. 18 Noninski repeated Mills and Kneizys light water Ni electrode experiment independently and reported 26-160% excess energy compared to input energy.23 Dufour et al. reported excess energy of 7mW in their H 2 gas loading experiment, corresponding to —25-30% of the input energy.13 Ohmori and Enyo reported 907mW of excess energy in a K 2 C 0 3 , Sn electrode electrolysis experiment. 32 Fujii et al. reported having excess energy of 7.8 W in a Li2SC>4, Pd/Ni electrode electrolysis experiment, which is more than 5% excess. 14 However, this excess heat was always reproducible. It is not conclusive whether using light water or heavy water produces more excess heat. Some research has reported that heavy water produced relatively larger excess heat and more transmutation products, 7 ' 1 0 while some have indicated that in both cases the excess heat and reaction products were similar. 31 Direct comparison is complicated since many parameters are modified with an electrolyte substitution. Thus, much work is required before carrying out a meaningful comparison. The excess energy for light water/H 2 LENR reported by various researchers tends to be either low (<10%) or high (>25%), with few reports of intermediate values (see Table 3, Fig. 3). More quantitative analysis is required to understand if this "two tier" result has a basic cause. Table 3. The range of excess energy various reports have achieved in their experiment Excess energy (%) 0-5 6-10 11-15 16-20 21-25 26-30 31-35 35+

2.4. Historical

Number reported 2 2 0 0 1 3 0 2

Trends

A review of historical trends indicates that a majority of researchers have examined both the transmutation reactions and excess heat generation, strongly suggesting that they expect both phenomenon in light water LENR. However, considerable work has also continued to study these phenomenons separately. Table 4 shows that heavy activity occurred in the early 1990 period, and then decreased. However, starting in 2000 onward, research in light water LENR again increased in activity.

40

Excess energy (%) Figure 3.

This graph shows Table 3 data in a graphical presentation.

This suggests that some time was required for researchers to digest the early work and become interested in devoting time to this new area of LENR.

3. Theory Many different theories have been proposed for the mechanism of reactions that takes place in LENR. However, a definitive match of theory and experiment has yet to be achieved. Thus the "best" theory remains unclear. In order to explain how the large Coulombic barrier is overcome, many theories introduce a neutral particle in the reaction matrix. Some of the theories of this type include Neutron Cluster formation by Fisher, 40 Free Neutron Reactions by Kozima, 41 R-Matrix Theory by Chubb, 42 Shrunken Hydrogen by Mills,43 Electron-Proton capture by Stoppini 44 and Proton/Deuteron Cluster by Dufour.45 The challenge now is to sort out how any of these theories can explain the unique signatures of heat and varied transmutation products reported experimentally.

Table 4.

Survey of the year and the key signatures of LENR focused in the study Years

Type of study Excess head and transmutation Excess head studies — transmutation not studied Transmutation studies — excess head not studied Excess head studies - transmutation not found

1990-1994 4 6

1995-1999 2 1 3

2000-2005

Total

6 1 5 1 Total

12 8 8 1 29

41 4.

Conclusions

In view of the rather extensive d a t a base for light water/hydrogen-based LENR, it is rather convincing t h a t this phenomenon is real. Since the measurements are very tedious and demanding, some errors are no doubt contained throughout the database. (The authors did not feel qualified to rule out any seriously reported d a t a by competent researchers.) However, it seems highly unlikely t h a t all of the d a t a are erroneous. From a practical point of view, the issue remains whether or not there is any unique advantage of light water/hydrogen L E N R versus heavy wat e r / d e u t e r o n LENR. Two applications are at issue for both: heat production a n d / o r transmutation. However, the experiments surveyed here suggest t h a t at this stage there is no clear evidence whether or not heavy water is more favorable t h a n light water for either application. Clearly many more comparative studies are essential t o clarify this issue. Another aspect is t h a t the heat reaction in these two cases appears to produce different reaction products. Thus, for wide applications involving public exposure the reaction products need t o be carefully evaluated relative to environmental compatibility a n d radioactivity. This evaluation not only applies t o the main reaction but possible parasitic ("side") reactions.

Acknowledgments We would like to t h a n k all the researchers in the field who has provided significant contribution in preparation of this paper. This work was partially supported by a grant from the New York Community Trust.

References 1. G.H. Miley, G. Name, M.J. Williams, J.A. Patterson, J. Nix, D. Cravens, and H. Hora, Prog. New Hydrogen Energy 2, 629 (1997). 2. J. Dash, G. Noble, and D. Diman, Trans. Fusion Technol. 24, 299 (1994). 3. J. Dash, G. Noble, and D. Diman, Surface Morphology and Microcomposition of Palladium Cathodes After Electrolysis in Acidified Light and Heavy Water: Correlation With Excess Heat, ICCF 4, Lahaina, Maui (1994). 4. J. Dufour, J. Foos, J.P. Millot, and X. Dufour, Fusion Technol. 31 198 (1997). 5. A. Arapi, R. Ito, N. Sato, M. Itagaki, S. Narita, and H. Yamada, Experimental observation of the new elements production in the deuterated and/or hydride palladium electrodes, exposed to low energy DC glow discharge, ICCF-9, Tsinghua Univ., Beijing, China, May 19-24 (2002). 6. R.T. Bush, Fusion Technol. 22, 301 (1992). 7. C.S. Cano, Comparison of Heat Output and Microchemical Changes of Palladium Cathodes under Electrolysis in Acidified Light and Heavy Water, MS Thesis, Portland State University (2002). 8. C.H. Castano, A.G. Lipson, S.O. Kim, and G.H. Miley, Calorimetric Measurements during Pd-Ni thin film-cathodes Electrolysis in L12SO4/H2O Solution, Proc. ICCF-9, Beijing, China, pp. 24-28, May 19-24 (2002). 9. D. Cirillo and V. lorio, Transmutation of metal at low energy in a confined plasma in water, ICCF11, Marseille, France (2004).

42

10. J. Dash and G. Noble, Intern'l. Symp. On Cold Fusion and Advanced Energy Sources, Belarusian State University, Minsk, Belarus, May 24-26 (1994a). 11. J. Dash and D. Chicea, Changes In The Radioactivity, Topography, And Surface Composition Of Uranium After Hydrogen Loading By Aqueous Electrolysis, ICCF-10, Cambridge, MA (2003). 12. M. Di Giulio, E. Filipppo, D. Manno, and V. Nassisi, Intrn'l J. Hydrogen Energy 27, 527 (2002). 13. J. Dufour, J. Foos, and J.P. Millot. Measurement of Excess Energy and Isotope Formation in the Palladium-Hydrogen System, ICCF-5, Monte-Carlo, Monaco: IMRA Europe, Sophia Antipolis Cedex, France (1995). 14. M. Fujii, S. Mitsushima, N. Kamiya, and K.Ota, Heat measurement during light water electrolysis using Pd/Ni rod cathodes, ICCF9, Beijing, China, May 19-24 (2002). 15. T. Hanawa, Z-ray Spectrometric Analysis of Carbon Arc products in Water, Proc. ICCF-8, Italy, 147 (2000). 16. X.Z. Li, Y. Deng, Y.J. Yan, H.F. Huang, W.Z. Yu, and C.X. Li, J. New Energy 6, 1, 80 (2001). 17. G.H. Miley, Product characteristics and energetics in Thin-Film electrolysis experiments, Proc. ICCF-7, Vancouver, Canada, 241, April 19-24 (1998). 18. R.L. Mills and S.P. Kneizys, Fusion Technol. 20, 65 (1991). 19. R. Mills, M. Nansteel, and P. Ray, J. Plasma Phys. 69, 131 (2003). 20. R. Mills, J. He, Z. Chang, H. Zea, K. Akhtar, Y. Lu, C. Jiang, and B. Dhandapani, Catalysis of Atomic Hydrogen to Novel Hydrides as a n New Power Source, 230 ACS National Meeting, Washington DC, Aug 28-Sept 1 (2005). 21. D.W. Mo, Q.S. Cai, L.M. Wang, and X.Z. Li, The Confirmation of Nuclear Transmutation Phenomenon in a Gas Loading H/Pd System Using NAA, ICCF-7, Vancouver, Canada, 105, April 19-24 (1998) 22. T. Mizuno, T. Ohmori, and A. Akimoto, Generation of Heat and Products During Plasma Electrolysis, ICCF-10 (2003). 23. V. Noninski, Fusion Technol. 2 1 , 163 (1992). 24. R. Notoya, Y. Noya, and T. Ohnishi, Fusion Technol. 26, 179 (1992). 25. R. Notoya, Nuclear Products of cold Fusion Caused by Electrolysis in Alkali Metallic Ions Solutions, Proc. ICCF-5, Monte-Carlo, Monaco, pp.531-538, April 9-13 (1995). 26. T. Ohmori and M. Enyo, Fusion Technol. 24, 293 (1993). 27. T. Ohmori and M. Enyo, J. New Energy 1, 15 (1996). 28. T. Ohmori and T. Mizuno, Observation of the Product Elements of Nuclear Transmutation Reaction on/in Several Metal Electrodes by the Cathodic Electrolysis in Light Water Solutions, ICCF-7, Vancouver, Canada, p. 109, April 19-24 (1998a). 29. T. Ohmori, T. Mizuno, Y. Nodasaka, and M. Enyo Fusion Technol. 33, 367 (1998). 30. T. Ohmori and T. Mizuno, Strong Excess Energy Evolution, New Elements Production, and Electromagnetic Wave and/or Neutron Emission in the Light Water Electrolysis with a Tungsten Cathode, Proc. ICCF-7, Vancouver, Canada, 279 (2000). 31. T. Ohmori, H. Yamada, S. Narita, and T. Mizuno, Excess Energy and Anomalous Concentration of K Isotopes in Potassium formed on/in a Re Electrode during the Plasma Electrolysis in K 2 C 0 3 / H 2 0 and K 2 C 0 3 / D 2 0 Solutions, Proc. ICCf-9, 284, May 19-24 (2002). 32. T. Ohmori and M. Enyo, Fusion Technol. 24, 293 (1993). 33. V. Violante, E. Castagna, C. Sibilia, S. Paoloni, and F. Sarto, Analysis Of NiHydride Thin Film After Surface Plasmons Generation By Laser Technique, ICCF 10 (2003).

43

34. H. Yamada, S. Narita, Y. Fujii, T. Sato, S. Sasaki, and T. Ohmori, Production of Ba and several Anomalous Elements in Pd under light Water Electrolysis, ICCF-9, Beijing, China, 123, May 19-24 (2002). 35. H. Yamada, S. Narita, H. Onodera, H. Suzuki, N. Tanaka, T. Nyui, and T. Ushirozawa, Analysis By Time-Of-Flight Secondary Ion Mass Spectroscopy For Nuclear Products In Hydrogen Penetration Through Palladium, ICCF10 (2003). 36. Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi, Observation of Low Energy Nuclear Reactions Induced By D2 Gas Permeation Through Pd Complexes, ICCF- 9, Beijing, China (2002). 37. G.H. Miley and P.J. Shrestha, Review of Transmutation Reactions in Solids, Proc. ICCF 10, Cambridge, MA, Aug 24-29 (2003). 38. G.H. Miley, P.J. Shrestha, and H. Hora, Current Trends in International Nuclear Research, (Ed.) E. Panarella, NRC Research Press, Ottawa, Canada (2003). 39. A.G. Lipson, A.B. Karabut, and A.S. Roussetsky, Anomalous enhancement of DDreaction, alpha emission and X-ray generation in the high current pulsing deuterium glow-discharge with Ti-cathode at the voltages ranging from 0.8-2.5 kV, ICCF-9, Beijing, China, (2002). 40. J.C. Fisher, Theory of Low-Temperature Particle Showers, ICCF-10, (2003). 41. H. Kozima, CF-Matter and the Cold Fusion Phenomenon, ICCF-10, (2003). 42. S.R. Chubb, Framework for Understanding LENR Processes, Using Conventional Condensed Matter Physics, ICCF-11, Marseille, France, (2004). 43. Black Light Power Inc. Website, accessed on 11/10/2005, http://www.blacklightpower.com/ techpapers.shtml. 44. G. Stoppini, Fusion Technol. 34, 81 (1998). 45. J. Dufour, J.H. Foos, and X.J.C. Dufour, Infinite Energy 4, 53 (1998).

DEVELOPMENT OF "DS-REACTOR" AS THE PRACTICAL REACTOR OF "COLD FUSION" BASED ON THE "DS-CELL" WITH "DS-CATHODE"

YOSHIAKI ARATA AND YUE-CHANG ZHANG Center for Advanced Science and Innovation, Osaka University, 2-1 Yamadaoka, Suita, Osaka 667-0871, Japan E-mail: arata@casi. osaka-u. ac.jp

It is well known that Double Structure Cathode ("DS-cathode") presented exactly evidence of strong cold fusion reaction, but could not use as the Practical Reactor because the most of the input energy is consumed inside the electrolyte as the energy loss; it means the "bad-efficiency". Then, to get "good-efficiency", we proposed a new "DS-cell" without the electrolyte, and named as the "DS-reactor" for this new DS-Cell to be utilized as the practical reactor. Therefore, it was concluded that DS-reactor adopted D2 gases with low temperature such as 100-200° C and suitable pressure of about 1—100 atm instead of D2 0-electrolyte as the nuclear fuel, and DS-reactor is constructed with following double structure, for instance, outer stainless-vessel and inner Pd-vessel. Moreover, DS-reactor is classified into two kinds of A-type and B-type based on the combination of between (sample and D2 gas) and (stainless-vessel and Pd-vessel); that is, A-type is combined to keep D2 gas inside outer vessel and sample inside Pd vessel with high vacuum condition and B-type is combination of D2 gas inside Pd-vessel and sample inside outer vessel. In this case, selection of the sample is the most important and should be adopted the sample to produce innumerable "Pycnodeuterium" inside the sample. Using the DS-reactor, existence of Cold Fusion was verified with "good-efficiency" to be utilized as the practical reactor.

1. Introduction In order to understand the function of the Double Structure Reactor (DS-reactor), it is important to know the principle of DS-cell/DS-cathode. 1 DS-cell is constructed with electrolyte ( D 2 0 / H 2 0 + LiOH) and DS-cathode together with Pt-cylindrical anode, and structure of DS-cathode is constructed with closed Pd-cylinder in which sample (nano Pd/Zr3NiO/Pd black, ...) is kept inside ultrahigh vacuum hollow space. When DS-cell is electrolyzed, the vacuum hollow space is filled up easily with ultrahigh pressure gas (D 2 /H 2 : 10 3 -10 4 atm) and the innumerable solid "Pycnodeuteriums" are produced inside the Sample.2 We discovered that the "Pycnodeuterium" cause easily nuclear reaction ("cold fusion") using not only DScell but also laser welding solid fusion reactor, sonoimplantation solid fusion reactor, 44

45

which were invented by us. However, these devices gave "bad efficiency; that is, their input energy was too large. Figure f shows principle of "DS-cell" and it will be given intuitive understanding for the principle. 3

© t

ID

12-

<>

Samples enclosed inside high vaccum Pd vessel

This white space becomes ultrahigh pressure Ds gas (~104 atm) in this patent

DS-cathode/DS cell for cold fusion

Figure 1.

Illustrated principle of "DS-cathode"/ "DS-cell"

Note: This is US-patent, 3 method of producing ultrahigh pressure; and it is realized by extremely pure deuterium with ultra-high over 10 000 atm pressure using electrolytic method. Fifty years ago, in 1955-1958, for the first time in Japan, we opened to the public the thermonuclear fusion experiment caused by generating several million centigrade degree with a current of several million ampere, which were the highest current and temperature in the world at that time. But Japanese could not buy deuterium gas in the market place at that time. Then, we generated deuterium gas by the same system of this device, which were made by oneself. This event was described in a US-magazine of the 21st century science and technology in detail. 4 Then, we thought this device will be used for cold fusion and named it "DScathode" / "DS-cell", then it can be easily understood intuitively relation between this US patent and "DS-cathode" / "DS-cell" from this figure. This situation was very important.

46

2. Graphic Illustration for "DS-Reactor" As already mentioned above, we had an idea that most of the input energy was consumed inside the electrolyte as energy loss, we proposed a new concept, which is a new DS-cell with no electrolyte. We call this new type DS-cell with no electrolyte as "DS-reactor". However, the principle is the same as shown in Fig. 2. "DSreactor" exhibited good results as we expected.

Q DS-cathode (Pd-olosed cylinder) © Anode (Pt-cylinder)

Heater

Heater

Pd vessel • Stainless steel vessel

DS-reactor Figure 2. "DS-reactor" was developed based on the "DS-cell", that is, the same principle in both methods. "DS-reactor" corresponds to "DS-cell" without electrolyte, and it is considered that "DS-reactor" includes A- and B-systems.

47

Two types of "DS-reactors" as shown in Fig. 2 are invented from "DS-cell". Upper side of the figure shows the usual "DS-cell" and the lower side diagrams describe A-type (left-hand side) and B-type (right-hand side) of "DS-reactors". Both "DS-reactors" are constructed with stainless vessel as outer vessel and Pd vessel as inner vessel as shown in the lower side of the diagram. D2/H2 gas is supplied to the gray zone space with high-vacuum conditions as indicated in A-type/B-type DS-reactors and kept to pressure, P atm, and temperature, T°C, that is (Pout, Tout) in A-type reactor and (P; n , Tin) in B-type reactor. Samples are set inside the white color zone space in both reactors, and after that, the samples and white space are kept in high-vacuum condition with the same condition in white zone of DS-cell (upper-side of the diagram).

Condition

(

No sample + D2

)

Pd vessel •

^

Sample: no sample 05/10/11-12 (purs Dj) Heat-Current \

•o

3

120 180 240 300 360 420 480 540 600 660 720

60 120 180 240 300 360 420 480 540 600 660 720

Time (min) Figure 3.

Time (min)

Characteristics of "DS-reactor" without sample during D2 gas charge.

Recently, we performed four kinds of experiments using the A-type "DS-reactor", and changed experimental conditions by setting different samples inside the inner vessel with white zone and different gases inside the outer vessel with gray zone. 3. Experiment 3.1. "Experiment-1"

([A]: No Sample + D2)

Figure 3 shows the results in the first set of the experiment. ("Experiment 1", [A]). In this case, inside the Pd vessel (white zone) is vacant (no sample) and D2 gas

48

filling up with 40 atm as the outside pressure (P ou t) of Pd vessel (gray zone) as the set-conditions before the experiment. When D 2 gas under P o u t of 40 atm is heated to 140°C as the giving temperature (Tout = 140°C), Pd vessel is heated by such D 2 gas accordingly, temperature of Pd vessel never goes higher temperature than the D 2 gas. When Pd vessel reaches to 70-100°C, D 2 molecules passing through the wall of Pd vessel as D + and enter inside the Pd vessel as D atom and becomes to mixed gas [D + D 2 (= D + D)] as time passes. As a final result, inner temperature of Pd vessel (white zone), T;n, never exceed the outer temperature as the giving temperature of the D 2 gas (gray zone), T o u t , that is always T out > T-m. These results were exactly confirmed by the experiment shown in Fig. 3, Namely, experimental results of left side AQ in Fig. 3 indicates the relation between D 2 gas pressure (P ou t = 40 atm) and temperature (T out = 140°C), which were supplied into the outside Pd-vessel (gray zone) and the penetrated inner D(D 2 ) gas pressure {P-m) and temperature (Tin) inside the Pd vessel (white zone), In other words, ( P n , T in ) never exceeds (P ou t, T o u t ): always P i n < P o u t and T in < T o u t . On the right-hand side Ai, only the scale of the temperature axis of Ao shown on left-hand side is enlarged to give distinct difference between Tout and T-m.

120 180 240 300 360 420 480 540 600 660 720

Time (min) Figure 4.

0

60 120 180 240 300 360 420 480 540 600 660 720 7

Time (min)

Comparison between figures A and B (Ai is the same with Ai in Fig. 3).

49

3.2. "Experiment-2"

([B]: Sample-)- H2) (Pd

black)

Bottom-right side diagram (Fig. 4, Bi) is the experimental result of the second set-condition (Experiment 2; [B]) with sample Pd black + H 2 . This means Pd black is set as a sample inside the Pd vessel (white zone) and kept under high-vacuum condition, and H2 gas with 40 atm is filled up as the outside pressure (P0ut) of the Pd vessel (gray zone) as the set-conditions before experiment. The experiment was performed under the same process of (Experiment 1, [A]). When H 2 gas is given with P ou t of 40 atm and Tout of 140°C inside the gray zone, H atoms penetrated into the Pd vessel are absorbed inside the Pd black, and the temperature difference T as Tout-Tin becomes a little smaller than that in (Experiment1; [A]) as shown in the relation between data Ai and Bi in the bottom side diagram (A and B in Fig. 4); here, both Ai in Figs. 3 and 4 are the same diagram. As a result, inner temperature Xin was always lower than given temperature -*- out; -^ out ^ -^ in-

And both temperatures were never reversed. This result is extremely important. We have expected that nano Pd is far better than Pd black as a sample because 1,2 we have obtained that nano Pd generated excess heat with much higher rate than

D (

Sample: nano Pd + D2

Sample: Pd black; gas: D; " \ W N —

141

• : Sample: Pd black » 05/10/11-12 (pure D2)

/"in

ff

140 139

/ Heat-Current \ \ stop )

'out

-0 Pout

13R

^

™

137

.

^^--^

?

Tl

: tem

2. Q-

sure

Pi

134

^3

CO

136

hf

TO

CD

=s

m

135

O ?

a -! '

h-°

v

133

,-

h~

132 131

/ 0

60 120 180 240 300 360 420 480 540 600 660 720 780 840

Time (min)

Figure 5.

) 120180 240 300 360 420 480 540 600 660 720 780 840

Time (min)

Comparison between figures C and D.

50

that of Pd black using "DS-cell" with "DS-cathode". Experimented data can be compared with Di in ("Experiment 4", [D]) and Ci in (Experiment 3, [C]) and T;n* becomes considerable higher than T o u t in case of Di experiment against Ci experiment as shown in Fig. 5. Moreover, T;n* in Di pulled up even the first giving temperature (T out ) of 140°C to over 180°C. It is concluded that "DS-reactor" will be workable as a "practical reactor".

3.3. "Experiment-3"([C]: sample "Experiment 4"([D]: sample

(Pd black) + D2) and (nano-Pd) + D2)

Figure 5(C) in the bottom-side shows the experimental result of the third setcondition: (Experiment 3; [C]), with sample Pd black + D 2 . This means D 2 gas is used instead of H 2 gas under the same condition as (Experiment 2, [B]). As a result, wonderful phenomena were produced that temperature inside Pd vessel (T n *) becomes higher than the giving temperature, T o u t , when the D 2 gas was supplied into the gray zone (outside of Pd vessel), that is T;n* > T o u t . Experiment's data can be compared with Ci in Fig. 5 and Bi in Fig. 4. That is, compared with the functions of H 2 gas and D 2 gas which induced "temperature inversion'" inside the Pd vessel (white zone) against the giving temperature (T out ) when the D 2 gas was supplied to outside Pd vessel (gray zone). This result clearly means generation of "pycnodeuterium nuclear reaction" inside Pd vessel (white zone). Figure 5(D) shows the experimental results of the forth-set condition ("Experiment 4", [D]) with sample of "nano Pd"+D 2 . We have already reported that D2/H2 gas can be much more absorbed inside nano Pd than Pd black and innumerable "pycnodeutrium" can be produced inside nano Pd. 1 ' 2

3.4. Fundamental

Characteristics

Between

(T-m, TOVLt) and (P-m,

Pout)

Figure 6 shows the summary of the experimental data of the temperatures and the pressures demonstrated through the (Experiments 1-4). In the case of without D 2 or without the sample such as Pd fine powder, Tin never went higher than the given temperature T o u t . On the other hand, when the samples produced "pycnodeuterium", T n was always higher than T ou t, that is, caused the temperature inversion. It is also noted that the degree of this excess of temperature depends on the type of the host material; that is whether the host materials can absorb much pycnodeuterium or not. In other words, "DS-reactor" certainly displayed the similar basic characteristics of the "DS-cell", but it gave the excellent characteristics as the fusion reactor much more clearly.

51

Summary of experimental data

0£>0iM

TV. ( Sample+D 2 ) Dependence on samples Nuclear fission zone ) No sample + D2 Sample + H2

Sample

Figure 6. Illustration of fundamental characteristics between gaseous temperature (T; n , T o u t) and pressure (Pi n , Pout) in "DS-reactor".

4. Conclusion Figure 7 shows the conclusion of the experiments already described, and demonstrates the present situation of "DS-reactor" as the practical reactor of "coldfusion". From the left-hand side of the horizontal line, the thick black and thin black dots correspond to Experiments 1-4. The vertical axis represents the T;n, which is inner temperature in the gray zone of the DS-reactor. For Experiments 1 and 2, Tjn's are lower than T o u t , that is, the efficiencies are always negative. For Experiments 3 and 4, T in *'s are higher than the given temperature T o u t . This means that these efficiencies were always positive and moreover, almost of the input energy was collectable. It is emphasized that T;n for Experiments 1 and 2 are always lower than T o u t and higher for Experiments 3 and 4. The excess energy obtained with the Experiments 3 and 4 should come from deuterium nuclear fusion reaction. What else explanation exists for this result? Chemical reaction energy is very small and never gives the explanation. We concluded that this should come from fusion. Also it is considered that the "DS-reactor" demonstrated to reach the practical level with high efficiency. It was concluded that the principles of the DS-reactor is the same as that of DS-cell with "DS-cathode", and the "DS-cell" was an excellent system to

52

Outer vessel D 2 /H 2 gas

Pd vessel

The present situation of DS-reactor as the practical reactor of Cold Fusion Generation of nuclear energy inside Pd-vessel

/Nano Pd\ V D2 gas /

(outer vessel)

/Pdblack\ \ D2 gas / Temperature given to outside (D2/H2 gas) (7 0u t> 100°C)<8> of Pd-reactor vessel

® I Pd black\ /Nilo sampleN D 2 gas

^ H2 gas /

- Actual basic line for (sample + D 3 gas) T=

T„+T*„,

/

Tin Never nuclear reaction

Figure 7.

Illustration of "Conclusion".

demonstrate exactly the existence of cold fusion, but gives a bad "efficiency" as a reactor, because in DS-cell, electrolyte is used essentially, then the most of the input energy is consumed inside the electrolyte itself, and then consequently, the "DS-reactor" which is "DS-cell" with no electrolyte will be utilized as a Practical Reactor. 5. Supplement: Measurement System of the Input/Output Power and Characteristics of Reacted Products for the DS-Reactor To keep the constant "giving temperature" (T out = constant), heating current should be changed automatically for the heater with always-const ant resistor. We set a new system to keep the constant "T o u t ", and measured its current transition as shown in Fig. 8, where the input power (W;n) is simply converted by a formula [Win = RI2, R is the constant resistance (50£1) and I is the measured current (A)]. When T out = 140°C, input power was about 1-2 W which is about 1-2% for the DS-cathode, but it is considered that when the radiation loss to the air is protected it will be decreased at the extremely small (%). These results show great characteristics of the DS-reactor as the practical use. Figure 9 shows generation of the much 4 He inside the DS-reactor with D2 gas and Pd black. Above A shows the starting base condition of "QMS" before the

53

Heater controlling system

/^->

Tcout

Heater Sample: Pd black; gas: D2

160-, 140-

0.8 -24

0.7- -22

T ^ n ^

-20

£Jr

7"out

0.6-

10080-

-18

0.5- -16

Current (A)

Temperature (°C)

120-

-14

0.4- -12 0.3-

60-

-10

1

-8 40 H

Current

/

Input power

Win

0.2- - 6

- -4 20-

0-

1

c

50

100

150

200

0.1- 9

•

250

• 0.0- - 0 300

*

Time (min) Figure 8. Characteristics of controlling current (input power) to make the constant "giving temperature".

reacted is injected into the "QMS". The period between B and C shows a part of M4-spectrum of the reacted gas, (the gas volume 5 Torr cm 3 ) which was injected to the special gas tank (volume 2000 cm 3 ) with Getter pump and the high vacuum 10~ 8 Torr, and the gas was kept inside the tank, 3 min, then the gases were injected into "closed QMS" (which was developed and published by us in 1995), And one pair spectrum of M4 (4He, D2) was more exactly shown in the period between C and D. The period from D to E exhibits the spectrums, 15 min, after starting, and remained almost of only He.

54

8x10"

c CD

4x10" 12

Figure 9. Spectral analysis of the inner gases in the "DS-reactor" using sample (Pd black) and D 2 gas. Acknowledgments The authors would like to t h a n k Dr. T. Yokobori, M. J. A. (Emeritus Professor; Tohoku University), Dr. T. Yamazaki, M. J. A. (Emeritus Professor; Tokyo University), Dr. H. Fujita, M. J. A. (Emeritus Professor; Osaka University), Dr. A. Inoue (Vice President, Professor; Tohoku University), and Dr. M. F u t a m a t a (Professor; Kitami Institute of Technology) for their kind cooperation.

References 1. Y. Arata and Y. C. Zhang: Proc. Japan Acad., 70B, 106 (1994); 71B, 304 (1995); J. High Temp. Soc. Jpn. 20, 148 (1994); (Special Vol.) 23, 1-56 (1997); (Special Vol.) 29, 1-44 (2003); Jpn. J. Appl. Phys. 37, L1274 (1998); 38, L774 (1999); 39, L4198 (2000). 2. Y. Arata and Y. C. Zhang: J. High Temp. Soc. Jpn. (Special Vol.) 29, 1-44 (2003); Y. Arata, II Nuovo Saggiatore (Italy phys. Soc) 20, 66 (2004). 3. Y. Arata, Methode of producing ultrahigh pressure gas, US-Patent, No.5, 647, 970 (1997). 4. 21st. Century Science and Technology, Summer (21st Century Science. Associates, Washington DC, 1995), p. 37.

P R O G R E S S IN EXCESS OF P O W E R E X P E R I M E N T S W I T H ELECTROCHEMICAL LOADING OF D E U T E R I U M IN PALLADIUM

V. V I O L A N T E A N D S. M O R E T T I * Associazione

EURATOM-ENEA

sulla Fusione, Centro Ricerche Frascati, Rome, Italy E-mail: [email protected]

Frascati,

C.P.

65-00044

M. B E R T O L O T T I , E. C A S T A G N A , A N D C. SIBILIA Universita

di Roma

"La Sapienza"

Dip. di Energetica.

Via A. Scarpa,

14, Rome,

Italy

F. SARTO ENEA,

Centro Ricerche

Casaccia

Rome,

Italy

M. M C K U B R E A N D F . T A N Z E L L A SRI International,

333 Ravenswood

Avenue,

Menlo Park,

CA 94025,

USA

I. D A R D I K , S. L E S I N , A N D T. ZILOV Energetics

LLC,

7 Fieldview

Lane,

California, NJ, USA or Energetic Industrial Park, Israel

Technologies,

Omer

A research activity has been carried out, during the last 3 years, in the field of triggering anomalous heat effects in palladium deuteride. An enhancement of the excess of power reproducibility in deuterated palladium was obtained by using He—Ne Laser irradiation during electrochemical loading. A preliminary correlation between excess of energy and 4 He concentration increasing above the background was found. The continuation of the experimental program confirmed that Laser triggering produce an interesting gain of reproducibility. An upgrade of the experimental set-up has been realized.

1. Introduction The material science research oriented to improve the effect of excess of power production into palladium cathodes loaded electrochemically with deuterium confirmed that the high concentration of deuterium into the lattice (d/Pd > 0.9) is a necessary condition to observe the phenomenon but not enough. Several research groups have been working in order to identify the most appropriate techniques to trigger *ENEA guest. 55

56

such an effect. The study presented in this work is leading with the development of the triggering by means of Laser irradiation during the electrochemical loading of palladium with deuterium in heavy water electrolyte. An isoperibolic calorimetric system has been developed allowing a Laser irradiation during the electrochemical loading. According to the idea that collective electron oscillations have a key role in LENR processes a proper trigger has been introduced to create surface plasmons (polaritons). 1 Laser triggering was selected because of it results to be the most appropriate under electrochemical loading. Plasmons are longitudinal plasma oscillations that do not couple with external radiation. A proper surface corrugation may produce such a coupling between the electronic oscillation and the external radiation. For such a reason, a proper acid etching has been done on the Pd samples used as cathodes into the electrochemical cell. In addition to that one may consider that a p-polarized Laser beam is the appropriate one to create charge separation on the surface of the specimen. High vaccum cap with electric connections < PT100--

Electrodes rotating support

PT100

SS cap and ring

Glass window for laser beam

Teflon cell

Figure 1.

Electrochemical cell for Laser triggering.

2. Experiments The electrochemical cell (Fig. 1), tested for He leakage (2 x 10~ 10 mbar 1/s), equipped with two small glass windows was placed into a thermostatic box (Fig. 2) (±0.15°C) also equipped with a window for the Laser beam (5 or 33 mW, 632 nm). The closed electrochemical cell is equipped with a recombiner. Cell power supply is an AMEL galvanostat, modulated, during the HI-LO current mode by an HP 33120 wave function generator. Output power is measured by means of the calibration performed by means of the average temperature given by the PT100 thermometers

57

mm wi LCR meter

'—-

1—

Wave generator

....

Temperature monitor Multimeter Data acquisition switch unit

ff-

Laser

Box

Galvanostat Figure 2.

Isoperibolic calorimeter.

located into the electrolyte, R/RQ measurement is done by means of a HP-4284 (four wires measurement). A calibration was done by using light water (0.1 M LiOH) and the calibration curve is shown in Fig. 3. Despites the behavior of the system was quite linear a proper fitting curve has been used in order to have R2 = 1. Three experiments have been carried out into the isoperibolic calorimetric system during the first campaign showing excess of power production during Laser irradiation with "p" -polarization. The produced excess of energy was ranging between 3.4 and 30 kJ. Figure 4 shows the input and output power and energy of Laser 4 experiment. The increasing of He concentration measured with a Jeol GCMate mass spectrometer revealed a satisfactory agreement between the expected value and the measured one by assuming a D + D = 4 He + heat reaction occurring into the lattice. 2 Calibration 25-5-2004 y=-0.1649x= + 5.3626X+ 24.337fl° = 1

60-

^^--Jr'

o S_ 30-

^—* ^^^^"^ —*-T (average)

^ "

- — Pdi. (T (average))

2010-

(

1

2

3

4

5

6

Pin ( W )

Figure 3.

Calibration curve for isoperibolic calorimeter.

58

An improvement of the system was carried out both to increase the number of thermometers into the cell and to use high ultra-vacuum technology for the cap and the glass windows of the cell. A particular effort was done in order to take into account the convective heat exchange due to the electrolyte fluid dynamics due to the gas bubble formation during the electrochemical process. Laser 4 experiment was carried out by applying a continuous electrochemical current. After achieving a loading threshold of 0.95, the cathode was continuously irradiated by using a 632 nm, 33 mW red Laser. Calorimetry gave 30.3 kJ of produced energy (19.4 MJ per mol Pd). Figure 4 shows the input and output power and energy evolution after applying the Laser irradiation. Excess of energy and power in Iaser4 experiment

Figure 4.

Excess of energy and excess of power in Laser 4 experiment.

The gas produced at the electrodes (Pd foil cathode and Pt wire anode) acts on the electrolyte producing a fluid dynamic regime that affects the temperature distribution, then the temperature field for the considered cell results to be correctly described by including the convective terms into the heat transfer equation: dT ( dT dT dT\ div(Xgrad(T)) + Q = pcp— + pcp [Vx— + Vy— +Vz—j,

(1)

with convective external boundary conditions (radiative mechanism is neglected because of the low temperature of the system, close to the ambient one). Assumptions • 3D transient. • Isotropic (Kx = Ky = Kz).

59

• Steady-state boundary conditions (thermostatic box) Tarab = cost. (£). • Radiative heat exchange negligible • Convection of the electrolyte mainly produced by the bubbles formation at the cathode, since the cathode has a reduced area and the deuterium flow rate is twice the flow rate of the oxygen at the anode. In order to reduce the computation time, we propose an approximate solution, in closed form, for the field of velocity. First of all, we have to calculate the velocity of the electrolyte at the interface between the hydrogen and the liquid. The situation is described in Fig. 5.

Figure 5.

Gas-liquid interface at the cathode.

Gas velocity Va2 is calculated by means of the current density. Let us assume the cathode to be a Pd foil having height h and width L. The bubbles of hydrogen form a layer that we measured to be S (2-3 mm) in our cell configuration. The laws of Faraday and of the gas give 22.4 x 1000 cm 3 /s, n = 2.

gas flow rate =

(2)

nF The gas flow rate for unit area is: „ K=

J x 22.4 x 1000 _ , „ = 2.

(3)

By integrating on the whole surface <5 it follows: W=

f LKdz Jo

= LKz.

(4)

60

So that the gas velocity is

- YL ~ K - L*£± _ vgas{z) - A - LS - u -

Kz s

(5)

.

In the specific case under study the motion and continuity equations read respectively: dv

1 d 1

r

A

= 0

(6)

r dr \ dr J dvr dvz dr dz

(7)

;-4=

Ilrmm_

••---

8.00 7.50 6.50 6.00 5.50 5.00 4.50 4.00 3.50 3.00 2.50 2.00 1.50 1.00 0.50 0.00

Figure 6. Velocity field into the electrochemical cell due to bubbles at the cathode.

The approximate solution will be carried out by solving iteratively the two equations with the following assumptions: • • • •

axial symmetry, density and viscosity be constant, steady state, negligible effect of pressure and mass.

The velocity of the liquid in contact with gas is estimated as 3 - 5 VA

V?

IO„B 12/^ ii + 7/iiE K

0.093,

(8)

where 9 x 106 Pa s, = 1.095 x 1 0 ~ 3 P a s ,

(9)

then V*

0.093V1

(10)

61

Step 1: - • — ( r—— ) = 0 (motion equation). (11) r or \ or J Solving the equation with the following BC vz = VQZ\ r = a, vz = 0 per r = R it follows: , „ V0 V0 -lnr uz = - I n i ? • - — — - + -—-—-. in (a/r) in (a/r)

(12)

Step 2: 1

C/V

(Jl)

-vr + — h -7-^ = 0 r o r oz

(continuity equation).

By calculating the derivative of w^and by taking into account that VQ(Z) = dvz dz

K InR 5 In (a/R)

K lnr 5 In (a/R)

K\n{r/R) 5 In (a/R):

(13) Kz/6, (14)

the substitution of (14) into the continuity equation leads to ()_C1n_ Vr{r

>-

JTr-[21n(r/r)-l] 46ln(a/R) '

r

'(15)

The integration constant is calculated by imposing the condition of zero flow rate in radial direction

2nh /

vr dr = 0 that gives the value of C I R :

(16)

Ja

IK

ClR

a2-R2+a2HR/a)

^"4T

jj^jf

'

(17)

Step 3: By replacing again vr(r) into the continuity equation we obtain VVz(r,z), the integration constant is calculated by considering now zero flow rate into the axial direction VVz(r,z) = -zK2ln^+Clz, 2?r / VVz{r,z)rdr = 0, Ja \ „ (a2-R2 + 2lnR/a)

2* 2 * 1

n£

IJ

^W

(18) (19)

62

Ifl

J~~l_

sX Temp on

0

3

max: 314.9 q: 314.0 p: 313.0 o; 312.0 n: 311.0 m: 310.0 I: 309.0 k: 308.0 j : 307.0 i: 306.0 h: 305.0 g: 304.0 f; 303.0 e: 302.0 d: 301.0 c: 300.0 b: 299.0 a: 298.0 min: 297,7

6

Y

Figure 7.

Temperature field into the cell (isotherms).

The two components of the liquid velocity are VVz and Vr Cm *(') = VVz{r,z)

Kr[2\n(r/R)-1] ASHa/R)

= -zK2ln(r/R)

+ Clz,

'

IK 45

Cl R

1 2

d

— J\oZ

a2 - R2 + a2 hx(R/a) [\n(R/a)]' (a2 -R2 + 2 In R/a) — a? -R

(21) and describe the velocity field into the electrolyte (see Fig. 6). A three-dimensional (3D) transient finite element analysis gives the field of temperatures into the cell, Fig. 7 shows the temperature distribution into the electrochemical cell. Figure 8 shows the comparison between the experimental results and the calculations, the comparison reveals a satisfactory agreement when the fluid dynamic

Model

p

*- Model without fluid-dynamics a - Experiment it- Model no fluid-dynamics

P(W) Figure 8.

Comparison between model results and experimental data.

63

of the electrolyte is included into the system description, in particular for power values larger t h a n 2 W. A new experimental campaign has been carried out giving one excess of power production over two experiments. T h e excess of power is shown in Fig. 9. T h e effects started after achieving a loading around D / P d = 0.94 and survived, under Laser irradiation for more t h e n 100 h. T h e maximum gain was about 15% of the input. T h e excess was stopped by current inversion t h a t produced a fast de-loading. After de-loading the difference between the input and the o u t p u t power disappeared. T h e effect is clearly shown in Fig. 9. T h e total energy gain was 49 kJ.

149 kJ excess of

Current

0.9 0.8

"W.WW

0.7

R/Ro<

0.6

5

- Pin (W) Pout (W)

0.5

I 0.4 0.3 0.2 0.1 50

100

150

200

250

300

Time (h)

Figure 9. Excess of power production under He—Ne Laser irradiation.

3.

Conclusions

T h e results of the additional investigation performed with the new experimental campaign are in good agreement with the results obtained into the first run of the work. It is confirmed t h a t the relevant effect of the Laser trigger, under appropriate conditions, to obtain excess of power production in deuterated palladium when the D concentration is close to the literature threshold. References 1. V. Violante et al., Analysis of Ni-hydride thin film after surface plasmons generation by laser technique, in Tenth International Conference on Cold Fusion, Cambridge, MA: LENR-CANR.org, 2003.

64

2. M. Apicella et at, Some recent results at ENEA, 12th International Conference on Condensed Matter Nuclear Science (ICCF12), Yokohama, Japan, November 27 - December 2 (2005). 3. T. J. Hanratty and J.M. Engen, A.I.Ch.E. Journal 3, 299-304 (1957). 4. A.D.JK. Laird, Trans ASME 76, 1005-1010 (1954). 5. S. Calvert and B. Williams, A.I.Ch.E. Journal 1, 78-96 (1955).

A N O M A L O U S E N E R G Y GENERATION D U R I N G C O N V E N T I O N A L ELECTROLYSIS

TADAHIKO MIZUNO AND YU TORIYABE Department

of. Engineering, Hokkaido University, Kita 13, Nishi 8, Sapporo 060-8589, Japan E-mail: [email protected]

Kita-ku,

We experienced an explosive energy release during a conventional electrolysis experiment. The cell was a 1000 cm 3 Pyrex glass vessel that has been in use for 5 years. It contained 700 cm 3 of 0.2 M K2CO3 electrolyte; a platinum mesh anode; and a tungsten cathode wire 1.5 mm in diameter, 29 cm long, with 3 cm exposed to the electrolyte. The estimated heat out was 800 times higher than input power, based on the data recorded up to the moment of the event. There were many elements deposited on the electrode surface. The major elements were Ca and S and the total mol was roughly estimated as 10 — 6 .

1. Introduction The cell was placed inside a constant temperature air-cooled incubator (Yamato 1L-6) with the outer door open, and the inner Plexiglas safety door closed. The event occurred in the first stage of the experiment before plasma normally forms. Soon after ordinary electrolysis began, voltage was increased to 20 V and current rose up to 1.5 A. Within 10 s, the cell temperature rose steeply up to 80°C and a bright white flash surrounded the cathode. The light expanded to the solution and at the same instant the cell exploded. The explosion blew off the Plexiglas safety door and spread shards of Pyrex glass and electrolyte up to 5-6 m into the surrounding area. The cell is equipped with a magnetic stirrer and the fluid mixes rapidly. Three separate platinum resistance temperature detectors (RTD) in the electrolyte all recorded ^80°C just before the explosion. This means the water in the cell was well mixed and the entire 700 ml volume of water heated up from 30°C to 80°C in 10 s. This is 35,000 calories or 147,000 J, which is ~800 more energy than was input into the cell before the explosion. Table 1 shows the rapid temperature rise recorded by the three RTDs just prior to the explosion, and it also shows that the fluid was well mixed. The effluent hydrogen and oxygen were mixed in the cell headspace. (Note that the inverted funnel described in Ref. 1 was not in use during this experiment.) There were 2-3 cm 3 of free hydrogen at the time, although this is an open cell so only minimal amounts of gas remain in the headspace. Oxygen gas and hydrogen gas were also mixed in with the electrolyte solution. It is likely that the platinum mesh 65

66 Table 1. Last four RTD electrolyte temperature readings prior to explosion. Seconds before explosion RTD number RTD-1 RTD-2 RTD-3

20 s

15 s

10 s

5s

30.0 29.4 31.1

32.1 31.9 32.5

50.4 48.6 50.1

80.1 82.2 78.3

anode catalyzed the hydrogen and oxygen to recombine rapidly in the electrolyte, triggering the explosion in the headspace. The vessel was old and may have had a scratch on the inner surface. It is possible that the tungsten cathode may have been exposed to the gas in the headspace. 2. Experiment 2.1. Electrolysis

Cell

Figure 1 shows the experimental setup, which is described in Refs. 1 and 2. We measure many parameters including sample surface temperature, neutron and Xray emission, mass spectrum of gas, input and output power, and so on. Figure 2 shows the schematic sketch of the cell and gas measurement system. 1 ' 2 The cell is made of Pyrex glass. It is 10 cm diameter and 17 cm in height and 1000 cm 3 in solution capacity. It is closed with a Teflon rubber cap, 7 cm in diameter. The cap has several holes in it, three for platinum resistance temperature detectors (RTD) (Netsushin Co., Plamic Pt-100 Jl), two for the inlet and outlet of the flowing coolant water, and one to hold a funnel that captures the effluent gas from the cathode. The funnel is made of quartz glass, and is 5 cm in the diameter at the top of the cell, and 12 cm in length. Gas leaving from the top of the funnel flows into a water-cooled condenser, which is connected to the funnel with another Teflon rubber cap.

\

Figure 1.

">VEimgen gas

Experimental setup.

67

Flow meter, mass spectrometer Cooler outlet Cooler inlet Teflon rubber cap Electrolyte cap Shrinkable teflon cover

Figure 2.

Detail of gas measurement

We measured several parameters, including the rate of gas flow, temperature of the sample surface, mass spectrum of gas, and input power. The measurement system was described elsewhere. 1 ' 4 The electrolyte was composed by basic K2CO3 solution and the volume was 700 cm 3 . Plasma discharge was changed by input voltage up to 350 V. The gas generated by the plasma discharge was continuously analyzed by the quadrupole mass spectrometer. 2.2. Measurement

of Hydrogen

Gas

A mixture of steam, hydrogen, and oxygen (from pyrolysis) passes from the cell to the condenser. The steam condenses and falls back into the cell. An 8-mm diameter Tigon tube is coupled with the gas exit of the condenser, connecting it to a gas flow meter (Kofloc Co., model 3100; controller: Kofloc Co., model CR-700). The flow to voltage transformer element is a heated tube of thermal flow meter system, the minimum detection rate of hydrogen gas flow is 0.001 cm 3 /s, and the resolution is within 1%. The power output from the measurement system was led to the computer through a logger. After the gas passes through the flow meter, a small constant volume of it, approximately 0.001 cm 3 /s, passes through a needle valve and is analyzed by the quadruple mass spectrometer. The rest of the gas is vented. The main composition of gas released from the cathode was then continuously analyzed by the above-mentioned method. 2.3.

Calorimetry

Temperature measurements were made with 1.5 mm diameter RTDs. Calorimetry was performed by combining the flow and isoperibolic method. Flow calorimetry is based on the temperature change of the cooling water. The cooling water is tap water flowing through Tigon tubing. It passes first through a constant temperature

68

bath to keep the temperature constant. Prom there, it flows through the outer jacket of the condenser, and then through the coil of tubing wrapped around the funnel. (The outside of this cooling water coil is covered with the anode, a platinum mesh.) The flow rate is measured with a turbine meter (Japan Flow Control Ltd., model T-1965B). The inlet temperature is measured before the cooling water enters the condenser, and outlet temperature is measured, where it exits the cell. Heat from both condensation and glow discharge electrolysis is combined together. Isoperibolic calorimetry is performed by placing three other RTDs in the cell electrolyte at different depths in the solution to measure the temperature. The solution is mixed with a magnetic stirrer. Figure 3 shows the notional sketch for heat measurement. Heat out can be divided into several factors. These are energy for water decomposition, heat of electrolyte, heat bring by the coolant, heat releasing from the cell wall and heat releasing with the vapor through the cell plug.

*-«J " M i l ! J" £'J3V1!U

t'iflUi

.it: •

„..

'I ' ! ( M t !E-3'e-tlS:>

_

f

•

-

'

;i ,i,

•i;j l o c i .v i

^JL.,^J,

Hw: « « « % $ # JWfli

Figure 3.

Schematic representation of heat balance.

The heat balance is estimated by input and output formulas, input and output power is given in the following equations: Input (J) = I (current) x V (Volt) x t, Out Hg + Hw + HC + Hx, here Hg = Heat of decomposition = / 1.48 dl dt, Hw = Electrolyte heat = / Ww Cw dT,

69

Ww is the electrolyte weight, C w the heat capacity, and dT is the temperature difference. Hc = Heat of coolant = / Wc Cc dT, Wc is the coolant weight, Cc the heat capacity, and dT is the temperature difference. HT = Heat release = f {WWCW + WCCC)TT; where Tr is the temperature change. The heat balance calculation is straightforward. Input power is only from the electric power source. Output is divided into several parts. The first factor is heat of water decomposition (designated Hg). It is easily calculated from the total electric current. The second factor is electrolyte enthalpy (Hw). It is easily derived from the solution temperature difference. The third factor is heat removed by the coolant (Hc). This is measured from the temperature difference between the coolant inlet and outlet, and the coolant flow rate. The fourth factor is heat release from the cell (HT). This is rather complicated and can be estimated with a semiempirical equation. We measured most of the heat in the condenser directly by monitoring the inlet and outlet temperature of the cooling water that passes through the condenser outer jacket. If there is a mixture of various gases, we have to measure the gas composition precisely, because even a small volume of gas generated by pyrolysis will remove a large amount of enthalpy. This was done with the precision gas flow meter and mass analysis. The first factor, water decomposition (Hs) has a large effect on the rest of the equation. 2.4. Electrode

and

Solution

The electrode is tungsten wire, 1.5 mm in diameter and 15 cm in length. The upper 13 cm of the wire is covered with shrink-wrap Teflon and the bottom 2 cm is exposed to the electrolyte and acts as an electrode. During electrolysis, the sample wire was consumed. The electrolyte solution was made from high purity K2CO3 reagent at 0.2 M concentration. 2.5. Power

Supply

The power supply was a model of EH1500H made by Takasago Co. Ltd. The electric power was collected with a power meter (Yokogawa Co., model PZ4000) in every 5 s. The electric power was measured in each 40 us, and the average of 100,000 values were recorded at 5-second intervals. 2.6. Data

Collection

All data, including the mass of cooling water flow from the flow calorimetry, the temperature of coolant entrance, and exit, electrolyte temperature measured by three RTDs, input voltage, current, electric power, and the amount of the hydrogen

70

gas generated were collected by a data logger (Agilent Co., model 34970A), and stored in a personal computer. 2.7. Element

Analysis

The sample electrodes and the electrolyte were subjected to element analysis by means of energy dispersion X-ray spectroscopy (EDX), Auger electron spectroscopy (AES), secondary ion mass spectroscopy (SIMS) and electron probe micro analyzer (EPMA).

Parameter change 300

1! 200

o c 55

1 O =>

=5

100

0) Q.

E 2 cf data ¥W 40803 # 1 Figure 4.

2.8. Mass

4 Time (1000 s)

Changes of voltage, cell temperature, and current.

Analysis

The generated gas was continuously analyzed a quadrapole mass analysis. A small amount of gas was introduced into a differential evacuation system and then brought to the mass analysis measurement system. We used mass analysis of Ulvac Rega-201 that is a mass filter type of Quadrapole mass analyzer. The analyzer can measure mass number from 2 to 400. 3. R e s u l t s a n d Discussion Figure 4 shows the changes of input voltage, cell temperature, and current for a typical experiment. Input voltage was usually increased stepwise from 0 V to more than 100 V and then decreased to 0 V. The input current usually rose to a maximum

71

Parameter change 100

>

6

— Cell temp.

80

0)

2

60

C

ro O

llf ro a. £

/

-

V

4

Current (A)

i

•-

3

40

2

^

S 20

|2

/•

0 1! 0

/

i

i ^

15 0

1

//' i

I""""""1 A

• 1

i

190

210

'u 250

2. 0

!ime(s)

Figure 5.

Time expanded graph of Fig. 4.

value of 4.3 A during conventional electrolysis with 1 cm 2 area of W electrode, but it usually decreased once plasma started, and stayed around 1.6 A when voltage ranged from 120 to 220 V. The time-expanded graph of Fig. 4 is shown in Fig. 5. It indicates input voltage, current, and temperature changes for the first 250 s in Fig. 4. Here, input voltage is increased at 182 s and reached to 40 V at 220 s, and at the same time, current increased to 1.8 A. Meanwhile, electrolyte temperature raise is within Idegree, it can be say almost constant.

100

f

80

— Terr

t»

>

5

I

J\ I

-- Cur 60

-Volt

1

1 J- \

20

1

n

c

23

| ddaia\\V»l24«l |

Figure 6.

\

A0

\

V^

1

40

!

4

3

g 3

2

>

1

. * ,

60

i

80

0 1 )0

Time (s)

Changes of voltage, cell temperature and current.

72

Changes of input and output 1E + 05

t

/

1E + 0 4 k

5

B"3 o 1

•#• Input

/

F 1E + 03

-©-Outpu t

/ /

| / 1E + 02

i /

1E + 01 y

L

J

1

# ;*A

20

1

L_L_

1

40

60

1

L

80

1 100

Time (s)

rcfdata\W50l24#l I

Figure 7.

Changes in input and output heat.

However, the changes of temperature during the explosive reaction were different from the usual experiment. The input voltage and current were 15 V and 1.5 A at 40 s, respectively; that equals 22.5 W, as shown in Fig. 8. The input power was supplied for 10 s; total input was roughly 300 J. The electrolyte temperature rose steeply from 40 to 60 s, within 20 s. After that, the electrolyte cell was shattered by the sharp increase of inner pressure. The heat out was estimated 800 times higher than the input power, based on the remaining output data. ,<^:

EDX aliased

Figure 8.

Electrode; above: before, bottom: after.

73

EDX spectrum

— I Before

1E + 05rr

1E + 04

O 1E + 03

^

1E + 02U

1

1

1

1

1 5

1

L

10

15

Energy (keV)

Figure 9.

EDX spectra for W before experiment.

There were many elements deposited on the electrode surface. The major elements were Ca and S and the total mol was roughly estimated at 10~ 6 , as shown in Fig. 10.

-Tip

EDX spectrum 1E + 05

1E + 04

1E + 03

1E + 02 l-J

1

J

1

I

5

I

!

I

I

10 Energy (keV)

Figure 10.

EDX spectra for W after experiment.

I

l_

15

74

If we assume the reaction occurred by the T S C mechanism, then the reaction products of a common isotope of tungsten would be as follows: 182W

+ 4

i

H

_> i s o T e + 5 6

F e+

- • 136Xe +50

-> -• -•

138

128_6

C r+ n

7

M e V

4

Me

y

48

B a + T i + 1 1 7 . 4 MeV Ce + 4 4 Ca + 107.2 MeV 154 S m + 3 2 S + 7 9 . 2 MeV 142

^158Gd+28gi+727MeV

However, it is still difficult t o explain the reaction by this mechanism, because of the absence of heavier pair elements.

References 1. Tadahiko Mizuno, Tadayoshi Ohmori, Tadashi Akimoto, and Akito Takahashi, Production of heat during plasma electrolysis in liquid, Jpn. J. Appl. Phys. 39, 6055-6061 (2000). 2. Tadahiko Mizuno, Tadashi Akimoto, Kazuhisa Azumi, Tadayoshi Ohmori, Yoshiaki Aoki, and Akito Takahashi, Hydrogen evolution by plasma electrolysis in aqueous solution, Jpn. J. Appl. Phys. 44(1 A), 396-401 (2005).

"EXCESS HEAT" I N D U C E D B Y D E U T E R I U M FLUX IN PALLADIUM FILM

BIN LIU, X I N G Z. LI, A N D Q I N G M. W E I Department

of Physics, Tsinghua University, Beijing E-mail: [email protected]

100084,

China

N. M U E L L E R , P. S C H O C H , A N D H. O E H R E Inficon

Limited,

Alte Landstrasse

Principality

of

6, LI-9496

Balzers

Liechtenstein

An early work at NASA, USA has repeated at INFICON Balzers, Liechtenstein in 2005. It is a confirmation of the correlation between excess heat and deuterium flux permeating through the Pd film. The maximum excess power density is of the order of 100 W / c m 3 ( P d ) .

1. Introduction Early in 1989, G. C. Fralick et al., of NASA, USA conducted an important experiment to search for the neutron radiation using gas-loading method in a D/Pd system instead of electrolysis.1 They could not find any evidences for the neutron radiation in a D/Pd system; however, they discovered unexpectedly the "excess heat" in a D/Pd system. Thanks to J. P. Biberian, we became aware of this NASA work after ICCF-11. This NASA experiment was very similar to our gas-loading experiments, which have been conducted at Tsinghua University since 1989. 2 ~ 4 The excess heat appeared in both our experiments and in NASA experiments whenever deuterium gas was pumped out from the Pd samples. In our early work,2 we used palladium wire only and heated Pd wire using the electrical current through it. G. C. Fralick et al. utilized the Pd-alloy tube in a hydrogen purifier, and heated this tube using an external electrical heater from outside of tube. Nevertheless, in W. Wu and X. Z. Li's work,3 we utilized Pd tube also, but we heated the Pd tube using electrical current through Pd tube. This is different from Fralick's heating from external heater. On the other hand, X. Z. Li and J. Tian 4 were using an external heater, but the pumping was done only at one side of the Pd tube. However, G. C. Fralick et al. pumped deuterium gas from both sides of the Pd-alloy tube. We now use a Pd disk heated by an external heater, and pump down from both sides of the Pd film (Fig. 1). Although the configuration varied in various experiments, the results are all similar, i.e., the "excess heat" appears while a deuterium flux leaving palladium is created. 75

76

Swagelok connection Thermocouple Heating coil

Figure 1. A thin palladium film is sealed between two tubes using a Swaglok connection structure. There are two small holes on the nut. Thermocouples are inserted into holes in order to measure the temperature of the edge of the Pd film. The heating coil winding is wrapped around the nut to hea.t the Pd film.

2. N A S A ' s Early Gas-loading Experiment In a hydrogen purifier (HP-25, commercial available through Johnson & Matthey Inc., Fig. 2), 13.8 atm. deuterium gas was fed into the palladium tube from both the inner side and outer side. It was heated electrically to 383°C. When the deuterium gas was pumped out using the mechanical pump, the temperature of the palladium tube increased suddenly from 383°C to 400°C in 15 s. It was not caused by the reduction of heat conductivity, because there was no such temperature variation when hydrogen gas was fed instead of deuterium gas. It was further confirmed by switching off the electrical power before starting the pump. In this case, the temperature dropped from 374°C to 370°C and then slowly increased back up to 375°C, again indicating the heating as the deuterium was removed from the palladium. As before, no neutrons were registered by either detector during the time the heating occurred.

Figure 2. Hydrogen purifier is utilized as a palladium tube-deuterium system with heating element wrapped in the insulator. The helical stainless tube on the top is for cooling the purified gas.

77

With the assistance of INFICON R&D Laboratory, this NASA experiment was repeated and the gas sample was analyzed using high-resolution quadruple mass spectrometer. This paper would report the result of excess heat first. The result of quadruple mass spectrometer analysis would be reported in another paper. 5 3. Tsinghua INFICON Collaboration Early in 1989, the hydrogen purifier was an existing equipment for NASA scientists to study the D/Pd system; however, it was not easily accessible for us in 2005. With the assistance from IERA, 6 we had experience in running Swagelok connection like that in Fig. 1. The advantage of this configuration was that it was easy to utilize the high-resolution quadruple mass spectrometer in the INFICON R&D Laboratory in order to identify the nuclear products from the D/Pd system. A Pd film with high purity (99.98%) was cut to be fit into the Swagelok connection. It was about 20 mm in diameter and 0.1 mm in thickness. The Pd film might be heated to 330°C using the electrical heater wrapped around the nut. The temperature of the Pd film might be monitored by the thermocouples inserted into the holes on the nut. The system was pumped to 10~ 6 mbar. Then the deuterium gas was filled into the system to 999 mbar. The electrical heater was turned on to heat the system from 25.3°C to 330.2°C in 1.5 h using '--113 W heating power while the room temperature is about 23.6-25.0°C. During the heating the deuterium pressure dropped first because of the strong absorption of the Pd film. The pressure was down to 996 mbar first; then, it increased slowly due to the heating. When we started pumping, the pressure was 1004 mbar. The Pd temperature started increasing when we started pumping as that seen in Fig. 3. When pressure was down to 0.1 mbar, the decreasing rate of pressure slowed down. An additional turbo-molecular pump was turned on at that time. The pressure was further down to 10~ 4 mbar. A very clear temperature rising was observed in this period. The temperature reached the highest point (339.8°C) after 70 min; then, it started decreasing even if the pumping continued to pump the pressure down to 10~ 5 mbar. This behavior was very important in order to exclude the effect of the heat conductivity. Usually, we might worry about that the heat conductivity might drop while the gas pressure dropped. Indeed, this last period just showed that the effect of heat conductivity in this temperature rising was not important. The electrical heating power was provided by a VARIAC power supply. It showed a stable voltage about 221.2 V(AC). We might worry about the room temperature fluctuation. It was monitored by a thermocouple and a mercury thermometer. The lowest was 23.1°C, and the highest was 25.0°C. 4. Discussion The absorption of deuterium gas into palladium is an exothermic process. Hence, the degassing of deuterium from the palladium is supposed to be an endothermic process. We were supposed to observe the temperature drop when we started pumping. This was true, when the data acquisition system was able to catch that

78

short temperature drop just after the starting point of pumping. It was caused by both the endothermic degassing and the adiabatic expansion. However, this short drop in temperature was always followed by a temperature rising which was corresponding to the correlation between heat and deuterium flux. This phenomenon was discovered in the study of gas-loading in palladium wire, 2 and was named as "pumping effect". The careful study using high precision calorimetry confirmed this phenomenon, and called it as correlation between heat flow and abnormal deuterium flux.3,4 The early NASA gas-loading experiment provided a strong evidence to this phenomenon unexpectedly.1 The collaboration with INFICON R&D laboratory has made us even more confident about this phenomenon. Deuterium flux and excess heat 340-

10,000

Start pump ingj' i

^

** / ,

\ \k ^

rf

/

1000 100 10

\t8 rong

pump ing

3

1

0.01

\ *

*•"

"

Stop pun. >ing ' * " •

?S0-

"a

Jr

—

1E-3 1E-4 1E-5

20:09 20:38 21:07 21:36 22:04 22:33 23:02 23:31 24:00 24:28 24:57

Time

Figure 3. Solid line shows the temperature at the edge of the Pd film. Dash-dotted line shows the pressure around the Pd film. The temperature started increasing when pumping was started. However, temperature dropped later even if the pumping was continuing.

We may estimate the excess power in this pumping period. The resistance of the heater was 433 fi at 330°C, it provides an effective heating power of 113 W at 221.2 V. This heating power was able to maintain a temperature difference of (330.2-24.0) = 306.2°C. Hence, the temperature difference of (339.8-330.2) = 9.6°C might imply an "excess power" of 3.5 W. The volume of the Pd film was about 0.031 cm 3 ; hence, the power density for the palladium was about 114 W/cm 3 . It is about the power density in a modern nuclear fission reactor. Acknowledgments This work is supported by the Natural Science Foundation of China (No. 10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds). References 1. G. C. Fralick et al., Technical Memorandum 102430 (1989). 2. X. Z. Li et at, The Proceedings of ICCF9, Beijing, China, May 19-24, 2002, Edited by Xing Z. Li, Tsinghua University Press (2003), p. 197.

79

3. W. Wu and X. Z. Li, Proceedings of ICGF9, Beijing, China, Mayl9-24, 2002, Edited by Xing Z. Li, Tsinghua University Press (2003), p. 412. 4. X. Z. Li et al, J. Phys. D: Appl. Phys. 38, 3095 (2003). 5. Q. M. Wei, Xing Z. Li, Bin Liu et al., High resolution mass spectrum for deuterium (hydrogen) gas permeating palladium film, The Proceedings of ICCF12, Nov. 27-Dec. 2, 2005,Yokohama, Japan, Edited by A. Takahashi, Y. Iwamura, and K. Ota, World Scientific (2006). 6. X. Z. Li, G. L. Schmidt, and J. Tian, The Proceedings of the 5th Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, March 19-21, 2004, Asti, Italy.

A B N O R M A L EXCESS HEAT OBSERVED D U R I N G M I Z U N O - T Y P E EXPERIMENTS

JEAN-FRANgOIS FAUVARQUE, P I E R R E PAUL CLAUZON AND G E R A R D JEAN-MICHEL LALLEVE Laboratoire

d'Electrochimie Industrielle, Conservatoire National rue Saint Martin, F-75141 Paris Cedex 03, E-mail: [email protected]

des Arts et Metiers, France

292,

A simple calorimeter has been designed that works at constant temperature; that of boiling water. Heat losses can be estimated accurately with an ohmic heater. As expected, losses are independent of the electric power input to the heater and the amount of evaporated water is linearly dependant on the power input. The device has been used to determine the heating power of a plasma electrolysis (the Ohmori— Mizuno experiment). We confirm that in this experiment, the heat output from electrolysis is greater than the electrical power input. The excess energy increases as the electrolysis voltage is increased from 200 up to 350 V (400 W input). The excess energy may be as high as 120 W.

1. Introduction Our experiment is an electrolysis experiment made in plasma mode with a tungsten cathode, a platinized titanium wire as an anode, and as electrolyte a water solution of potassium carbonate (K2CO3 at 0.2 M). In the same type of experiments, Mizuno 1 ' 2 reported both excess heat and excess hydrogen production. The explanations found in the bibliography for this phenomenon are, for example, transmutations in the cathode material. 3 The abnormal observations are concerned with the appearance of osmium, iridium platinum, and gold, without quantitative measurements. 3 We thought it would be quite interesting to confirm these results with the help of a simplified experimental setup. 2. Experimental We decided to do our experiments at a constant temperature, the boiling point of water, and to measure the heat emissions only by weighing the mass of water in the experimental device. A water storage container inside the device allows us to maintain the electrolyte at a constant water level, and thus keep the K2CO3 concentration constant. This container, being graduated, also gives us a way to confirm the mass of water boiled off. An interesting repercussion of this operating mode concerns the thermal losses. Once the boiling temperature is reached and overall thermal stability is achieved, 80

81

the thermal losses, which depend only on the temperature, remain constant, and this is true whatever thermal emissions are observed. This allowed us to hold the experiment in a simple beaker of an appropriate size and then to avoid the of an opaque Dewar vessel. This allows us to visually observe the cathode condition. Finally, the use of an ohmic heater allowed us to bring the device at the suitable boiling temperature and to maintain this temperature at this level much more quickly than by electrolysis alone. We also verified that other sources of inaccuracy were insignificant. For example, in the range of power used, the recondensation level inside the device was low, and few unboiled droplets of water sprayed outside the beaker. The excess heat that we were trying to measure is quite large (30-100%). So, it is not necessary to obtain very precise measurements. 3. Experimental Device Description Figure f shows the details of the experimental setup: • A SARTORIUS balance, the heart of the device, measuring up to 6 kg at an accuracy of 0.1 g. • Beaker containing between 1 and 1.51 of electrolyte. • Tripod (not shown in this figure) is placed on the balance to hold the electrodes and a container of pure water. • Continuous current electricity supply (500 V, 4 A). • Wattmeter to measure the input energy (Unigor 390 LEM).

Glass tube Distilled water reserve

Anode4

Ohmic heater Electrolyte reserve ((Sartorius)},^balance

1

i

ooo.o g

Figure 1. Experimental setup. Electrolyte reserve is 2 1. The tripod used to hold components in position is not shown.

82

Figure 2.

Photograph of the experimental apparatus.

The input energy was also frequently measured by use of the inlet voltage and the mean current intensity as given by a recorder. These results were compared the wattmeter data. ® A tungsten cathode of 2.4 mm diameter made with 2% of thorium (this type of electrode is often used for commercial scale welding). This cathode rod is shielded with a Pyrex tube. About 15 mm of the rod extends out from the tube, where it is exposed to electrolysis. In some experiments, ceramic tubes were used instead of Pyrex. ® An anode made up of a wire in platinized titanium in a cone or cylinder shape around the cathode to regulate the water current. This is made quite large, to cope with the boiling, and to stop unboiled droplets of electrolyte from leaving the beaker. The anode and cathode are 4 cm apart. ® An ohmic heater rated to about 400 W (enough to evaporate 34 g of water in 300 s). ® A distillated water container equipped with a tap, which allows us to maintain a stable water level inside the beaker during the experiment. ® Various measuring instruments for the electrical components. A typical run lasts 10-20 min, divided into 5 min measurement periods. The evaporated water quantity may reach 50-100 g, which corresponds to energy ranging from 113,000 to 226,000 J. In some cases, we used a Geiger-Muller device to check for possible nuclear radiation. The results of these nuclear observations were always negative (Fig. 2).

83

4. Results and Discussion 4.1.

Calibration

Using an ohmic heater, which can remain inside the beaker permanently, we have verified the response of our device to heat emission. It was necessary to verify that the thermal losses were constant beyond a certain input power level, and then that every increase in power would give a loss of water corresponding exactly to the energy supplied in the device during the measurement period. The electrolyte level is maintained constant, due to the supply of water (at 20°C) from the reserve. The energy used for the boiling of 1 g of water is then: 2260 J (latent heat at 100°C) + (100°C - 20°C) x 1 x 4.18 (heat needed to bring l g of water from 20 to 100°C) = 2594 J. Figure 3 shows the results. Note that from about 300 W inlet power, the experimental curve and the theoretical straight line are rigorously parallel, and the thermal loss is 75 W. Three important features can be deduced when we maintain the power of the ohmic heater at about 400 W. We were able to verify the validity of our measurement of the latent heat of water evaporation. The power increase due to the experiment is directly measured by the water loss during a given time unit. Losses due to the recondensation inside the experimental device, as well as those caused by unboiled droplets driven out of the beaker, seem to be negligible. 4.2.

Results

We made a parametrical study on the influence of the voltage applied during glow discharge electrolysis. The temperature was brought to the boiling point (100°C)

Vaporized water with re-feeding 700 600

«

400"

0- 300

30

40

m (g/300s) Figure 3.

Device calibration using ohmic heating only.

84

with the auxiliary resistance heater. Then electrolysis was begun at 200 V. This high voltage is needed to produce a suitable plasma around the cathode. Plasma generation is greatly enhanced by the high-electrolyte temperature. The Joule heating effect during electrolysis immediately gives rise to an envelope of steam around the cathode, and a plasma, that is supposed to be hydrogen plasma according to Mizuno. Table 1 gives the value of the COP, which is the ratio of the energy of vaporization divided by the electrical energy supplied to the device (which of course includes energy consumed by the ohmic heater). It is very important to confirm that the device is thermally stable. The selected definitive values for the inlet energies are the values of the wattmeter, considered to be more reliable than those based on voltage and mean registered current. Table 1.

4.3.

Five-minute test results

Voltage (V)

COP (energy out/energy in)

Number of tests

200 250 300 350

1.0 1.05-1.12 1.12-1.15 1.31-1.41

3 8 8 4

Remarks

(1) The calculation of the COP is straightforward. Let us take the 200-volt data. The mass of evaporated water is 63 g, with for 34 g due to auxiliary resistance heater. The mean current was 1.25 A, and the duration of the test is 300 s (5min). Energy out: 63 g - 34 g (auxiliary resistance) x 2594 J = 75,226 J. Energy in: 200 V x 1.25 A x 300 s = 75,000 J. The COP is then: 1.0. (2) The COP values bands are not correlated with the inaccuracy of the measurements. The results presented here were collected over several hours of operation of the cathode. The cathode is corroded at the very high temperatures of the experiment, so between experimental runs we push more of the cathode through the Pyrex shield, keeping the length of exposed cathode at about 15 mm. That explains the variation bands. (3) Reproducibility is within a range of about 5%. 4.4.

Discussion

The very simple device used allowed us to highlight with reproducibility an abnormal excess heat, which increases with voltage. We believe that we have confirmed abnormal excess energy for voltages higher than 200 V with our present device. The data presented here for 350 V correspond to input power exceeding 400 W. The abnormal excess heat exceeds 120 W without

85

taking into account the gas formation or luminous radiation. This power is therefore definitely significant. We did not find any classical explanation for this thermal effect, and we are examining the possibility of less classical explanations. 5. Conclusion The initial purpose of these experiments was to investigate the potential of a simple experimental device to confirm the results obtained by Mizuno. 1 ' 2 We think that this first step has been accomplished and that we can say that ratios between output and input energy (COP) of 1.3 and 1.4 have been reached with satisfactory reproducibility. In a second step, we will try to explain this phenomenon in order to increase the COP. In any case, the device presented in this paper is a very simple device, which can be used to rapidly verify hypotheses without sophisticated means. For example, we have verified that this phenomenon does not seem related with the heavy water, which is found at one part in 7000 in natural water. We increased the concentration of heavy water by a factor of 100 in our electrolyte, i.e. to 1 part in 70. We did not see any perceptible change in our results. Acknowledgments The authors want to express our deep appreciation to M. M. D. Noel, J-L. Naudin, and O. Horner of "EDF Les Renardieres" for fruitful discussions. References 1. D.Y. Chung, Y. Aoki, F. Senftle, and T. Mizuno, ICCF11 Conf. (Marseille, 2004). 2. T. Mizuno, T. Akimoto, and T. Ohmori, Fourth Meeting of Japan CF Research Society (Iwate University, Japan, 2003). 3. D. Cirillo, A. Dattilo, and V. Iorio, ICCF11 Conf. (Marseille, 2004).

SEEBECK E N V E L O P E CALORIMETRY W I T H A P d | D 2 0 + H 2 S 0 4 ELECTROLYTIC CELL

W U - S H O U ZHANG, 1 " J O H N D A S H , A N D Q I O N G S H U W A N G Low Energy

Nuclear

Laboratory, Portland State OR 97207-0751, USA E-mail: dashj@pdx. edu

University,

Portland,

Anomalous excess heat in P d | D 2 0 + H2SO4 electrolytic cells was confirmed using an accurate method of heat measurement, Seebeck Envelope Calorimetry. A cell was placed in the calorimeter, which measures the output heat flux directly and avoids many of the problems other methods have. The maximum excess power thus far was 1.3 W (or 11 W / c m 3 ) with input power of 13 W at a current density of 0.4 A / c m 2 . Calibrations were carried out before and after electrolysis experiments using a P t | H 2 0 + H2SO4 electrolytic cell, a dummy cell with inner resistor, or a pure resistor. Different calibrations gave consistent device constants within experimental error. Pd cathodes were analyzed by scanning electron microscopy and energy dispersive spectrometry. Unexpected elements were observed on the sample surface after electrolysis.

1. Introduction After the successful public demonstrations of excess heat in Pd|D20 + H2SO4 electrolytic cells at Boston (ICCF10) in 2003,1'2 we confirmed this anomalous effect using a more accurate calorimeter: a Seebeck Envelope Calorimeter (SEC). The SEC is a cube; the electrolysis cell is placed inside it. The SEC converts the heat flux through the six walls of the cube into a voltage signal using many thermocouples distributed uniformly in the walls. Many problems of isoperibolic calorimetry and mass flow calorimetry can be avoided by this method. 3,4 In this report we present the calorimetric results for the Pd|D20 + H2SO4 electrolytic cell, results with Ti added to the D 2 0 + H2SO4 electrolyte, and the results of analysis of the Pd cathodes. 2. Experimental Setup Closed cells are similar to that used before1'2 except that the height is less in order to fit into the SEC as shown in Fig. 1(a) and described below. The electrolytic cell is a Pyrex cylinder (capacity is about 280 ml, 4>-m = 50.7 mm and <^0ut = 57.0 mm, tAlso at: Institute of Chemistry, Chinese Academy of Sciences, P.O. Box 2709, Beijing 100080, China. 86

87

wall thickness = 3.2 mm, h = 142 mm). A PTFE female top cap is 0.8 mm, and also has two holes, 1 mm diameter each, for the electrode lead wires. A PTFE rod is fastened to the perforated plate and the top cap ensures that the perforated plate is at a fixed distance above the electrolyte. A gasket (<j)-m = 35 mm, <^out = 57 mm, wall thickness = 2.5 mm) made of ethylene propylene (resistant to sulfuric acid) is used to seal the top cap against the top edge of Pyrex cylinder.

PFTE cap PFTE rod Tape PFTE tube - PFTE plate with - many holes Pyrex cylinder -280 ml

—

Anode Cathode

(a)

Styrofoam box it: SEC (sat

j

DC power

(b) Figure 1.

(a) Schematic of electrolytic cell, (b) Schematic of calorimetric system.

The Pd cathode is cut from a 99.9% palladium foil with 0.5 x 10 x 10 mm 3 (Alfa Aesar, Stock No. 11514). It is then cold rolled to the desired thickness. The platinum anode is a foil 37.5 x 23.8 x 0.12 mm 3 . Pt leads are made of wire ( 1 mm x ~150 mm) covered with heat-shrink Teflon tube.

88

The electrolyte is heavy water (99.9 at.%, Aldrich catalog No. 347167) mixed with 96.4% H 2 S0 4 (J.T. Baker, lot No. K10030) by the volume ratio of 6.7:1. Two types of catalysts were used in these experiments, one contains 0.5% Pd on coconut charcoal (United Catalysis); another contains 0.5% Pt on 1/8 in. diameter alumina pellets (Alfa Aesar). Before each experiment, the catalyst was thoroughly dried in an oven at 88° C in order to drive out the liquid adsorbed during previous electrolysis. A schematic of the calorimetry system is shown in Fig. 1(b). The SEC (Thermonetics Corp.) has inner dimensions of 18.3 x 18.3 x 18 cm 3 (W x D x H). A fan (Panaflo®, Model FBA08A12H1A, 80 x 80 x 25.5 mm 3 , DC12 V, 173 mA, 2.08 W) is used to eliminate temperature gradients in the SEC. 3 The temperature of the SEC wall (TSEC wail) is controlled by a constant temperature bath (NESLAB, RTE-111); the temperature stability is ±0.1°C. The SEC is covered with Styrofoam to avoid the influences of room temperature fluctuations on calorimetry. A HP 6267B DC power supply (0-40 V, 0-10 A) is used for galvanostatic electrolysis. The electrolysis current is measured with a shunt resistor, which is a standard resistor of 0.1 fl with 0.04% precision (Leed & Northrup 4360). The electrolytic cell is placed in the center of the SEC. Eight K-type thermocouples are used to monitor temperatures: one is for ambient temperature outside the SEC; one is for air temperature in the SEC; two are attached on the outside of the cell wall at the middle height of electrolyte; four are attached on the wall at the middle height of catalyst. All the data are monitored by a Keithley 2000-20+scan digital multimeter. The data are automatically logged every minute using TestPoint 3.3 software. The mass of the cell was measured before and after electrolysis using a My Weigh i500 balance (max. 500 g, d = 0.1 g). After Jan 1, 2005 this was replaced with an Ohaus D54 balance (max. 2000 g, d = 0.01 g). The Pd sample is weighed with a Mettler H70 (max. 160 g, d = 0.1 mg). Calibration experiments are conducted using a Pt|H20 + H2S04 electrolysis cell, a pure resistor, or a dummy cell with a resistor in it. Calibrations are carried out before and after every electrolysis experiments. Surface topography and element analysis of the palladium cathode surface is performed using an ISI-SS40 scanning electron microscope (SEM) with an attached Oxford model 5565 energy dispersive spectrometer (EDS). 3. Results 3.1. Calorimetric

Results

First, we present calibration results. A resistor provided by the SEC manufacturer was placed at the center of the SEC. TSEC wail was the same as that used for the experimental P d | D 2 0 electrochemical cell calorimetry. After the calorimeter reached steady state with the fan turned on, the background signal was stable. Then, power was applied to the resistor. After the output signal reached steady state, the power was turned off. The output signal was monitored during the cool

89

down. The device constant is the quotient of average stable input power to the average net output signal at steady state. The net output signal is the gross output signal minus the signal produced by the power supplied to the fan. For input power of 11 W, the fan power decreases by 23 ± 3 mW (1.4%) during calibration or calorimetry. The decrease in fan power during calibration is the same magnitude as the decrease during calorimetry, so there should be no net effect on the calculated excess power. One calibration requires about 12 h. Figure 2(a) shows the results of one of the calibration experiments. It gave the device constant of 182.34 ± 0.20 W/V. The time constant is 15 min here. Due to the large inner volume (6 1), the time constant of the SEC is mostly determined by the heat capacity and conductivity of the sample under test, rather than the SEC itself. (a)

20 60

,"f~ "

_

i«

V0M (mV)

£

.

>

o

*

7"SEC wall = 30°C

if

-

i I

J 20 •

utpu t signal:

i?

-

-P(W) = (0.18761 + 0.0034) Vout (mV) 5 -(2.12 x 10~ ±3.9x io- e )(i/ o u

pin (W)

°

'

8

j

CD

? '5 - x a.

2

= 2 . e x-\0-*, Ff = 0.99999

TsECwal

f

-

(mV|f/

,

S

j /

= 20°C

5 10 o Q. 3 Q.

—

/

5

(b) 0

•

20

40

60

80

100

Net SEC signal output: l/oll, (mV)

Time (h)

Figure 2. (a) An example of calibration (Exp. No. 051005); (b) calibrations at different input power, where x 2 is the sum of squared residuals; R2 is the coefficient of determination (Exp. No. 041228).

Calibrations were performed at input power ranging from about 1 to 20 W. In this range, the device constant changes only slightly, as shown by the equations in Fig. 2(b). This means that the SEC behaves as an ideal calorimeter. The slight nonlinear term of the device constant with increasing power is caused by the nonlinear increase in electromotive force produced by the SEC thermocouples. However the device constant varies. For example, there were 11 calibration runs during December 2005. The device constant ranged from 180.6 to 181.8 W/V, a variation of less than 1%. The before-and-after calibrations for an experiment typically give device constants, which differ by less than 0.5%. The actual device constant used for calculating the excess power and energy is the average value of those obtained before and after the electrolysis with the same power input as that used in electrolysis. Besides the resistor, a P t | H 2 0 + H2SO4 electrolytic cell or a dummy cell with a resistor in it was also used to calibrate the SEC. Both of these cells have the same dimensions as that used for P d | D 2 0 + H2SO4 electrolysis; this arrangement could exclude the errors induced by the difference between temperature distributions of

90

(b) 80 70 O *2

60

13 01

50

Q.

7"sECWal|-35°C

E I2

12

16

40

Time (h)

Time (h)

Figure 3. An example of electrochemical calorimetry on the P d | D 2 0 + H2SO4 cell for sample Pd-A (Exp. No. 050110), (a) power signals and (b) temperatures. Parameters: total current is 3.65 A, average current density is 0.52 A / c m 2 , total input heat is 474.40 k j , excess heat is 19.46 k j , average input power is 11.980 W, average excess power is 0.492 ± 0.015 W (without including mass loss) to 0.753 ± 0.053 W (including mass loss of 0.7 g).

working cell and calibration resistor. The results showed that those three different calibrations gave the same device constant within experimental error. Seven Pd samples have been tested in experiments; four of them gave reproducible excess heat. The calorimetric results for the best sample, Pd-A, are presented here in detail. The sample Pd-A (9.0x37.2x0.35 mm 3 , total area of 7.08 cm 2 , weight 1.3418 g) was cold rolled from 0.5 to 0.35 mm thickness. One example of excess heat production and related parameters is shown in Fig. 3. Figure 3(a) shows that the power input decreases rapidly in the first two hours because the input power heats the cell, as shown in Fig. 3(b); therefore the elec-

y*=*i 0?

i *

y

_ Time (h) Time (h)

Figure 4. Other examples of excess heat produced in the P d | D 2 0 + H2SO4 cell for sample PdA. (a) The maximum excess power in Exp. No. 041125. Parameters: average current density is 0.42 A / c m 2 , total input heat is 592.24 k j , excess heat is 44.05 kJ, average input power is 13.143 W, average excess power is 0.978±0.032 W (without including mass loss) to 1.273±0.065 W (including mass loss of 0.9 g). (b) An example of heat bursts during excess power production in Exp. No. 041122.

91 Table 1. Excess heats at different temperatures for sample Pd-A, with ~ 0.02 g/ml Ti added to the electrolyte. Exp. No.

T S E C wall (°C)

Electrolysis time (h)

Average input power (W)

Average excess power including mass loss (W)

041126 041128 041125 041130 041120 041204

10 15 20 25 30 35

11.5 9 12.5 9 13.5 8.5

12.922 12.000 13.143 11.640 12.763 11.149

0.046 0.171 1.273 0.944 0.819 0.296

± ± ± ± ± ±

0.067 0.065 0.065 0.074 0.061 0.075

trolyte conductivity increases and over-voltages on the two electrodes decrease with time. These factors make the cell voltage decrease correspondingly. Another phenomenon is that the catalyst temperature (indirectly measured on the outer wall of the cell) has some fluctuation possibly because of the coarse grains of charcoal (about 2 x 3 x 6 mm 3 ) and the inhomogeneous properties of the solid/gas reaction. Fine particles of catalyst produced by pulverizing the large grains can improve the stability and uniformity of temperature. However, this method does not improve the catalysis and it makes the catalyst more difficult to handle. Part of the water produced by the recombination of oxygen and deuterium gases is adsorbed by the catalyst. The fraction of the water adsorbed depends on electrolysis current and time, and the temperature and activity of the catalyst. It is from 40 to 80% in our experiments. Heat bursts have been observed from sample Pd-A, in addition to the stable excess heat, in three different experiments. One example is shown in Fig. 4(b). The excess heat was measured at different SEC wall temperatures; one set of results is shown in Table 1 and Fig. 5. We have conducted calorimetry with TSEC wail

0.5

o.o 10

20

30

SEC wall temperature (°C)

Figure 5. Dependence of excess power on temperature of SEC wall for Sample Pd-A, the current is 3 A (the corresponding current density is 0.42 A / c m 2 ) ; the input power is 11-13 W.

92 Table 2.

Excess heat at different current densities for sample Pd-A.

Electrolysis current density (A/cm 2 )

Excess power including mass loss (W)

0.14 0.28 0.42 0.49

0.090 0.191 0.470 0.513

± ± ± ±

0.007 0.016 0.025 0.032

at 40°C, which causes the electrolyte temperatures to approach boiling. Therefore, the mass loss is great due to the evaporation increase at higher temperature, and the excess power calculation is not accurate. Therefore, the highest temperature listed here is 35°C. Beside the dependence of excess power on temperature, the excess power is proportional to the current density up to at least 0.5 A/cm 2 as illustrated in Table 2 and Fig. 6. Our setup now cannot identify the excess power at higher current more than 4 A because the catalyst cannot recombine all of the off gases produced by higher currents. These results also agree with the reported behavior of excess power found as early as 1989.5 From October 2004 to November 2005, we have conducted electrochemical calorimetry on Pd|D20 + H2SO4 systems for seven Pd samples; the results are summarized in Table 3. In the seven samples, sample Pd-A, Pd-E and Pd-F gave excess heat in 70% of the experiments with Ti in the electrolyte. Pd-F uses two almost identical cells with Pd cathodes connected in series. Sample Pd-B produced excess heat in the first experiment only. Samples Pd-C and Pd-D have never given any excess heat. The electrolyte used for samples Pd-A and Pd-B was electrolyte previously used for Ti|D20 + H2SO4 electrolysis. Therefore, some titanium was dissolved in the electrolyte. 7 To identify the effects of titanium additive on the excess heat, we dissolved titanium in electrolyte from experiments involving sample Pd-D. Its

0.0

0.1

0.2

0.3

0.4

0.5

Current density (A cm"2)

Figure 6.

Dependences of excess power on current density for sample Pd-A (Exp. No. 041115).

93 Table 3.

Summary of excess powers for different samples from Oct. 2004 to Nov. 2005.

Pd No.

Sizes (mm 3 )

Exp. No.

Pex,max(W)*

Rp** without Ti

Rp** with Ti

C T i(g/ml)

A B C D E Fl F2 Total

0.35 x 9 x 37 0.25 x 10 x 61 0.4 x 25 x 25 0.05 x 11 x 34 0.25 x 25 x 25 0.3 x 9 x 25 0.3 x 9 x 23

041012-050714 050120-050227 050316-050503 050720-050805 050811-051006

0.978 0.226 0.010 0.019 0.759

2/9

10/17 1/12

~ 0.02 ~0.02

0/1 4/4

~0.03 ~ 0.03

051006-051109

0.461 ± 0.020

9/11

~0.03

± ± ± ± ±

0.032 0.016 0.018 0.017 0.161

0/6 0/4 0/2

10%

53%

* Maximum average excess powers do not include the mass losses. ** Rp = Reproducibility.

effects on excess heat are also shown in Table 3. The concentration of titanium is expressed by the mass of titanium per unit volume of electrolyte. The data in Table 3 indicate that titanium in the electrolyte enhances excess heat production. 7 3.2. Scanning

Electron

Microscopy

Measurements

We analyzed Pd sample surfaces before and after electrolysis, and we found changes in the characteristic X-ray spectra. In particular Pd L/3/La ratio is higher on the Pd cathode after electrolysis. As noted previously this may be due to the occurrence of silver after electrolysis,2 because Ag La overlaps with Pd L/3. For comparison, first we present the blank results. Figure 7 shows the SEM and corresponding characteristic X-ray spectrum with an EDS for a Pd sample before electrolysis. We find the surface is very smooth and the Pd L/3/La ratio is 0.41, compared with 0.42, the ratio expected for pure Pd. Figure 8 shows the surface pictures of sample Pd-A after electrolysis for 429 h. The cathode bends toward the anode during electrolysis as observed previously.6 The photo and SEM picture both indicate that the Pd electrode is covered with

(a) 30,000— (b)

pd

PdLB — ^ - = 0.41 PdLa

J

No Ag detected

20,000-

U

10,000~

Pd

o

i

\

ji -

•

-

.

X - . j

f"

. . . . . . . .

.

Energy (keV)

Figure 7. (a) SEM image of a Pd sample before electrolysis, (b) X-ray spectrum on the total area of (a) measured by EDS.

94

iflsg

\*

(a)

.

"! •,

$

(b)

Figure 8. (a) Light microscope photo of sample Pd-A after electrolysis for 429 hours, (b) SEM picture of square region shown in bottom right corner of sample Pd-A in (a).

a deposit. The EDS results of Table 4 show that this deposit is mostly Pt, which dissolves from the anode. Figure 9 shows part of the characteristic X-ray spectrum from the dark spot S2 in Fig. 8(b). Spot S2 is from a hole in the surface. It should be the bare Pd surface. Bright spot S3 is at the edge of the hole, wiiere the Pt is deposited. It seems likely that the holey regions are places where palladium-deuterium electrode reactions occur after some time electrolysis. Figure 9 shows an increase in Pd L/3/LOJ. Using deconvolution software, it is found that S2 has 6.5 at.% Ag and S3 has no Ag. Other results in our group show that Pd Lfi/La may be 1 or greater on the Pd cathode after electrolysis in heavy water. This is convincing evidence of the presence of localized concentrations of Ag. 7 Besides sample Pd-A, we also measured silver on other Pd samples after electrolysis. Another example is shown in Fig. 10 and Table 5; this sample also produced excess heat. Because the results are qualitatively the same as those of sample Pd-A, we will not discuss them in detail. 4. Discussion and Conclusion Our SEC calorimetric results showed that excess heat is produced in a Pd|D20 +H2SO4 electrolytic cell, thus confirming the positive results obtained by isoperibolic calorimetry. The excess heat was qualitatively reproducible for some samples. Table 4. Element compositions at spots shown in Fig. 8(b). No.

Pd (at.%)

Ag (at.%)

P t (at.%)

Ag/Pd

34.2 54.8 56.3 35.5 52.0 38.2

0 3.6 0 4.5 0 0

65.8 41.7 43.7 60.0 48.0 61.8

0.000 0.065 0.000 0.126 0.000 0.000

95

S2

Pd

ft

30,000-™:

PdLB =0.47 PdLa

Z

A g = 6.5% Pd

20,000-:

1 Ag

Ag

10,000-^

r TAg

0

«

i

•

'

I

1

"I"

1

' 1

J1

1

'1

1

'»

Energy (keV) Figure 9.

X-ray spectrum at spot 2 shown in Fig. 8(b).

Ti additions to the electrolyte improved reproducibility of excess heat, possibly by depositing on the cathode and catalyzing reactions, which produce excess heat. Localized changes in the surface topography of the Pd cathodes correlate with changes in the characteristic X-ray peaks of Pd. As before, these are interpreted

Figure 10. (a) Light microscope photo of sample Pd-E after electrolysis for 93 hours, (b) SEM picture of square area shown around the top left corner of sample Pd-E in (a). Table 5.

Element compositions at spots shown in Fig. 10(b).

No.

Ti (at.%)

P d (at.%)

Ag (at.%)

P t (at.%)

Ag/Pd

1 2 3 4 5 6 7 8 9 10

0 0 0 0 0.3 0 0.9 0 0.4 0

52.3 77.9 80.1 73.5 71.0 79.8 29.9 61.6 86.7 67.9

4.8 3.2 5.3 3.4 2.1 5.7 1.1 3.8 3.5 2.5

43.0 19.0 14.7 23.2 26.6 14.5 68.2 34.6 9.5 29.5

0.092 0.041 0.066 0.046 0.030 0.072 0.035 0.061 0.040 0.037

96

in terms of localized concentrations of Ag, which is thought to be produced during electrolysis. Acknowledgments We t h a n k Dr. E d m u n d Storms for valuable advice on calorimetry. This work was supported by a grant from the New York Community Trust. Wu-Shou Zhang was partially supported by K.C. Wong Education Foundation, Hong Kong.

References 1. A. Ambadkar and J. Dash, Electrolysis of D2O with a palladium cathode compared with electrolysis of H2O with a platinum electrode: procedure and experimental details, see: http://www.newenergytimes.com/Library/2003DashJ-ColdFusionRecipe.pdf 2. J. Dash and A. Ambadkar, Proc. ICCF11, Marseille, France, Oct. 31-Nov. 5 (2004), p. 477. 3. E. Storms, Proc. ICCF10, Cambridge, MA, USA, Aug 24-29 (2003), p. 183. 4. B. Bush and J.J. Lagowski, Proc. ICCF7, Vancouver, Canada, Apr. 19-24 (1998), p. 38. 5. F. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal. Chem. 26, 301 (1989). 6. S. Miguet and J. Dash, J. New Energy 1, 23 (1996). 7. Q. Wang and J. Dash, Proc. ICCF12, Yokohama, Japan, Nov. 27-Dec. 2 (2005).

OBSERVATION A N D INVESTIGATION OF N U C L E A R F U S I O N A N D SELF-INDUCED ELECTRIC D I S C H A R G E S IN T U R B U L E N T LIQUIDS ALEXANDR I. KOLDAMASOV Scientific Center of System Research and Technology, Moscow, Russia HYUN IK YANG Hanyang University, Ansan, Korea DENIS B. McCONNELL (ed.) Fusion Research Corporation, Vancouver, Canada ALLA A. KORNILOVA Moscow State University, 119899, Moscow, Russia VLADIMIR I. VYSOTSKII Kiev National Shevchenko University, Vladimirskaya St. 64, 01033, Kiev, Ukraine E-mail: [email protected] ANDREY V. DESYATOV Federal State Unitary Enterprise

"Keldysh Research Center", Moscow, Russia

Stimulation and optimization of intense light emission using cavitation phenomena in different liquids are studied and discussed. The process of formation and mechanisms of excitation of directed laser-like beams in the volume of cavitating machine oil are studied. One of the analysed mechanisms of beam excitation is connected with stimulated nuclear reactions. The problem of stimulating nuclear fusion using cavitation phenomena in liquids is also discussed.

1. Introduction The aim of this report is to present some preliminary results of experimental and theoretical investigations of the processes and phenomena connected with optimal fusion reactions in turbulent liquid targets. It is well known that one of the most promising and ecologically safe types of fusion reactions is the p + B 1 1 —> 3He4 reaction with AE = 8.7 MeV energy release and without the creation of neutrons or formation of radioactive waste. For this reaction the optimal energy for interacting with moving protons is about -EpBiopt = 675 keV. In the usual uniform systems like cold or warm stationary plasma the probability of such a reaction is very low. This is the direct result of the high Coulomb potential barrier. 97

98

In our opinion one of the most promising methods for enhancing the probability of this reaction is connected with the use of turbulence and cavitation phenomena in the volume of a liquid (in this case, light water). We believe that the same enhancement should generally take place for any type of fusion reactions with positive energy release, during the cavitation of bubbles in an appropriate liquid. There are several theoretical models for such enhancement. One of them ("coherent non-stationary interference model") is connected with the process of barrier-free fusion in the volume of a non-stationary (e.g., selfcompressing) microcavity (e.g., Refs. 1-4). In this non-stationary model the barrierfree fusion is possible for any over-threshold reaction with positive energy release. Other ("direct") models are connected with both high-impulse pressure and high temperature during collisions of atoms of the cavity walls during bubble collapse. In fact such models are connected with the microaccelerating (microhot) method of fusion using surface forces. We believe that these "direct" models are not able to ensure the necessary requirements for effective fusion because of the relatively low temperature (no more than 5000-10,000K in multibubble systems) and the relatively low pressure in a cavitation region.5 It is also evident that tunneling quantum processes cannot provide a sufficient probability of nuclear transmutation.

2. E x p e r i m e n t a l S e t u p Schematic and general views of the installation for the production of controlled turbulence and formation of cavitation bubbles in the working chamber are presented in Fig. 1.

Figure 1.

Scheme and general view of the experimental setup.

99

The total volume of circulating liquid is 201. The working chamber is made from plexiglas tube with diameter of about 8 cm and length of about 15 cm. The chamber wall is about 3 cm thick. A special insert (hermetic plastic plug) with an orifice hole is situated inside the working chamber. The diameter of the orifice hole is about 1 mm. In the experiments, different kinds of orifice hole with special variable profile and variable cross-section have been used. In these experiments two different liquids were investigated; machine oil and distilled light water. 3. E x p e r i m e n t s a n d R e s u l t s of Investigation of C a v i t a t i o n in P u r e Machine Oil In the first case we have studied the optical and nuclear processes that take place during cavitation of machine oil. In this case different successive phenomena were observed as the pressure was increased. Several stages of the cavitation process were observed: Stage 1. At low pressures (less than 20-30 atmospheres) and low velocity of machine oil (see Fig. 2; flow is from left to right) the color of the moving liquid in the working chamber is tawny.

Figure 2,

The view of the working chamber at very low pressure of machine oil.

Stage 2. At a pressure of about 30 atmospheres the formation of cavitation bubbles in the volume behind the orifice hole begins. Behind the orifice hole turbulence is initiated, and large-scale oil density fluctuations are observed. Stage 3. At a pressure of about 40 atmospheres the average size of the fluctuations becomes small. In the space behind the orifice hole a translucent fog of small bubbles forms, giving it a milky appearance (see Fig. 3).

100

Figure '\.

T\\v \\r\v of the working chamber nt low prcsMiu- o;" iiia<-liine oil.

Stage 4. At a pressure of about 60 atmospheres, a rapid increase in transparency of the turbulent oil takes place. As a result the chamber with cavitations at the downstream of the orifice hole becomes completely transparent. The steps of this process at increasing pressures P are presented in Fig. 4. At the latter stage, a small blue plasma jet appears in the cavitation zone. It forms in the region of turbulence and cavitations, immediately behind the orifice hole of the insert. This stationary plasma jet is about 2 mm long and about 2 mm in diameter.

Figure 1. Increasing of the cavitation marhin^ oil transparency in the working chamber at pressure increasing: Pi < P% < P3.

101

Stage 5. With additionally increased pressure up to 70-80 atmospheres a directed bright light beam appears in the central part of working chamber (see Fig. 5).

Figure 5.

Generation of the directed bright light beam in the turbulent machine oil.

The color of the beam is blue-white and is very bright. The diameter is about 6 mm. The main question is: what is the nature and origin of the directed luminous beam? It was not a directed light beam from the internal part of the hole because the initial diameter of the directed beam is four times greater than the diameter of the output aperture of the insert (orifice hole). It also was not equilibrium thermal radiation (sonoluminescence) from the region of cavitation. Several arguments support these conclusions: Argument 1. The length (about 5-10 cm) and very narrow cylindrical form of the beam are sharply different from the dimensions and shape of the usual cavitation region (jet-like cone, sphere or short cylinder). This is supported by a simple calculation: The processes of formation and collapse of bubbles take place immediately downstream of the transition zone at the exit of the orifice hole. The size of this transition zone approximately equals the diameter of the orifice hole (D = 1-1.3mm). It is well known (e.g., Ref. 6) that the time for the collapse of cavitation bubbles with typical initial radius JR0 « 5/xm does not usually exceed r m a x « 20 ns. Approximately the same amount of time is needed for formation of bubbles in the volume of moving liquid behind the orifice hole. It is also well known from hydrodynamic principles that the longitudinal velocity of moving fluid (moving bubbles) at P < 100 atmospheres does not exceed ti m a x « 10 4 -10 5 cm/s. Hence the size of the cavitation region does not exceed L m a x « D + 2v m a x r m a x « 1-1.3 mm. This is very small compared to the length of the observed directed beam (5-10cm).

102

The angular properties of this directed light beam are similar to those of a laser beam. Argument 2. The rather bright observed luminescence and rather high derived temperature (about 105 K) are comparable only to the intensity and temperature spectrum from sonoluminescence of single bubbles, and are the direct result of the spherical symmetry of the bubble at collapse. In the case of multibubble cavitation, the sonoluminescence spectrum indicates that the temperature inside a bubble at collapse is relatively low (2000-5000 K), and the intensity of the sonoluminescence is also low ("cold sonoluminescence").7"9 Argument 3. The intensity of sonoluminescence decreases strongly with increasing temperature of the cavitating liquid (e.g., at increasing temperature from 1°C up to 40°C the intensity decreases by 100 times 8 ). But in our system the intensity of radiation does not depend on the temperature in the explored interval from 20 to 60°C. So, the observed phenomenon is not the usual kind of sonoluminescence. There are reasons to believe that the intense directed beam could arise from one of the following three possible mechanisms: (1) Cherenkov emission of fast electrons; (2) single-pass laser generation at UV-, VUV- or soft X-ray wavelengths; (3) stimulated nuclear reactions in the volume of the directional turbulent oil jet, accompanied by spontaneous optical radiation. We consider each of these mechanisms in more detail: (1) Using three different methods, we have studied the mechanism whereby Cherenkov radiation might be emitted by fast electrons when accelerated along the axis of the chamber to velocities v > c/n(u>) in the field of large separated charges. • We used a ground connection to neutralize the separated volume charges in the chamber. This did not influence the directed properties or intensity of the laser-like beam. • We measured the angular distribution of the directed beam and found that it differed from the distribution typical of Cherenkov radiation: sin 9 = c/n(ui)v. • We investigated the action of an external transverse magnetic field on the direction and angular properties of the directed beam. The result was negative—a transverse magnetic field with magnitude of 300-500 Oersted did not significantly influence the direction of the beam. In view of these results, the directed beam is not believed to be connected with Cherenkov radiation. (2) The possible mechanism of single-pass induced laser generation is connected with the ionization and recombination of oil molecules in the cavitation region (similar to the processes in a gas-dynamic laser).

103

The first step would be intense ionization of the moving atoms and molecules. Formation of a moving hot plasma would then take place in the region of cavitation immediately downstream of the orifice hole. During the second step the process of recombination of moving atoms and molecules and the formation of inverted states in the active medium would contribute to self-cooling of the moving plasma farther downstream. Such a two-stage process could be steady and thus could lead to single-pass generation of a steady laser beam. The central question is—what could be the pumping source for such a laser-like regime? It is well known from fundamental laser and plasma physics that for pumping of a plasma laser (which is based on ionization and recombination) the temperature T of the active medium must be such that k^T > 5cpi- Here ipi is the ionization potential of the lasing atoms in the oil ( (50-100) eV [i.e., T > (0.5-1) x 10 6 K]. Since the temperature in the centers of cavitation in a multibubble system is no more than (0.5-1)xl0 4 K (e.g., Ref. 5), a much more energetic pumping source is required for the lasing to arise from the cavitation process. We believe that one possible source of energetic plasma for the hypothetical laser mechanism may be fusion reactions in bubbles in the cavitation region or the turbulent jet zone. (3) Nuclear processes would also be needed for the generation of spontaneous optical radiation in the directional turbulent oil jet. In both cases 2 and 3 a source of nuclear energy would be necessary. There are many reactions that might occur in cavitating machine oil (e.g., carbon-nitrogen cycle). These reactions are being researched now and results will be reported in the future. During steady operation of the chamber we also observed another phenomenon— formation of self-induced electric discharges ('lightnings') near the plasma jet (along the exterior surface of the insert). The average length of the lightnings was several cm. Such discharges are connected with ionization in the region near the orifice hole and the accompanying accumulation of free charges on the exterior surface of the insert. The typical frequency of such lightnings is several Hertz. Examples are presented in Fig. 5. Stage 6. At increasing pressures of up to 90-95 atmospheres the process of rapidly increasing intensity of the blue-white directed beam takes place. The frequency of lightnings also increases. At this time, in the space upstream of the orifice hole, an additional short intense green jet appears (see Fig. 6). The green jets are not in the region of turbulence and cavitation. The color of the oil in the area upstream of the orifice hole remains tawny and the motion of the liquid appears laminar. To stimulate the formation of the green jet we used a ground connection to neutralize separated volume charges in the chamber. There are two possible mechanisms for formation of the green jet.

104

t: : 1"; II•:*• ; ' ; '• • l:!: l:^Hllllllllllli^ll^

F i g u r e (). T l n r o s t o p of 1 IK- p r e s s u r e - d e p e n d e n t process of b a c k g r e e n j e t f o r m a t i o n in t h e w o r k i n g c h a m b e r a t i n c r e a s i n g of t h e l i q u i d p r e s s u r e .

One mechanism is connected with possible action of a blue-white backdirected light beam to unexcited atoms of machine oil and corresponds to a usual luminescence. The other mechanism is connected with microdischarges from the acute edges of the charged dielectric insert in the volume of the neutral liquid. The process of formation of a high charge on the insert is the result of friction with the water transiting through it. This mechanism is more likely because it would take place only in the presence of an additional ground connection for the liquid in the working chamber. 4. Investigation of Cavitation in Distilled Water In the case of distilled water the properties of the cavitation region fundamentally differ from the case of machine oil. As before, there are several stages of the cavitation process. In this case the intense laser-like directed beam was absent at any regime and any investigated pressure. The brightness of sonoluminescence in pure water at any

105

Figure 7

I-'di'iiiiition a n d collap.^e of vu\ ilat inn bul>!>i<^ in d i M ' l K d wal( y

pressure was likewise low. The formation of cavitation bubbles and their collapse at pressures near 30-40 atmospheres are shown in Fig. 7. At pressures above 50-60 atmospheres, weak sonoluminescence of cavitating bubbles takes place (see Fig. 8). The color of the low-intensity sonoluminescence is blue, and is located on the lefthand side of the photograph. The size of sonoluminescence area is about 1-2 mm. The luminescence in the central and right-hand side parts of the photograph is the result of the scattering of light in pure turbulent water. The intensity of radiation weakly depends on the pressure in the interval 60-90 atmospheres and decreases with the increase of the water temperature. According to all the tests that were discussed above it is the usual multibubble sonoluminescence. The spectrum of hydrogen from this sonoluminescence area was investigated. Spectra of the two most intense lines are shown in Fig. 9. By analyzing the relative intensities of the two lines with wavelengths A = 656.28 and 486.13nm (550-600 and 15-20 AU, respectively), the temperature of the luminescing centers was calculated to be T « 3000 K. This is a temperature typical of multibubble sonoluminescence. 5. Additional Studies Additional physical and nuclear tests on cavitating machine oil and distilled water have also been carried out.

Figure 8.

Sonoluminescence in distilled water.

106

1

1

630

640

Amplitude

m«iift»»wnii<M'* >.„nm 489.5

482.8

476.1

X

3

650

660

670

im

680

Figure 9. Spectra of two measured lines of hydrogen radiation of the sonoluminescence area. T h e possibility of the realization of one of the most optimal fusion reactions: p + B —» 3He for these liquids was investigated. T h e process of He 4 creation was investigated by the analysis of the optical spectrum of luminescence of the stationary plasma jet and identification of He spectral lines in real time. One of the main problems of identifying such reactions is connected with the search for an optimal method of controlled B 1 1 isotope insertion in the cavitation zone. Experiments have shown t h a t uncontrolled insertion of ions of B 1 1 isotope as an admixture leads to suppression of the sonoluminescence. T h e possibility of the realization of reactions of the carbon-nitrogen cycle in moving turbulent machine oil was also investigated. These processes were studied using various nuclear and spectral methods, including correlation analysis of the radiations from the luminescence region. In several cases the generation of directed intense hard X-ray (or gamma-ray) beams was detected outside the working chamber with cavitating machine oil or distillated water. This hard irradiation was detected using X-ray photographic plates t h a t were isolated in black paper and fixed on the external surface of the plexiglas working chamber. Initial calorimetric tests have shown t h a t the final (output) thermal energy of hot circulating machine oil in some cases exceeds the input electrical energy used for liquid pumping. These results, including studies of nuclear t r a n s m u t a t i o n and energy release, will be reported in the near future following additional research. References 1. V. I. Vysotskii, On possibility of non-barrier dd-fusion in volume of boiling D2O. Proceedings ICCF4, 1994, 4, pp. 6-1-6-3. 2. V. I. Vysotskii, Conditions and mechanism of non-barrier double-particle fusion in potential pits. Proceedings ICCF4, 1994, 4, pp. 20-2-20.5. 3. V. I. Vysotskii and R. N. Kuzmin, Nonequilibrium fermi - condensate of deuterium atoms in microcavity of crystals and the problem of nonbarrier cold nuclear fusion realization, Soviet Phys. - J.T.P. 64(7), 56 (1994).

107 4. V. I. Vysotskii and A. A. Kornilova, Nuclear Fusion and Transmutation Biological Systems. Moscow, "MIR" Publishing House, 2003. 5. D. J. Plannigan and K. S. Suslick, Nature 434, 52 (2005). 6. B. P. Barber et al, Phys. Report 281, 65 (1997). 7. W. B. NcNamara et al, Nature 401, 772 (1999). 8. K.Yasui, Phys. Rev. Lett. 83, 4297 (1999). 9. O.Baghdassarian et al, Phys. Rev. Lett. 86, 4934 (2001).

of Isotopes in

D E S C R I P T I O N OF A SENSITIVE SEEBECK CALORIMETER U S E D FOR COLD F U S I O N STUDIES

EDMUND STORMS Lattice Energy, LLC, Santa Fe, NM, USA E-mail: storms2@ix. netcom.com A sensitive and stable Seebeck calorimeter is described and used to determine the heat of formation of PdD. This determination can be used to show that such calorimeters are sufficiently accurate to measure the LENR effect and give support to the claims.

1. Introduction Heat production is an essential feature of the cold fusion effect and its measurement has been a frequent object of criticism.1 Since 1989 when Profs. Fleischmann and Pons (F-P) 2 first revealed their observations, calorimetry has evolved from the simple isoperibolic design and become increasingly accurate 3 with use of the Seebeck type. 4 " 7 The Seebeck (Kelvin) calorimeter consists of thermal-electric converters that completely surround the source of heat. Temperature at the outside of these converters is held constant while temperature at the inside is allowed to increase. The average temperature difference generates a voltage that is used, after calibration, to determine the rate at which heat passes through the thermal barrier created by the converters. Because the design is very simple, operation is easy to understand and potential errors are easy to determine. When used in a study of cold fusion, a gas-tight glass cell containing an electrolyte and electrodes is placed in the enclosure. Because the measured voltage represents an average of heat loss through all parts of the barrier, the device is only slightly sensitive to where the cell is placed within the enclosure. A fan is used to distribute heat more evenly and to reduce the cell temperature by removing heat from it more rapidly. The calorimeter is completely insensitive to where heat is being generated within the cell. A calorimeter suitable for measuring the cold fusion effect must be sufficiently sensitive to detect a few tens of milliwatts superimposed on tens of watts. In addition, it must remain stable over long periods of time. The method of calibration must define the same characteristics as when heat is produced by an unknown source. Power production can be calibrated by generating heat using a resistor contained in the device. A dead cell or conditions expected to produce no anomalous energy can also be used. If the calorimeter is sufficiently sensitive, the total amount of energy given off by a known chemical reaction can also be measured. In this 108

109

work, power is calibrated using a resistor in the cell or by using a Pt cathode and a quadratic equation, watt = A + B x V + C x V 2 , shows the relationship between generated voltage (V) and applied watts (W). In addition, the calorimeter is used to measure the total amount of energy absorbed when a Pd cathode is loaded with D. Because this quantity is well known, 8,9 the method gives further demonstration that the calorimeter is indeed accurate and able to detect small amounts of energy. Defining the accuracy of a calorimeter using a few numbers is not practical because several different and independent potential errors exist. Because of bubble action at high current, the amount of power being applied to a F^P cell is noisy. In addition, use of a fan adds additional noise, especially at low applied current as is the case during this study. This causes random fluctuations in measured power, which are as much as ±10 mW during this study. If this fluctuation is too great, it can mask small changes in anomalous power, but it does not introduce an error that might be interpreted as anomalous power. On the other hand, the calibration constant or the sensitivity of the calorimeter can change with time. These changes can be produced by changes in reference temperature, in room temperature, in the amount of recombination taking place in the cell, or in physical parameters when new samples are placed in the cell. This potential drift is the main source of incorrect results. These potential errors are explored in this work. 2. Description The device described here is made by gluing together commercially available thermoelectric converters, as shown in Fig. 1, using waterproof epoxy glue. The panels are connected electrically in series. Once assembled, the outer surface is covered with an electrically insulating, waterproof epoxy paint. The electrical resistance of this coating must be tested and found to be high (>1 Mohm) before final assembly. If the resistance is too low, unwanted voltages will be generated by chemical reaction between the cooling water and the metal plates. These assemblies

Figure 1. Glued panels assembled into two haves of a calorimeter. The length is 13.9 cm, the width is 6.9 cm and the total depth when assembled is 14.8 cm.

110

Figure 2. Assembled calorimeter with \vat In lliis design, the wires pass out of the cell through plastic water cooled channels.

are placed within watertight plastic boxes that are designed to cause even water flow over the outside surface. When assembled, the two boxes are stacked one on top the other as shown in Fig. 2. Figure 3 shows a typical open calorimeter containing an electrolytic cell and a small fan. Baffles are provided to insure air is passed over and around the cell. Wires and plastic tubes are passed into the cell through channels that are in good thermal contact with the cooling water. In one design, these channels, visible in Fig. 3, are stainless steel tubes, which pass the length of the device within the

Figure 3. Completed calorimeter with calorimeter through metal tubing so as The cell is attached to the calorimeter at lower left is used to measure current

cell and fan in place. Notice that the wires pass into the to isolate the interior from changes in room temperature. using plugs to allow easy removal. The stack of resistors through the cell and fan.

Ill

cooling water. These wires carry current to the cell and fan and allow applied voltage to be measured at the calorimeter boundary. Circuits are arranged so that current and voltage used for calibration and for electrolysis are measured using the same resistor and DA channels. In this way, any measurement errors caused by errors in the DA channels are cancelled. Measurements are made using National Instruments data acquisition boards and Labview. Switching from electrolysis to calibration can be accomplished by throwing one hardware and one software switch, which allows automatic calibration over the entire power range. A typical result is shown in Fig. 4. Table 1 lists calibration equations obtained over 5 months of examination. Experience and analysis of this information indicate that the uncertainty immediately after calibration is about ±16 mW, while drift caused by changes in room temperature and other factors can introduce an additional uncertainty of ±25 mW during long runs. If the average coefficients are assumed to be constant during the time shown in the table, the maximum uncertainty at 8.3 W of total power would be ±60 mW. In other words, the calorimeter is stable to within ±60 mW or 0.7% over 5 months if no effort is made to recalibrate. Because calibration is so easy, these small drifts can be easily identified as error. At no time has anomalous power outside of this uncertainty suddenly appeared without being related to something done on purpose to the surface of the cathode. Notice also, that calibration values based on Joule heating of a resistor located in the cell agree very well with values obtained by using a platinum cathode. This shows that the location of heat production within the cell has no effect on measured values. Because the cell contains a recombiner, no gas (except orphaned oxygen) is expected to leave the cell. To determine if the recombiner is working and to measure

20 -i

-7 W = 0.16942 + 83.650*V-2.8193"V A 2

18-

/

16-

/

14-

I

12-

8.

10

f

j

/

-

/

8-

/

9-

y 6

"

4

"

/

o Joule heat

/

* Electrolysis

j *

2-

y /

0.00

PI (8-23-05) 0.05

0.10

0.15

0.20

0.25

0.30

Seebeck voltage

Figure 4. Typical calibration using an internal resistor. Four points are taken going u p in power and four are taken going down, in sequence. The random error is the standard deviation of points from the drawn line. Data are taken after a delay of 90 min to allow the calorimeter to reach steady state.

112 Table 1. Date

Coefficients in calibration equation A

2/14/05 2/17/05 2/21/05 2/26/05 3/10/05 3/15/05 3/21/05 3/24/05 3/29/05 4/29/05 5/7/05 5/19/05 5/22/05 5/26/05 5/29/05 6/1/05 7/2/05 Average=

-0.020 0.006 0.001 0.001 -0.051 -0.022 0.002 -0.027 0.000 -0.013 -0.052 -0.076 -0.116 -0.093 -0.065 -0.078 -0.203 -0.047

B 83.02 82.85 83.04 83.35 83.18 83.86 83.30 83.76 83.40 83.82 83.40 83.25 83.33 82.94 83.04 83.46 83.49 83.323

Error (mW)

C 0.12833 2.012 0.366 -1.220 0.325 -1.927 -0.764 -1.737 -1.556 -1.998 -1.516 -1.258 -0.841 1.053 0.587 -2.371 -1.940 -0.745

7 17 17 11 24 10 16 28 19 16 24 10 5 17 16 13 15 16

the D/Pd ratio using the orphaned oxygen method, a small plastic tube carries gas from the cell to a reservoir of oil. Any change in gas pressure within the cell is detected as a weight change of oil applied to a balance (±0.01 g), as is visible in Fig. 5. This method allows the amount of orphaned oxygen resulting from D entering the Pd cathode to be determined and, from this, the D/Pd ratio. The method is calibrated by weighing the sample (±0.00005 g) at the end of the study to determine the amount of contained deuterium. Because D2 is lost from the

Figure 5. View of calorimeter and oil reservoir for measuring D / P d ratio. The switch in the foreground allows change from electrolysis to calibration. Water is circulated using a pumped (1.5 l/min) constant temperature bath (±0.01° C).

113

1.0774-

1.07723 TL F

1.0770 -

Weigh

s o 1.0768 -

1.0766 -

Weight = 1.0773 - 3.3180e -4x 1.0764- — i — i — i — i — i — | — ^—I—'—II — ' — 1 — > ~ 0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.(

2.0

2.2 2.4

Square root time

Figure 6. Determination of deuterium content of sample. Notice that the sample can be removed from the calorimeter and weighed within 2 min after turning off the current. The sample is dried quickly by washing with acetone.

sample once electrolysis stops, weight is measured as a function of time starting when current is stopped. The weight is plotted as a function of square root of time through which a least squares straight line is drawn, as shown in Fig. 6, which is extrapolated to zero time. A constant of 7600 g oil/mol contained D is typical when the measured contained deuterium is combined with the measured displaced oil. When current is applied to a Pd cathode, the surrounding D2O is decomposed into D2 at the cathode and O2 at the anode, with D2 and Pd reacting to produce /?-PdD x . This reaction is endothermic, as can be seen in Fig. 7, because more energy is used to decompose D2O than is produced when forming PdD. The greater the applied current, the more power is absorbed for a shorter time. This reaction * •

"i

•J^vfcV*

0.00-

* ... ° * V „A!'".-•'•-...

" •

0.05-

-'-V

,,

f . ' <.

• Heater

I "^'£t'-" -0.10-

- 0.152 A

F' A

'• 0.069 A

I

' 0.041 A

1/ -0.15100

200

300

400

500

600

Time (min)

Figure 7.

Power measurements during loading at various applied currents.

114

uses energy, measured as power, that can be calculated from the reaction {x/2)D20

+ Pd = PdD x + (ar/4)0 2)

where x is equal to the average D/Pd ratio. As the cathode takes up deuterium, the Pd converts to a-PdD followed by a layer of /3-PdD of increasing thickness with a range of composition. Eventually, after most of the sample is converted to the final composition, reaction stops and conditions return to zero power (energy). At this time, the composition is in steady state with a stable gradient and a constant rate of diffusion During loading, deuterium is added to the cathode to produce the composition change shown in Fig. 8. Note that initially, all D2 produced by electrolysis is combined with Pd. As the deuterium content increases, a smaller fraction of available D2 is absorbed, with a sudden termination as a limit is reached. The remaining D2 and O2 are recombined by the contained catalyst and remain in the cell. If applied current is sufficiently small, the initial conversion to /3-PdD becomes visible, as noted in Fig. 8.

Figure 8. Composition of a cathode during loading. Note that at low current, loading of the alpha phase becomes visible. The lines show the loading rate if all D2 produced by the current entered the Pd cathode. The horizontal line shows the published composition at the /3-PdD phase boundary at 1 atm D2 and room temperature in the presence of a-PdD.

3. Calculation of Enthalpy of Formation The energy used during the loading reaction can be calculated by integrating data, such as shown in Fig. 7, between zero power and the curve drawn through the data points over the duration of the loading process. However, the shape of the curve is difficult to define unless slow loading rates are used. For this reason, the analysis will only be applied to a current of 0.041 A as shown in Fig. 9. This curve gives a value of -106 kJ/mol Pd. Termination of the reaction is assumed to occur at an average D/Pd of 0.8, the measured value for this sample, and at 460 min. The

115

reaction equation becomes: 0.4D2O + Pd = PdD 0 . 8 + 0.2O2, where Ai7f(D20) = 294.6 kJ/mol. Because Pd and 0 2 are assumed to be at standard-state, their enthalpy values are zero. The enthalpy of formation of PdDo.g is Afff(PdD 0 . 8 ) = -106 + 0.4 x 294.6 = 11.8kJ/mol. This value can be calculated from the published equation: 9 Aff f (PdDx) = 44.99 - 41.89a; = 11.5kJ/mol for x = 0.8. Because of scatter in the power measurements and because the sample does not have a uniform composition, the potential error in this measurement is about ±2 kJ/mol. Agreement with the previous measurement is well within the possible error of both results, thereby demonstrating the potential accuracy of this calorimeter.

200

300

400

500

600

Time (min)

Figure 9. Data used to calculate enthalpy of formation of PdDo.go using 0.00974 mol of Pd. The first three points were taken while the calorimeter was approaching steady state and must be ignored.

4. Summary A Seebeck calorimeter can easily be constructed with characteristics that eliminate most errors thought to cause anomalous energy from cold fusion. In addition to being stable and accurate, the calorimeter is sufficiently sensitive to accurately measure the enthalpy of formation of PdD x to give 11.8 kJ/mol using only 1 g of palladium. References 1. J.R. Huizenga, Cold Fusion: The Scientific University Press, New York, 1993), p . 319.

Fiasco

of the Century,

2nd edn. (Oxford

116 2. M. Fleischmann, S. Pons, and M. Hawkins, Electrochemically induced nuclear fusion of deuterium. J. Electroanal. Chem. 261, 301 (1989) and errata in Vol. 263. 3. E. Storms, Calorimetry 101 for Cold Fusion (2004), www.LENR-CANR.org. 4. B.F. Bush and J.J. Lagowski, Methods of generating excess heat with the Pons and Fleischmann effect: rigorous and cost effective calorimetry, nuclear products analysis of the cathode and helium analysis, The Seventh International Conference on Cold Fusion. 1998. Vancouver, Canada: ENECO Inc., Salt Lake City, UT. 5. J. Warner, J. Dash, and S. Frantz, Electrolysis of D 2 0 with titanium cathodes: Enhancement of excess heat and further evidence of possible transmutation, The 9th International Conference on Cold Fusion, Condensed Matter Nuclear Science (2002). Tsinghua Univ., Beijing, China, Tsinghua Univ. Press. 6. W.-S. Zhang, Z.-F. Zhang, and Z.-L. Zhang, Primary calorimetric results on closed P d / D 2 0 electrolysis systems by calvet calorimetry, The 9th International Conference on Cold Fusion, Condensed Matter Nuclear Science. 2002. Tsinghua Univ., Beijing, China, Tsinghua Univ. Press. 7. E. Storms, Use of a very sensitive Seebeck calorimeter to study the Pons-Fleischmann and letts effects, 10th International Conference on Cold Fusion (2003), Cambridge, MA: LENR-CANR.org. 8. Y. Sakamoto et at, Calorimetric enthalpies for palladium-hydrogen (deuterium) systems at H(D) contents up to about [H]([D])/[Pd] = 0.86, J. Phys.: Condens. Mater. 8, 3229 (1996). 9. Y. Sakamoto et at, Calorimetric enthalpies in the b-phase regions of Pd black-H(D) systems, 6th International Conference on Cold Fusion, Progress in New Hydrogen Energy (1996), Lake Toya, Hokkaido, Japan, New Energy and Industrial Technology Development Organization, Tokyo Institute of Technology, Tokyo, Japan.

SOME R E C E N T RESULTS AT E N E A

M. A P I C E L L A , E. C A S T A G N A , L. C A P O B I A N C O , L. D ' A U L E R I O , G. M A Z Z I T E L L I , F . S A R T O , A. R O S A D A , E. S A N T O R O , A N D V. V I O L A N T E ENEA

Frascati Research Center V.le E. Fermi, E-mail: violanteQfrascati.

45 00044 Frascati enea.it

(RM),

Italy

M. M C K U B R E A N D F . T A N Z E L L A SRI International,

333 Ravenswood

Ave.,

Menlo Park,

CA 94025,

USA

C. SIBILIA La Sapienza

University,

Via Scarpa,

14 00100 (Roma),

Italy

Recent research activity at ENEA, in the field of Condensed Matter Nuclear Science, has been oriented to material science and Laser triggering in order to increase the reproducibility of excess of power production during loading of palladium with deuterium. Isoperibolic calorimetry in gas phase, isoperibolic and flow calorimetry with electrochemical systems have been carried out. Nuclear ashes detection was done by means of high resolution and high sensitivity mass spectrometer. Material science studies allowed to obtain a palladium showing high solubility for hydrogen isotopes and giving deuterium concentration at equilibrium larger than 0.95 (as D / P d atomic fraction) with a reproducibility larger than 90%. Excess of power production by using the above-mentioned material achieves a reproducibility up to 30% without triggering. Laser irradiation with a proper polarization seems to have a significant role in further increasing of the excess of power production reproducibility. Heat bursts exhibit an integrated energy at least 10 times greater than the sum of all possible chemical reactions within a closed cell. The energy gain calculated at the end of the experiments is observed with deuterium but not with hydrogen. Preliminary measurements give a 4 He signal in reasonable agreement with the expected values by assuming a D + D = 4 He + heat (24 MeV for event) reaction.

1. Introduction The dissolution of hydrogen isotopes into a metal lattice is not only a problem of thermodynamic equilibrium between the hydrogen inside the lattice and the hydrogen in the external phase (gas or liquid) but is also a problem of not equilibrium because of the occurrence of a transport process. Both aspects of the phenomenon are correlated since the equilibrium concentration of the solute is achieved when the chemical potentials of the hydrogen in both phases are equal and since the transport process inside the metal lattice is driven by the gradient of the chemical potential. The migration of interstitials in a metal under an applied external bending is well known as Gorsky effect.1 The deformation field produces the defects migration 117

118

toward the expanded areas. Lewis and co-workers 2-4 showed that internal stresses are generated during insertion and diffusion of interstitial hydrogen and that the resulting strain production represents an opposing force to the flux produced by the concentration gradient. The effect of the stress as limiting factor in achieving the deuterium-loading threshold in palladium to have excess of power production is studied.

2. Stress Field Limiting Hydrogen (Deuterium) Solubility in Palladium The chemical potential of the hydrogen in solid solution in a metal lattice is strongly influenced by all field force, like the stress field, modifying the free energy of the system. The hydrogen isotopes dissolving into a metal (i.e. palladium) occupies interstitial positions and expands the lattice. This process generates a stress field when remarkable concentration differences (strong gradients or coexistence of different phases) are created. The situation is quite similar to the stress produced by a temperature gradient as shown in Fig. 1.

Figure 1.

The effect of the hydrogen concentration profile on the stress field.

Therefore, the loading process may be inhibited by a stress gradient, for instance behind the external surface, where the effect is traceable to the effect of a strong temperature gradient. Thus, in the zone at high concentration, compressed by the zone at low concentration, the chemical potential of the solute increases and the loading can be inhibited. In the following such a problem will be approached in order to have an analytical tool to estimate the effect of the stress field on the loading and to identify the metallurgical conditions that can reduce this effect allowing the increasing of the amount of hydrogen dissolved in the metal. Chemical potential of hydrogen

119

dissolving into a metal lattice, in presence of a stress field, becomes 5 Ms = Ms ~ "V (°xx

+ °TO + <*zz) = Ms - % trCT = /X* - t4(Jh,

(1)

where fi* is the hydrogen chemical potential into the lattice without stress, Fis the partial molar volume of the solute and <7h the trace of the stress tensor. 3. Flux Equation with a Stress Field A diffusive flux of hydrogen within a homogeneous and solid media is created by a gradient of chemical potential and by the field of the applied forces so that the expression for the flux is

where M is the mobility, c the solute concentration, and F is the vector given by the sum of the applied forces acting on the hydrogen interstitially dissolved in the solid. By replacing the relationship between diffusion coefficient and chemical potential, D = Mc(dn/dc), into Eq. (2) it follows:

J-

=~DVc+^m„,_,

(3)

DFc

A little of algebra leads to J=-DVc

+ D~c.

(4)

For a stress field the flux equation becomes: J =-D

(VC - — V ^ ,

(5)

where <x is the local stress. The analysis allows us to study the mass transfer problem when the stress field is created during the loading. In the following, we will consider a system where the diffusion is well described by one-dimensional time-dependent model (foil, membrane or wire). 6 By introducing the fraction of relaxed stress ry into the flux equation it follows:

^-K-i-'1-'^!)A mass balance on a foil leads to: dc _, d (dc

V

da\

m=DI-x\d-x-{l~7l)RrcTx)-

(6) . . (7)

Let us to consider the well-known stress (a) strain (e) relationship: a = Ee,

(8)

120

where E is the Young's module. The relationship between strain and concentration for Pd /3-phase (assuming that it may be extrapolated up to a loading atomic fraction close to one) e(c) = [l + b(c-c/3min)},

(9)

where cp m ; n is the hydrogen concentration value for the a + (3 phases coexistence limit, b = 0.044 and c = C/CQ the dimensionless concentration (co is the metal atoms concentration). Let us introduce the following dimensionless parameters x = x/L,

T = L2/D,

(10)

where L is the characteristic length of the system (typically the thickness or the radius), so that the resulting dimensionless transport equation is

where we introduced r\ as a parameter giving the percentage of stress that is released by plastic deformation or by dislocation slipping; it is clear that when the release of the stress is complete the transport equation reduces to the Fick's one. Equilibrium concentration profile

0.8 Pd Young module 1010 Pa 0.6

I

0.4 0.2 0.0

+.

0

•(

|.

1

(

+ — )

_(_

0.25

1

1

0.5

Space coordinate (arb. units) Figure 2.

Equilibrium H concentration profile within a Pd foil with Young's module = 10 1 0 Pa.

Equation (11) describes the interstitial diffusion of hydrogen into a metal (e.g. palladium) under a stress field. The effect of stress at steady state translates on a different concentration profile, then a different loading that depends on the properties of the material such as the Young's module. The transport equation (11) is solved with the boundary conditions c = 1, x = 0 and dc/dx = 0, x = L/2 and including the calculation of the relaxed stress on the basis of the mechanical properties of the material (ay). Some calculations have been done by using indicative values of the Young's module in order to make more

121 Equilibrium concentration profile

o

0.25

0.5

Space coordinate (arb. units)

Figure 3.

Equilibrium H concentration profile within a Pd foil with Young's module = 1 0 n Pa.

clearer the effect. Figures 2 and 3 show the equilibrium concentration profile, from the external side up to the symmetry plane, for two palladium foils with different Young's module. In the first case the value of the Young's module is 1.0 x 10 10 Pa while in the second case the value is 1.0 x 10 11 Pa (these value are chosen in order to magnify the effect). It is clear that the loading reduces when the Young's module increases. The calculation of the concentration profiles evolutions has been used to calculate also the evolution of the R/RQ ratio by assuming the foil as a parallel of electric resistances and by considering the well-known Baranowsky curves. Figures 4 and 5 show the evolution of the R/Ro ratio for the two considered above-described loading conditions. Figures 4 and 5 reproduce typical situations that one may observe experimentally. (1) High loading: after achieving the maximum the R/Ro reduces to 1.4 and to 1.6 for H and D, respectively. (2) Low loading: after achieving the maximum R/Ro reduces only a little bit since the dissolution of H or D stops because of the stress (unless a contaminant on the surface inhibits the dissolution of H or D).

R/Ro in Pd with high H solubility: calculated evolution 2.0

a

200

400

600

800

1000

Time (arb. units)

Figure 4.

Calculated evolution of R/Ro

for high solubility (reduced stress) material.

122

R/RQ in Pd with low H solubility; calculated evolution

t

2.0 r

Pd foil Young module 1011 Pa

1.0 f

0.5 L 0.0 200

400

600

800

1000

Time (arb. units)

Figure 5.

Calculated evolution of R/RQ for low solubility (high stress) material.

The model allowed us to seek for a material showing a homogeneous loading able to minimize the concentration gradients and then the stress field. Some treatments, based on cold and annealing steps allowed us to optimize metallurgical structure of the materials in order to increase the H(D) loading. The row material was palladium foil 0.5 mm thick able to reach a loading ratio of about 0.8 (hydrogen atomic ratio). The treatment has been done in two steps: 1. Cold rolling of the row material leading Pd foil 50 /im thick. 2. Annealing at different temperatures (ranging from 700 and 1100°C) for different times. Figure 6 shows a simply cold worked sample. Figure 7 shows the effect of the annealing (1100°C for 5 h) after rolling , the sample microstructure is changed and it is clear the growth of the grains. Figure 8 shows the microstructure of a sample annealed for 1 h at 850°C after rolling.

Figure 6.

Cold worked palladium.

123

Figure 7.

Palladium annealed at 1100°C for 5 h.

Figure 9 shov/s the effect of the treatment (i.e. of the metallurgical structure on the H (D) loading). H/Pd = 0.97 has been obtained in the sample cold worked and annealed at 850° C for 1 h. A possible interpretation of. such a results is that in the last considered sample the concentration profiles are maintained relatively flat because of the reduced size of the grains. The above-described tests have shown a satisfactory reproducibility. Another interesting effect found in the experiments is the correlation, that some time occurs, between the loading dynamics and the loading ratio. One may observe that after loading at constant current density for a certain time, the concentration of the solute in the metal does not increase any more and sometimes a de-loading takes place. On the basis of the concepts exposed in the previous section, we assumed that such a behavior was promoted by the creation of a stress field very close to the surface of the sample under the electrochemical loading. Stress removal has been performed by applying a low-high current mode, just to avoid the creation of a new stress field. The effect of this technique is well described in Ref. 6.

Figure 8.

Pd cold worked and annealed at 850° C for 1 h.

124

Thermal treatment effect on hydrogen loading

0.6

—. I

0.0 600

800

700

900

1000

1100

1200

1300

Temperature (°C) Figure 9.

Effect of the thermal treatment on the loading.

4. Calorimetric Results Flow and isoperibolic calorirnetric measurements have been performed by using pre-treated palladium into electrochemical cells with LiOD 0.1 M electrolyte. 4.1. Flow

Calorirnetry

Excess of power measurements has been carried out by using a flow calorimetric system composed by a Memmert thermostatic box (±0.05°C), Haake thermostatic bath for coolant water, Bronkhorst high precision mass flow meter and controller (0.3-0.1 cm 3 /s), read by the data acquisition system in order to have a precise measurement of the output power. He leakage tested cell (2 x 10~ 10 mbar 1/s) is immersed into a water jacket cooled by a water coolant pipe. Inlet and outlet iniei ouuei temporal measurement

Temperature contra with external circuit pumping unit (only pumping purposes)

I

««™

,

Temperature c )ntrol with external circuit / pumping unit /

\\

'

Flow controller with solenoid ! valve liquiflow i r

.•"•"'*

1k

J \

^

r

'^^

i ^

: i Thermal ' pncubatioa *Mfe • ! ?£rrKjnrg#§#j$ ft ! tjn* / £

i

' V | y A;

,

!

\ 1 i

! i

i

nnmn

c '*J«f • r;8Bt?iisti**t^

—j !• • • • alized water batr

Figure 10.

^vw^rt^i

.,

Flow calorimeter system.

125 4000

I

3500 3000 2500 2000 1500

N§i

2* !

] •3&fe*&ss$

\

- P|„ (mW) -PM(mW)

1000 500

\

\,.^

0

20,000 40,000 60,000 80,000 100,000

Time (s)

Figure 11. LiOH.

Input and output power during an experiment performed with LiOH 0.1 M electrolyte

temperatures of the coolant are measured with two Pt 100 thermometers (four wires measurement). The closed electrochemical cell is equipped with a recombiner. Cell power supply is an AMEL galvanostat, modulated, during the HI-LO current mode by an HP 33120 wave function generator. Output power is measured by means of the mass flow rate and coolant temperatures, R/RQ measurement is done by means of an HP-4284 (four wires measurement). Figure 10 shows a schematic view of the flow calorimetric system. Several experiments have been done by using light water (LiOH 0.1 M electrolyte) obtaining a calorimeter efficiency of 97.5% (output = 0.975 input, because of the heat losses). No excess of power production has been observed by using H2O despites a very high loading (H/Pd = 0.97) was always achieved. A different behavior has been observed in several cases by using LiOD electrolyte. Excess of power has been obtained in CI, C3, and C4 experiments under high loading of D into Pd (D/Pd > 0.92). Figures 11 and 12 show the input and Calibration energy (LiOH) 10,000

100,000,000

p-N

! Output energy

[Calorimetric efficiency - 97.5%|"

UJ

60,000,000

6000

40,000,000-

4000

of

20,000,000

0 20,000

40,000

60,000

80,000

100,000

Time (s)

Figure 12.

Plot of energy and power (input and output) for calibration with H2O 0.1 M.

120

P„ (mW)

£ -

P«* (mW)

£

20.000

40,000

60.000

Time (s)

Figure 13. Experiment C3: excess of power versus time (input and output). C3 experiment: plot of energy and power.

output power and energy for an experiment that may be considered as a reference experiment performed with light water. No evidences of excess of power are observed and the output energy perfectly respects the efficiency of the caloriinetric system that recover 97.5 of the input power, so that the output energy curves always maintains below the input. Figures 13 and 14 show the C3 experiment evolution of the input and output power and energy. After 25,000 s, at high loading (D/Pd > 0.92) the output power overcame the input one and the bursts survived up to 60,000 s giving an output power 80% larger than the inputDespites the short lifetime of the burst a completely different behavior, of the energy curves (Fig. 14) (if compared with the reference experiment) may be observed: during the excess of power production also the output energy curve overcome the input one. A similar behavior has been observed in C I and C4 experiments. Three excesses of powers have been observed over nine experiments although the achieved D concentration in Pd (atomic fraction) was always larger than 0.9. Then the load100.000.000

0

10.000

20,000

30.000

40.000

50.000

60.000

70.000

Time (s) Figure 14.

Isoperibolic calorimeter and electrochemical cell for Laser triggering.

127

ing threshold D/Pd > 0.9 is clearly only a necessary condition. An upgrade of the experiment has been conceived in order to increase the reproducibility of the excess of power production. 4.2. Isoperibolic Triggering

Calorimetry

under Plasmons-Polaritons

Laser

An isoperibolic calorimetric system has been developed allowing a Laser irradiation during the electrochemical loading. According to the idea that collective electron oscillations have a key role in LENR processes a proper trigger has been introduced to create surface plasmons (polaritons). Surface plasmons are quantum of plasma oscillations created by the collective oscillation of electrons on a solid surface. Surface plasmons may be generated by mechanisms able to produce charge separation between Fermi level electrons and a background of positive charges (i.e. lattice atoms): 1. 2. 3. 4.

Electrons beam. Laser stimulation. Lattice vibrations. Charged particles interacting with a surface.

Laser triggering was selected because of its results to be the most appropriate under electrochemical loading. Needs to underline that plasmons are longitudinal plasma oscillations that do not couple with external radiation. A prism or cylindrical lens in contact with the surface to be irradiated with a Laser can be used in order to have the required coupling. The alternative is to irradiate a rough surface and for such a reason a proper acid etching has been done on the Pd samples used as cathodes into the electrochemical cell. In addition to that one may consider that a p-polarized Laser beam is the appropriate one to create charge separation on the surface of the specimen. The electrochemical cell, equipped with two small glass windows was placed into a thermostatic box (±0.15°C) also equipped with a window for the Laser beam (5 or 33 mW, 632 ran) as shown in Figure 14. All the instrumentations and the data acquisition system are quite similar to the equipment above described for flow calorimetric system. Four experiments have been carried out into the isoperibolic calorimetric system and have been labeled Lasers 1, 2, 3, 4. Laser 1 was a calibration done by using light water (0.1 M LiOH) and the calibration curve is shown in Fig. 15. Despites the behavior of the system was quite linear a proper fitting curve has been used in order to have R2 = 1. Laser 2 experiment was performed by using 0.1 M LiOD electrolyte in heavy water. After 320 h about a square wave current was applied in order to increase the D loading into the cathode, according to the effect described in Section 1 of the work. After achieving a loading D/Pd of about 0.94 a 632 red Laser of 5 mW was continuously applied under continuous current electrochemical conditions. An

128

Calibration 25-5-2004 - . • . - : -. .•-

•- 3 6 2 6 * + 24.337A" = 1

~+~ T (average) Pdi. (T (average))

0

1

2

3

4

5

6

An(W)

Figure 15.

Calibration curve for isoperibolic calorimeter.

excess of power, ranging from 60 mW up to «300 mW (see Fig. 16), was revealed. At the end of the experiment the excess of energy was 23.5 kJ (17.3 MJ/mol Pd). In Laser 3 experiment a 33 mW, 632 nm Laser was applied after achieving a loading D/Pd = 0.95 under square wave current mode. During the experiment the Laser polarization was changed from "p" to "s" and vice versa. The effect is shown in Figs. 17 and 18. Seems clear, as expected, that the excess of power takes place under "p" polarization and disappears by applying "s" polarization. An amount of 3.4 kJ of energy (2.5 MJ/mol Pd) was produced during the experiment. Laser 4 experiment was carried out by applying a continuous electrochemical current. After achieving a loading threshold of 0.95 the cathode was continuously irradiated by using a 632 nm, 33 mW red Laser. Calorimetry gave 30.3 kJ of produced energy (19.4 MJ/mol Pd). Figure 19 shows the input and output power and energy evolution after applying the Laser irradiation. Laser 2 experiment: excess of power

31^

33b

330

Time (h)

Figure 16. Evolution of the input and output power, last 30 h under Laser irradiation (ppolarization), 632 nm, 5 mW. 4 He production estimate 6.12 X 10 1 5 .

129

Esp LiOD, 5-07-2004 Pol.P

— /cell (A)

.

— P.(W) P... (bar)

—fliflicoretla

Time (h)

Figure 17. Excess of power under Laser triggering (p and s-polarization effect). 632 nm, 33 m W HI LO current mode.

5.

4

H e Measurements

Increasing of 4 He concentration in the electrochemical cell was expected, by assuming that the excess of energy produced was created by a D + D = 4 He + 24 MeV reaction. He tight cells (2 x 1 0 - 1 0 mbar 1/s He leakage test) have been used in both flow and isoperibolic calorimeters. The gas in the cell was analyzed at the beginning of the experiment, during the experiment when no excess of heat was observed and at the end of the experiment. A gas sample was sent from the cell to an inlet system for the mass spectrometer. All the manifolds were realized by using VCR fitting and maintained under baking before and during measurements. The manifold is under vacuum at 2 x 1 0 - 5 mbar before sending a gas sample. The whole line was checked for He

Laser off

I Esp LiOD. 5-07-2004

J.b

\ 33

3.2

i

x — (cell (A) — P„(W) P.-(bar) — MR, coretla — PW(W)

. 2 6

P.pol

7Z.

103

Time (h)

Figure 18.

Excess of power under Laser triggering (Laser off effect). HI-LO current mode.

130

Excess of energy and power in Iaser4 experiment •Output energjE-|tA £ = 30kJ| Inptttetjierjgy 2.20

S

g 150,000

Figure 19.

Excess of energy and excess of power in Laser 4 experiment.

leakage giving 10~ 10 mbar 1/s. A 707 Saes getter was used to trap deuterium, oxygen and nitrogen from the sample gas before sending it to the MS. Figure 20 shows a scheme of the system. The mass spectrometer used was a high resolution and high sensitivity Jeol CG-Mate. Figure 21 shows the resolution for mass 4. It is clear that the resolution is high enough to separate 4 He and D 2 (resolution limit is 10~ 4 amu). Figure 22 shows the results of the analysis giving the 4 He concentration measured in the cells at the end Lasers 2-4, experimental values are also compared with the expected values and with the background. 6. Conclusions Heat effects are observed with D, but not with H, under similar (or more severe) conditions. All VCR fitting, He leakage of the line <10 MKSbaraton

Figure 20.

mbar l/s MKSbaraton

Mass spectrometer inlet line.

131

JEOL GC-MATE Peak profile for mass i Sensitivity in SIM mode is up to some fm-gr D2

f AM = 0.0256 amu

4

j

_Jl

I

Figure 21.

j

i

_J

He

Jeol GC Mate mass 4 resolution.

Heat bursts exhibit an integrated energy at least 10 x greater than the sum of all possible chemical reactions within a closed cell. Experiments reproducibility was significantly improved as a result of material science study. Some conditions are required to have a reproducible excess of power: 1. 2. 3. 4.

Loading threshold D/Pd > 0.9 (necessary condition). Suitable material to have a reproducible loading above the threshold. Trigger. Suitable status of the material to have coupling with trigger.

Three excess of power over three effective experiments have been achieved by respecting these conditions during electrochemical experiment! The accordance 4-He Mass spectrometry for laser trigerred experiments

O

0.80x10'°^.

X

0.60x10"

Figure 22. The expected amount of increasing of 4 He is in accordance with the energy gain by assuming a D + D = 4 He + 24 MeV reaction.

132

between revealed 4 H e and produced energy seems to be a clear signature of a nuclear process occurring in condensed matter.

Acknowledgments T h e authors would like to t h a n k Dr. Guido Petrini of Sued Chemie for his support for all the scientific aspects concerning catalytic materials. In particular, for giving b o t h the catalysts t h a t have been used for MATRIX experiment and for closed electrochemical cells. Dr. R. Hartens, Dr. 0 . Seguin, Dr. S. Quill, Dr. A. Kusai, and Dr. F . Dalia of J E O L for their help in optimizing for the experiments the J E O L J C - M a t e Mass spectrometer used. Mr. D. Lecci, Mr. F . Marini, Mr. Polinari, Mr. Marcelli, and Mr. Bettinali of E N E A for their technical support. Dr. S. Lesin, Dr. A. El Boher, and Dr. Tanya Zilov of Energetics Technologies Ltd. for the very useful interaction t h a t positively affected t h e research work.

References 1. H. Wipf, J. Less-Common Met. 49, 291 (1976). 2. F. A. Lewis, J. P. Magennis, S. G. McKee, and P. J. M. Sebuwufu, Nature (London) 306, 673 (1983). 3. F. A. Lewis, B. Baranowski, and K. Kandasamy, J. Less Common Met. 134, L27 (1987). 4. F. A. Lewis, X. Tong, K. Kandasamy, R. V. Bucur, and Y. Sakamoto, Electrochem. Acta 218, 57 (1993). 5. R. A. Oriani, Trans. Fusion Technol. 26, 235-266 (1994). 6. A. De Ninno, A. La Barbera, and V. Violante, Consequences of lattice expansive strain gradients on hydrogen loading in palladium. Phys. Rev. B, 56 (5), 2417-2420 (1997).

HEAT M E A S U R E M E N T D U R I N G P L A S M A ELECTROLYSIS

K. I I Z U M I , M. F U J I I , S. M I T S U S H I M A , N. K A M I Y A A N D K.-I. O T A Chemical

Energy

Laboratory, Yokohama National University 79-5, Hodogaya-ku, Yokohama 240-8501, Japan E-mail: [email protected]

Tokiwadai,

It is important to establish an accurate heat measurement system to confirm the excess heat from the cold fusion phenomenon. During plasma electrolysis, an accurate heat measurement is especially difficult, because the input power is large and it causes significant evaporation of electrolyte and heat loss to the environment from the body of the electrolytic cell. In this study, a flow calorimetry system has been developed for accurate measurement. The energy balance of plasma electrolysis was measured at 100-102%, and the current efficiency were from 115 to 122% during the plasma electrolysis in 0.3mol/dm 3 Na2CC>3 light water solution. Clear excess output energy has not been observed. Excess gases of 15-22% generation beyond Faraday's law was confirmed. The excess gas generation might be due to a plasma reaction.

1. Introduction Mizuno et al. reported excess heat and hydrogen generation during plasma electrolysis. 1,2 To confirm them, an accurate determination of energy balance that includes the sum of latent and sensible heat is required. To determinate the sensible heat an accurate measurement is difficult because of the high input energy of plasma electrolysis. In this study, to perform accurate heat measurements, we developed a flow calorimetry system using a flow cell system, and we measured the energy balance during plasma electrolysis. 2. E x p e r i m e n t Figure 1 is a schematic diagram of the electrolytic flow cell. The cell was composed of acrylic tubing. It had an internal diameter of 2 cm, an external diameter of 5 cm, and was about 30 cm in length. The anode was a 2 cm diameter hollow cylindrical platinum mesh (99.99% purity, 55 mesh). The cathode was a 1.5mm diameter tungsten rod (99.95% purity). It was placed at the center of the cylindrical anode. The distance between the electrodes was 1 cm. The electrolyte was 0.2 M K 2 C 0 3 light water solution or 0.3 M N a 2 C 0 3 light water solution. The electrolyte circulated in this system, passing through a reservoir. The temperature difference between the inlet and outlet of the electrolyte was measured with Pt resistance thermometers. Hydrogen and oxygen generated 133

134

W cathode Teflon coating 99.95%, 1.5mm 1.5 cm in length .I I |h

.—K Electrolyte ,^ outlet Acrylic plastic tubing Pt anode 99.99% 2cm, 55 meshs 1.0 cm in length

1_J~

__ Pt resistance thermometer

Electrolyte inlet Figure 1.

Schematic diagram of a flow calorimetry cell.

during electrolysis were collected in the reservoir, and the rate of gas generation was measured. During electrolysis, the cell voltage and the current, the inlet and outlet temperatures of the electrolyte, room temperature, reservoir temperature, and the electrolyte flow rate were measured. The heat loss through radiation from our system should be negligible, because the flow of the electrolyte was controlled so that the temperature increase of the electrolyte was kept under 5°C, and the electrolyte temperature was kept very close to the room temperature. Table 1 shows the experimental conditions during the energy balance measurements in 0.3 M Na2CC>3 light water solution. The inlet temperature of the electrolyte were kept at 26°C. The flow rates of the electrolyte were fixed at the range of 681-825 ml/min. Electrolysis was conducted at constant voltage. The energy balances were determined by the experimental operation times of 1, 2, 3, and 4h, respectively. The energy balances of the run numbers hl-h4 were measured during plasma electrolysis at 95 V, and that of run number h5 and h6 were measured during normal electrolysis at 34 and 39 V, respectively. Also, cell voltages, inlet temperatures and flow rates of the electrolyte were kept constant during the energy balance measurements.

135 Table 1.

Experimental conditions during energy balance measurements

Run

Operation time (h)

Inlet temperature of the electrolyte (°C)

Flow rate (ml/min)

Cell voltage (V)

hi h2 h3 h4 h5 h6

1 2 3 4 1 1

26 26 26 26 26 26

688 707 710 681 684 684

95 95 95 95 34 39

The input energy was measured as the product of the cell voltage and the current. The output energy was the sum of sensible and latent heat. The sensible heat was determined by the temperature difference between the outlet and inlet of the electrolyte. The latent heat was determined from the flow rate of the gaseous product. The energy balances were calculated by the following equations. Ein = UI,

(1)

Hs = / E A T d C P )

(2)

Hh = feAH,

(3)

Eovlt = Hs + HL,

(4)

EB

(5)

= *£*.

Here, Ein, U, I, Hs, / E , AT, d, Cp, H^, fg, AH, Eout, and EB were the input energy, the cell voltage, the cell current, the sensible energy that was obtained by the temperature increase of the electrolyte, the electrolyte flow rate, the increase between the inlet and outlet of the electrolyte temperature, the density of the electrolyte, heat capacity of the electrolyte, the latent energy of the H2 and O2 evolution, the generated gas flow rate, the enthalpy change of the water electrolysis, the output energy, and the energy balance, respectively. The current efficiency is the gas generation amount per the theoretical amount by the Faraday's law. Therefore, the details are as follows: / t h = n(I/F)(JRTgas)/(Pair V = /g//th-

-

PH2O),

(6) (7)

Here, n, /th, F, R, T gas , P a ; r , J3H2O, and 77 were gas generation amount per electron, theoretical generated gas flow rate, Faraday constant, gas constant, temperature of the H2 and O2 produced during electrolysis, atmospheric pressure, vapor pressure, and current efficiency, respectively. The theoretical generated gas flow rate was determined from Faraday's law of water electrolysis. Therefore, the ratio of hydrogen to oxygen was 2:1.

136

3. Results and Discussion Figure 2 shows the cell voltage and the current as a function of time. The cell voltage was controlled by a step function, which increased the voltage by 10 V at 20-s intervals. At the beginning, the current increased with the voltage from 20 to 80 V. After that, the current decreased with the increase of the voltage from 80 to 130 V. Plasma discharge started in this region. The bright plasma was observed above 130 V. Once, bright plasma was formed, it was maintained above 90 V. Plasma discharge stopped if the voltage dropped below 90 V, and the current increased from 2 to 13 A at this moment. The resistance of the cell during plasma discharge was higher than that of normal electrolysis. 200 160

12

>" •— 1 2 0 (D D)

c

\1 YlPlasma discharge i

-

J

0 0

1

1

1

2

4

6

CD 3

4

O

egjon 1

8

10

Time (min) Figure 2. Trend of input voltage and current during normal and plasma electrolysis in 0.2 M K2CO3 light water solution.

Figure 3 shows the current as a function of time during normal and plasma electrolysis. The experimental conditions are shown in Table 1. Before plasma electrolysis at 95 V, the current increased to 130 V by lOV/s. After bright plasma formed, the voltage decreased to 95 V by 50mV/s and the energy measurements were started. At the beginning, the currents were ca. 2.2 A for the plasma electrolysis and the currents decreased to 1.9 A after 100 min of operation. After the plasma electrolysis, the consumption of the tungsten cathodes was observed. On the other hand, the current was constant due to the constant voltage during normal electrolysis. Figure 4 shows photos of tungsten cathodes before and after plasma electrolysis at 95 V in 0.3 M Na2C03 light water solution. The tungsten cathodes were consumed by means of plasma electrolysis. For 1 h operation, the cathode decreased 0.5 mm in length and 0.09 g of the tungsten was consumed. For 4h operation, the cathode decreased 3.6 mm in length and 0.30 g was consumed. During plasma electrolysis, much of the cathode was consumed, and the electrode surface area was reduced.

137

A O O Q • A

A-*A

•-•-* -

hi h2 h3 h4 h5 h6

3

o

^ ^ e ^ 100

200

300

Time (min) Figure 3. solution.

Cell currents during normal and plasma electrolyes in 0.3 M N a 2 C 0 3 light water

Figure 5 shows the outlet temperatures of the electrolytes during normal and plasma electrolysis. The inlet temperatures were 26°C in all cases. The outlet temperatures decreased due to the current decreases during plasma electrolysis. On the other hand, the outlet temperatures were constant due to the constant voltages and currents during normal electrolysis. Figure 6 shows the current efficiency during normal and plasma electrolysis. The current efficiency of the plasma electrolysis were 115-122% except the fluctuation of h4 after 100 min and these of normal electrolysis were 91-98%. The excess gas generation could not be explained by Faraday's law. Therefore, the excess gas must have been generated by the plasma process. Also, a small amount of CO2 was detected during plasma electrolysis by means of a gas chromatograph. Figure 7 shows the energy balances during normal and plasma electrolysis. The energy balances of the plasma electrolysis were 100-102% except during a period of fluctuation shown in the data for h3. The energy balance for normal electrolysis was 91-98%. Although, a small amount of excess energy was detected during plasma electrolysis, clear excess was not observed.

^mm jnii

mi

(a) Before electrolysis

(b) After 1 h

(c) After 4 h

Figure 4. Photos of tungsten cathode before and after plasma electrolyes at 95 V in 0.3 M Na2CC>3 light water solution, (a) Before electrolysis, (b) after 1 h, and (c) after 4 h.

138

31.0 A hi

R

30.5

CD 30.0 •3 •<-•

2 CD

29.5

fc

29.0

O.

° h2

^W ***

.C

O h3

a h4 • h5 A h6

\

28.5 28.0

I

1

100

200

300

Time (min) Figure 5. Outlet temperatures of the electrlolytes in during normal and plasma electrolyses in 0.3 M Na2CC)3 light water solution.

4. Conclusions The energy balance during plasma electrolysis was 100-102%. Clear excess energy could not be detected. The current efficiency during plasma electrolysis was 115-122%. A small amount of CO2 was also detected during plasma electrolysis by means of a gas chromatograph. A gas generation reaction other than the electrochemical process took place during the plasma electrolysis, and generated excess gas. Further study is necessary, especially, related to the composition of the effluent gas.

140

100

200

300

Time (min) Figure 6. solution.

Current efficiencies during normal and plasma electrolyses in 0.3 M Na2CC>3 light water

139

108 106 en 104 o cCO CO 102

> A O O • • A

ergy

X!

c LU

100 98 96

1

100

hi h2 h3 h4 h5 h6

1

200

300

Time (min) Figure 7. solution.

Energy balances during normal and plasma electrolyses in 0.3 M Na2CC>3 light water

References 1. T. Mizuno, T. O h m o r i , T . A k i m o t o , a n d A. Takahashi, Jpn. J. Appl. Phys. 3 9 , 6055 (2000). 2. T . Mizuno, T . A k i m o t o , K. A z u m i , a n d T. O h m o r i , Jpn. J. Appl. Phys. 4 4 , 396 (2005).

EFFECT OF A N A D D I T I V E ON T H E R M A L O U T P U T D U R I N G ELECTROLYSIS OF HEAVY WATER W I T H A PALLADIUM CATHODE

Q. W A N G A N D J. D A S H Low Energy

Nuclear

Laboratory,

Portland State University, E-mail: dashjQpdx. edu

Portland,

OR 97207,

USA

A titanium additive to a heavy water-sulfuric acid electrolyte has been found to increase the thermal output during electrolysis with a palladium foil cathode. Eight runs, about 6 h each, over a period of 16 days, gave an average of 1.8 W excess thermal power output compared with a light water control cell. This is about twice the excess obtained in co-deposition experiments. The excess thermal power output ranged from 0.5±0.1 to 2.6±0.1 W, which was an average of about 17% more than the input power. The additive apparently catalyzes heat-producing reactions on the surface of the palladium. After electrolysis, the Pd cathode contained localized surface concentrations of Ag, Ni, Fe, Ti, S, and Pt.

1. Introduction During electrolysis of D2O-H2SO4 electrolyte with a Ti cathode and a Pt anode, Ti erodes from the cathode and dissolves in the electrolyte. 1 When this electrolyte containing dissolved Ti was used for electrolysis with a Pd cathode and a Pt anode, enhanced excess heat was observed. Also, localized concentrations of unexpected elements were found on the surface of the Pd cathode. This report contains data on the variation of excess heat production with concentration of Ti in the electrolyte and on the variation of the magnitude of the excess thermal power over a period of 16 days. Data on the distribution of elements on the Pd cathode are also presented. 2. Experimental Methods and Results The closed electrolysis cells and the excess heat calculation method used for this research were described previously.2 Figure 1 shows the circuit diagram used for electrolysis. A control cell with two Pt foil electrodes is connected in series with an experimental cell containing a Pt foil anode and a Pd foil (0.35 mm thick) cathode. The Pd was Alfa Aesar stock number 11514, 99.9% Pd (metals basis). The as received thickness was 0.5 mm. It was cold rolled to 0.35 mm thickness and then sheared to produce a cathode 23 x 25 mm. A 1 mm diameter Pt lead wire was then crimped to the Pd cathode through a hole, which was punched in one end of the Pd. A 1 mm diameter Pt lead wire was crimped to the Pt electrodes in the same way. The electrolyte in the control cell contained concentrated H2SO4 and deionized 140

141

EbOin the ratio 1:12.3. The experimental cell electrolyte contained the same batch of concentrated H2SO4 and Aldrich D 2 0 (catalog number 34,716-7) in the ratio 1:6.7. The average current density on the Pd cathode was about 0.3 A/cm 2 .

Figure 1. Circuit containing a constant current DC power supply and a control cell in series with an experimental cell. The black circles indicate the locations of eight thermocouples attached to the outside of each cell. The output of the thermocouples and the cell voltages were monitored with a computer. The cell temperature was then calculated as the arithmetic average of these eight readings.

Figure 2 shows the effect of Ti additions to the experimental cell electrolyte on excess thermal power. Data points with no added Ti and with 0.002 g/ml added Ti show that no excess heat was produced. After increasing the Ti content to 0.011 g/ml, two consecutive runs gave significant (0.2 and 0.4 W) excess thermal power. At 0.022 g/ml Ti concentration, three runs gave 1.2, 0.7, and 1.0 W excess thermal power. At higher concentrations of Ti, a Ti compound deposits on the cell wall. Figure 3 gives the excess heat results for eight consecutive runs with a new batch of electrolyte containing heavy water and sulfuric acid in the same ratio as before and with 0.024 g/ml Ti added. The data in Fig. 3 for six of eight runs show that the calculated excess thermal power assuming no mass loss is almost the same as the results obtained when the mass loss is included in the calculations. For the 8/9 and 8/15 data, the control cell

142

(3-23-05)-(5-9-05) Excess thermal power versus Ti content of the electrolyte CO

x a 1.5

£

0.5 0.005

0.01

0.015

Ti (g/ml)

Figure 2. Excess heat approximately doubled after Ti content of the electrolyte was increased from 0.011 to 0.022 g/ml. At higher concentrations of Ti, a Ti compound deposited on the cell wall.

lost ~ 1 g more mass than the experimental cell, and the calculated excess thermal power is not accurate. For the other runs, both cells lost less than 0.5 g, and the calculated excess thermal power is thought to be accurate. The Pd electrode used for the data in Fig. 3 was examined with a scanning electron microscope equipped with an energy dispersive spectrometer. Characteristic X-ray spectra were taken from each of the rectangles, on both the concave and the convex sides shown in Fig. 4. Figure 4 shows light microscope photographs of the two sides of the Pd cathode from which excess heat reported in Fig. 3 was obtained. The electrode is approximately 2.3 cm wide and 2.5 cm height. The EDS spectra were obtained by scanning the area in each rectangle. Examples of the spectra are shown in Fig. 5. Excess thermal power obtained using Pd cathode with Ti added to the electrolyte (August 2005) o

CO

x o

3

E

1.5

0

0

2

Q. "CO

9

2.5

•

;

•

0

o

•

*

•

•

•

O

4 -XS with mass correction

•

1

CO

co CD

o

X HI

0.5

0

B -XS with mass correction no Ti

-_

0 —' B ' 8/1

jtV -XS without mass correction no Ti

"

8/6

8/11

8/16

8/21

8/26

Date Figure 3. Excess thermal power with and without mass correction. Average excess is 1.8 W. Mass correction was calculated in order to account for the loss of recombination heat due the escape of gases from the cells.

143

l

!P*(WP

iflsRp (•ikt^'iP """ X"

gj&'K

•f

|

*' i

"•- j l

•

/A

f

¥$••••••

4k'r 1 ''

'

i nr—

•

''

Figure 4.

B£

Iff;

(a) Side facing anode (concave), (b) Back side (convex).

The upper spectrum in Fig. 5 was taken from the rectangle on the left-hand side of center in Fig. 4a, and the lower spectrum in Fig. 5 was taken from the rectangle in the upper left corner of Fig. 4a. Both spectra have predominant Pd La peaks at 2.84 keV, but the Pd L/3 peak at 2.99 keV is far more intense in the lower

PdLcc No Ag detected

3

4

Energy (keV)

PdLp

,

Figure 5. The upper spectrum was taken from the rectangle on the left-hand side of center in Fig. 4a, and the lower spectrum was taken from the rectangle in the upper left corner of Fig. 4a.

144

spectrum t h a n in the upper spectrum. T h e expected intensity ratio, P d L/3/La, is 0.42, 3 whereas this ratio in t h e upper spectrum is 0.43, and it is 0.97 in t h e lower spectrum. A possible explanation for this difference is t h a t Ag, which has its L a peak at 2.98 keV, is present at some locations on t h e P d cathode after electrolysis, as proposed previously. 4 Further evidence t o support this suggestion is t h a t t h e Ag L/3 peak at 3.15 keV is fully developed in the lower spectrum, b u t it is not prominent in the upper spectrum. ISIS deconvolution software was used t o determine the ratio A g / P d for each of the rectangles in Fig. 4. This ratio was 0.64 for t h e lower spectrum and zero for the upper spectrum in Fig. 5. T h e number on each rectangle is the ratio A g / P d for t h a t area. For example, t h e number 0.64 for upper left corner, concave side, tells us t h a t the number of Ag atoms is 64% of t h e number of P d atoms in t h a t area. T h e concave side faced the anode during electrolysis. T h e silver is concentrated near the left edge of the concave side. Ag was not detected in two rectangles near t h e center of the concave side. No high concentrations of Ag were found on the convex side of the P d electrode. 3.

Discussion

T h e addition of about 0.02 g / m l of T i t o the electrolyte enhances t h e o u t p u t of excess thermal power, and also improves reproducibility. T h e mechanisms, which produce these effects are not known. However, Ti is known t o have catalytic properties. 5 It may be t h a t a complex of Ti deposits on t h e P d cathode and activates sites, which would otherwise remain dormant. T h e spectra in Fig. 5 b o t h have small T i peaks, which probably result from the deposition of a Ti complex. In addition to P d , Ag, and Ti, the lower spectrum in Fig. 5 contains appreciable amounts of S, Fe, Ni, and P t . These elements are not detected in t h e upper spectrum of Fig. 5. S and P t most likely are deposited from the electrolyte. T h e origin of Fe and Ni is not known. It is unlikely t h a t these elements were present in appreciable amounts in the electrolyte. Acknowledgments This research was supported by a grant from t h e New York Community Trust. References 1. J. Warner and J. Dash, Proc. 8th Int. Conf. on Cold Fusion; SIF Conf. Proc.,Vo\. 70 (Edited by F. Scaramuzzi), Bologna (2000), p. 161. 2. J. Dash and A. Ambadkar, Proc. 11th Int. Conf. on Cold Fusion (Marseille, France, 2004), p. 477. 3. G. G. Johnson, Jr. and E. W. White, American Society for Testing and Materials Data Series DS 46 (1970). 4. J. Dash, G. Noble, and D. Diman, Trans. Fusion Technol. 26, 299 (1994). 5. J. Liu, Y. Yu, Y. Li, H. He, H. Tan, and K. Xu, Chem. Abstr. 131, 1303 (1999).

T H E R M A L ANALYSIS OF CALORIMETRIC SYSTEMS

L. D ' A U L E R I O , V. V I O L A N T E , E. C A S T A G N A , R. F I O R E , A N D L . C A P O B I A N C O ENEA

Frascati Research

Center, E-mail:

V.Le E. Fermi 45, 00044 Frascati violanteQfrascati.enea.it

(RM),

Italy

PR. DEL P R E T E La Sapienza

University,

Via Eudossiana

18, 1-00184 Roma,

Italy

F . T A N Z E L L A A N D M. M C K U B R E SRI International,

333 Ravenswood

Ave.,

Menlo Park,

CA 94025,

USA

Calorimetric analysis has been carried out for both electrochemical and gas loading experiment. A finite element modeling for steady state and transient gave a satisfactory agreement with the experimental results. For electrochemical cells modeling was applied for isoperibolic and flow calorimeters with the main goal to optimize the system. For high-temperature gas loading experiments the modeling was applied to translate the temperature field (steady state and transient three-dimensional analysis), then, in such a case calculations allowed to perform the calorimetry. This experiment was a replication of the MATRIX experiment performed at SRI by some of the authors. 1 , 2 A correlation between 4 He production and excess of power during gas loading of deuterium in palladium was observed. Excess of power was estimated by means of the temperature measurements and by comparing experimental data with both the calibration data and the modeling results. Also the effect of the room temperature evolution was considered in the mathematical model of the experiment. 4 He tights stainless steel cell have been filled first with a Pd-based catalyst then loaded with deuterium or hydrogen (blank). After filling cells with gas we observed a different thermal behavior of the cells CI and C2 containing deuterium, compared to the cell C4 containing hydrogen. The temperature increasing in cells CI and C2 was estimated to be produced by an additional power source of 0.1 W. The measured excess of helium was consistent with expected value obtained by assuming that the excess of energy was produced by a D + D reaction giving 4 He+heat (24 MeV). The slope of the temperature increasing was larger in cells CI and C2, and after achieving a stationary condition for the system the temperature of cells CI and C2 increased again. During the thermal effect an analysis of the gas was done for the cells CI and C2. An increasing of the helium content was revealed for both the cells. The He concentration increased up to a factor larger than 2 in both cells CI and C2.

1. Isoperibolic Calorimetry at High Temperature This experimental device has been realized to observe the behavior of palladium particles adsorbed on a carbon support, in equilibrium with deuterium gas at particular loading conditions. The purpose of the study is to analyze and describe the thermal conditions and the heat flow around the experimental apparatus, in order 145

146

to characterize correctly all the system, thus improving the response level of the calorimetric apparatus in term of efficiency and heat excess signal. In a following step an accurate comparative study of heat and gasses out of cells will be performed. An important aspect is the evolution of the room temperature (T am b); it will be observed that a variation of few degrees in the room produces a corresponding variation in the active zone, although lower because smoothed by the inertia of the device. In order to separate the effect of heat excess from the effect of the room temperature evolution, a transient calorimetric description of the system is required, considering the effect of the room temperature evolution and oscillations in the mathematical description of the experiment.

1

H

h

Cells Feeding Sampling System

N

Known Volume

Mass Spectrometer |_ Cataly_sts

Figure 1.

j

Experimental set-up and detail of the reaction cell.

The model studies the transient system by taking into account the non-linearity given by the radiative heat transfer, that couples with the convective mechanism on the top of the cell, and the time-dependent boundary conditions given by the room temperature behavior.

147

The numerical simulation represents an important tool, able to translate the temperature measurement and map into heat flux evaluation: we use the finiteelement model (FEM) like an instrument of numerical simulation based on mathematical model of heat transmission. The solution can be achieved by solving the transient thermal model through a typical heat transmission equation (Fourier equation) over a three-dimensional domain. In Fig. 1, the experimental set-up and a detail of the reaction cell are shown. The experimental system has been realized assembling four 50 cm 3 stainless steel cells (Figs. 2 and 3) within a heated stainless steel support that is maintained at a controlled temperature (200°C) by nine resistance heaters. The palladium is contained as supported small particles in the active bed that is placed in the bottom of the cell. A small tube is used to refill the cell with deuterium in order to compensate the adsorption on the catalytic bed. The pressure of the cell, the catalyst, and the gas temperature are continuously monitored during the experiment; the system composed by the four cells and the stainless steel support is thermally insulated from the environment by using CaSi0 4 bricks. From the overview of experimental device shown in Figs. 2 and 3, we observe that it is possible to subdivide it in four parts, each one characterized by the same thermal behavior. Then the solution can be 3D Domain

7

Figure 2.

Mesh for FEM,

148

Figure 3. Four 50 cm3 stainless steel cells of MATRIX.

achieved by solving the transient heat transfer equation over the three-dimensional domain shown below (Fig. 3) with the relative boundary conditions marked over a significative section represented in Fig. 4. The heat transfer mechanism can be assumed to be convective around the experimental device but coupled with a radiative mechanism on the top due to the local high temperature. The environment temperature is time-dependent, so that the boundary conditions are moving: the first problem to solve is to obtain a proper approximating function for the room temperature. The domain can be assumed composed by nine regions each one different for chemical and physical parameters but homogeneous and isotropous (Ax = Xy = Xz); the model does not take into account the convective effect within the cells.

CZZ1

Kn

=-H(T-Ta)-OE(T4-Tg) dn

I

1 K„

=0 dn

•

Figure 4.

Kn

?L=-H(T-Ta)

dn

Boundary conditions.

149

The model is based on the classic Fourier equation: 8T div (A grad (Temp)) + Q = pcp df where A is the thermal conductivity (W/cm K), r the density (g/cm 3 ), and Q is the thermal load. The relative boundary conditions have the generic expression: Kn^

= -H(T-Ta)-ae(T'l-T*),

(2)

where H is the convective heat transfer coefficient (W/cm 2 K), T a the room temperature, e and s, respectively, the emissivity and the Boltzmann coefficient. During this analysis we have consider two external zones with different thermal features: on the top the temperature is more elevated than elsewhere. We can observe that the noise in the room temperature is smoothed by the device thermal inertia; so we can assume that the real forcing function, that should be applied as moving boundary condition, is a function obtained by filtering the noise from the room temperature. This condition can be obtained by mens of a Fourier's series development of the experimental data:

Tb

Tb Fourier

Figure 5.

Room temperatures and their approximation by Fourier series.

in

/ (x) = A0 + V ] (-4; cos ix + Bt sin ix).

(3)

i=l

The room temperature and the relative Fourier development are shown in Fig. 5. The results are represented in the last two pictures; in Fig. 6a comparison could be made between calculated and experimental data: the agreement between experiment and model appears to be satisfactory. In the final analysis, we consider the influence of heat power, concentrated within the active bed, over the thermal field; Fig. 7 shows the effect of an addictional

150

500 495

39 185 180 0 30 45 Time (h)

60

15

30

45

60

75

75

Calculated Experimental Figure 6.

Comparison between calculated and experimental data.

thermal load on the temperature behavior in corrispondence of measurement points, calculated with 0.1 W of power excess; the model reveals an increasing of about 1.2°C for an additional thermal load of 0.1 W corresponding to about 30 W for cubic centimeter of palladium. 2. Isoperibolic C a l o r i m e t r y at Low T e m p e r a t u r e The isoperibolic calorimeter for the characterization of deuterium loading on Palladium foils by electrolytic method Fig. 8 shows both a picture of the apparatus and its axial section, which allows to high light the most significant elements are shown. The experimental cell is formed by a Teflon shell closed on the upper side by a stainless steel cap; two circular quartz windows are placed for laser excitation of

Figure 7. Effect of an addictional thermal load on the temperature behavior in correspondence of measurement points, calculated with 0.1 W of excess of power.

151

;J^"

Figure 8.

Picture of the apparatus and its axial section.

Palladium surface. Inside a thin palladium plate constitutes the cathodic element surrounded by an anodic platinum wire. The temperature is continuously monitored through two Pt 100 sensors inserted in suitable measurement seats; a capacitive pressure sensor and a safety mechanical valve complete the experimental set-up. The calorimetric apparatus is entirely inserted in a thermostatic box to allow a stationary room temperature (24°C). Like for the previous one, also for this calorimetric device a numerical simulation with FEM method could represent a helpful tool to translate the temperature map into heat flux evaluation: a three-dimensional

Measurement

Palladium cathode

Quartz window for

Teflon Figure 9.

Three-dimensional domain for FEM analysis.

152

analysis allows to obtain, in operation phase, the theoretic efficiency of device in terms of sensitivity. Moreover, in planning stage, the numerical approach allows the feasibility of improvements in order to optimize the experimental apparatus functionality. The calorimetric study of the system, in such a case, has been carried out by means of a calibration with H2O. The constancy of room temperature allows to achieve a steady-state model whose solution is obtained through the application of Fourier equation on the three-dimensional domain shown in Fig. 9, where also the calculation mesh, the heat transfer equation, and the boundary conditions can be observed. In Fig. 10, the temperature behavior calculated in correspondence of measurement points within the electrolitic cell between 0 and 1 W of power supplied is shown; in the same picture the temperature profile obtained during a calibration campaign is represented. The difference between the sensitivity calculated and experimental one is about 1.3°C for Watt of power supplied under the considered working conditions: therefore the agreement between experimental and calculation data results reasonable.

Sensitivity 304 303 302 301 7"(K) 300 299 298 297 ,s**^ 296 0

_* ^^~ ^**

^rC-~-""*"

^*^* --""" J--*"" '""

^-r^-"""""4"

0.2

0.4

0.6

0.8

1

—*— S calc 1.2 -*— S exp

P(W) Figure 10. Calculated and measured temperature in correspondence of measurement points within the electrolytic cell between 0 and 1 W of power supplied.

3. Flow Calorimetry at Low Temperature A flow calorimeter for the loading of deuterium on palladium thin foils is shown in Fig. 11. A copper coil, in which water flows with suitable rate, envelops fully the electrolitic pirex cell. Inside cell, a palladium cathod and a platinum anod are placed. The cell is surrounded by a water jacket and is put in a plexiglass shell. A thermostatic box assures constant environment temperature. Two Pt 100 sensors are placed in correspondence of water inlet and outlet of copper coil, while the box temperature, the cell temperature, and pressure are continously monitored. The

153

temperature difference between the coming in and coming out water is proportional to the power produced inside the cell. Then the efficiency of the calorimeter is represented by the heat recovering capacity of water coil. The goal is to keep heat losses as lower as possible. The aim of this paper is to describe a possible approach to characterize the thermal behavior of flow calorimeter, such obtaining an accurate efficiency measurement: a multi-step procedure which links the heat generated by cell with the temperature profile of coil axis is described. In first approximation, it was considered that the entire heat produced is transferred to the coil water with 100% of efficiency and uniform power distribution, then, through a monodimensional approach, the temperature profile along coil axis is calculated by the equation below: rVcpdT=(W/L)dxJ1

(4)

where r is the density of water, V the volumetric flov/, L the coil length, and x is the abscissa of coil axis. In the following step a FEM calculation model was realized: the heat transfer equation in steady state is calculated over the two-dimensional domain shown in Fig. 12, with the same hypothesis described for isoperibolic calorimeter. The temperatures calculated in the first step are put inside the coil trace as inner boundary condition (2"), thus obtaining the temperature T around coil surface.

Figure 11.

Flow calorimeter.

154

Water temperature T w

Coil surface temperature=P

Figure 12.

Two-dimensional domain.

Fourier equation is div(A * grad (T)) + Q = 0.

(5)

Outer boundary condition Kn(dT/dn)

= H(T-Text).

(6)

Kn{dT/dn)

= H(T - Tw).

(7)

Inner boundary condition

Equations (5)-(7) allow us to calculate the temperature profile along coil axis: the solution is obtained by numerical calculation through Fortran code application. rVcpdT = Hp(T' - T)dx,

(8)

First step 27.4 27.2 27

HT!~ltti

2 6 8

o °L 26.6 K 26.4 26.2 26 25.8

Figure 13.

l^TT , rjL.-"

50

100 s(cm)

150

200

Coil temperature profiles in the first step and second steps.

155 where p is t h e perimeter of coil. For a more accurate analysis it is possible to repeat t h e iterative calculation of Eqs. (4) and (5) until the difference between two following steps is lower t h a n a slight value. In Fig. 13, t h e t e m p e r a t u r e profiles in the first step and in the second one are shown.

4.

Conclusions

T h e satisfactory agreement between t h e calculated and measured t e m p e r a t u r e values revealed t h a t t h e method applied to design the calorimetric devices and to translate t h e t e m p e r a t u r e m a p into thermal load is appropriate for the scope. In particular the methods allows to carry out an high-temperature isoperibolic calorimetry taking into account the fluctuation of t h e room t e m p e r a t u r e .

References 1. M. McKubre, F. Tanzella, P. Tripodi, D. Di Gioacchino, and V. Violante, ICCF8 Lerici (May 21-26, 2000) Conf. Proceed., Edited by Italian Phys. Soc. Vol. 70, p. 23. 2. M. McKubre, F. Tanzella, P. Tripodi, and P. Hagelstein, ICCF8 Lerici (May 21-26, 2000) Conf. Proceed., Edited by Italian Phys. Soc. Vol. 70, p. 3.

SURFACE P L A S M O N S A N D LOW-ENERGY N U C L E A R REACTIONS TRIGGERING

E. C A S T A G N A , C. SIBILIA A N D S. P A O L O N I La Sapienza

University,

Via Scarpa,

14, 00100 (Roma),

Italy

V. V I O L A N T E A N D F . S A R T O ENEA

Frascati Research Center, V.le E. Fermi 45, 00044 Frascati (Roma), E-mail: [email protected]; [email protected]

Italy

The study presented deals about both theoretical and experimental aspects of Surface Plasmons (SP) excitation. The principles of phenomenon rising are showed, together with the description of experimental devices needed to obtain such an excitation. The correlation between SP occurrence and electrochemical conditions is approached.

1. Introduction Surface Plasmons (SP) (polaritons) are quantum of plasma oscillations created by the collective oscillation of electrons on a solid surface. SP may be generated by mechanisms able to produce charge separation between Fermi level electrons and a background of positive charges (i.e. lattice atoms): • • • •

Electrons beam. Laser stimulation. Lattice vibrations = Phonons. Charged particles on a surface.

Existence of plasmons has been revealed at the gas/metal and electrolyte/metal Interfaces.1 A strong electric field enhancement arises during SP excitation. This phenomenon could be explained both with classical2 or quantum mechanical3 considerations. 2. Theoretical Aspects Bulk plasmon frequency is

<4 =

,

2.1

where N is the electron density at the Fermi level, e the electron electric charge, mefr the electron effective mass, £0 = 8.854 x 10~ 12 F i n - 1 the vacuum dielectric constant, and u is the separation distance. 156

157

The dielectric function of a metal is complex: (2.2)

E2 = E = E' + iE". The dependence of the wave vector

(2.3)

K = K' + iK"

of the plasma oscillation from the frequency at the surface of two semi-infinite mediums (Fig. 1) is the dispersion relation, which under certain conditions could be written as 4 K K

,

UJ

C\ „ x

-

j

E\E'

£!+£''

LO jsie'

., C V £i + e'

(2.4) e"

2e'2

If conditions e'<0,

e"<|e'|,

£i < |e'|

(2.5)

are satisfied, it follows: ,_w

j ei(w 2 -wj) c y w2(ei + 1) - w%2

•

(2.6)

i Y.

«1 y

Figure 1.

«

._, —.-«..

\s\-

""'"

' • •

Interface between two semi-infinite mediums and reference axis.

Expression (2.6) can be easily plotted (Fig. 2). Surface plasmons (polaritons) excitation by electromagnetic stimulation comes out when the real part of the x component of the wave vector of the incident wave results to be equal to the one of the SP (Fig. 2). The laser beam dispersion relation is K^

C

\Je\ sin#.

(2.7)

Electric field has to belong to the incidence plane, i.e. the wave has to be polarized in the p mode: if the electric field is perpendicular to incidence plane, and thus parallel to the interface (s-type polarization), it would assume the same value in the two mediums, without giving rise to the charge displacement needed to excite SP.

158

5x10

16

-Pd-air interface -Pd-glass interface

4x10

1

3x10 2x10 1 x10

0.5x10"

1.0x10"

1.5x10°

2.0x10 8

K>"1) Figure 2.

Surface plasmons dispersion law for a Pd-air interface and a Pd-glass interface.

The comparison between the expressions (2.6) and (2.7) gives the following plot (Fig. 3). No matching condition results to be possible between light lines and SP dispersion curve at an air-Pd interface: the matching condition cannot be satisfied on smooth surface, because the interaction between photons and plasmons cannot simultaneously satisfy the energy and momentum conservation.4 It is possible to obtain SP excitation also using a corrugation lattice or by corrugating the metal surface itself: such a corrugation increases the x component of the laser beam wave vector, making thus possible the coincidence with SP wave vector:6 Kx = -sm6±AKx c

= KSP,

(2.8)

where AKX is defined as

AKX = ±ng, 2TT 9 =

—

•

(2.9) (2.10)

The plot (Fig. 4) shows the possibility to satisfy the matching condition between the wave vectors of the two curves of interest. 3. Electro-Magnetic Field Enhancement due to Surface Plasmons Excitation Surface Plasmons resonance could give rise to a big local field enhancement, due to a focusing effect: a broad e.m. wave is confined in a surface. This phenomenon

159

5x10 16 4X10 1

<3? 3 x 1 0 '

i 3

2x10 1 6 Pd-air interface

K x '=co/c K'= a>/tcsin(30")

1x10'

1.0x108

0.5x10°

1.5x108

2.0x108

<(m-1) Figure 3.

Comparison between SP and laser beam dispersion law at two different incidence angles.

could be understood considering the wave vector component perpendicular to the interface between the two media: OJ

Kxl

Ei

(3.1)

E + Ei E2

K.

c V E + Ex

(3.2)

The field enhancement could be in a phenomenological way expressed as: 2 1^121 \Eo\

\Ki\ K"

(3.3)

Enhancement of about 102 factor could be obtained in this classical calculation. Using appropriate structures and quantum mechanical computation the enhancement factor could be equal to several magnitudo orders, ~ 106 (linear response). 3 4. Surface Plasmons in Electrochemical Conditions The electrochemical interface is well represented by a double layer structure in contact with a space of charges. 7

160

5x10

,16

/ / ,16

4x10

^ y

%

1 3

3x10

:

/ / /

16

/

im.

/

sp,a

2x1016

1x10

/

~—-^^

Z

/ 1 1

16 -

?

,

Pd-air interface K^ = co/csin(30")

/ /

i-f

i

0.5x10

B

1.0x10s

1.5x10B

2.0x10',8

<(m"1) Figure 4.

Increment h.Kx of laser beam wave vector due to roughness, giving rise to SP resonance.

Charge displacemet Uk associated with a SP of wave vector k in terms of harmonic oscillator in second-quantized form is: 7 h k (4.1) (ak + atk)e ikr e —kz , 2mu)s V nA where A is the area of surface and the dimensionless factor k/nA is required to normalize the oscillator amplitude. 8 After calculation, the total energy of the interacting system results to be: uk =

H = Y,f^s{b+b+

1/2) ~e2/Az.

(4.2)

k

Above equation shows that the change in zero-point energy of the SP oscillator system precisely corresponds to the classical image potential energy. External point charge induces a polarization charge density in a metal that is identical to the distribution induced by a set of SP. In principle, an electrochemical interface may be equivalent to a system with SP excitation. At the interface between metal and electrolyte the electrode potential EQ is given by:9 eE0 = AG A + Ad

+ AG Id

Vc,

(4.3)

where AG A is the free energy of atomization of the metal, AGj the free energy of ionization (that is the ionization potential), AG Hid the free energy of hydration, and 6 is the metal work function.

161

To create the double layer the minimum value of cathodic fall (Vc)min has just to overcome the coulombic attraction between the positive surface ions and the electron gas wave at metal surface: (Vrc)min = hujSp.

(4.4)

Similar considerations can be done by replacing the electrolytic solution with a plasma, i.e. in a glow discharge. The two systems are equivalent by considering that AGnid = 0 for plasma. A kinetic term (kT) has to be added to the right term of the above expression accounting for the plasma temperature. This relationship is very well working8 by assuming as theoretical plasmon frequency with the proper electron plasma density for the selected material. The values are shown in Table 1. Table 1. Metal

(n^s)theo

Ag Al Au Be Bi C Ca Cd Co Cr Cs Cu Fe In K Li Mg Mo Na Nb Ni Pb Sn Sr Ta Te Ti Tl V W Zn Zr

6.22 11.17 10.96 12.87 7.63

— 5.65 7.99 13.71 18.45 2.54 10.74 13.5 8.84 3.04 5.58 7.63

— 4.10

— 13.64 9.40 7.21 4.95

— 11.03 12.51 4.87 15.55 16.12 9.47 10.82

(eV)

Plasmons energy for several metals (e£ 0 )theo (eV)

( r ^ s ) e X p (eV)

(e.Eo)exp (eV)

14.44 13.05 17.17 17.39 14.91 22.85 10.30 13.91 16.62 14.17 6.34 15.52 16.20 12.2 7.21 9.83 12.48 17.62 8.65 18.62 16.28 13.27 14.42 9.59 19.69 15.51 14.48 11.64 15.81 20.65 14.67 15.94

17.68 10.82 18.24 14.07 10.39 22.27 6.22 10.75 12.65 17.18 2.33 13.50 11.17 7.99 2.75 5.79 7.49 15.55 4.17 13.79 13.79 9.83 9.97 5.51 13.57 12.65 12.44 6.78 15.27 17.18 12.2 12.87

12.1-13.6 17.2-18.6 13.1-14.8 18.6-19.2 8.4-8.7 15.2-18.9 10.8-11.4 8.6-10.2 16.8-17.7 16.7-17.4 6.2 14.7-15.4 17.1-18.0 9.5-11.9 6.7-7.4 11.1-11.7 11.6-13.0 16.6-17.2 8.7-9.0 19.9-21.6 16.3-17.3 8.8-10.2 10.6-13.0 8.4-9.2 16.8-21.4 11.0-12.4 16.8-17.6 10.5-11.5 17.3-18.0 16.2-22.6 9.8-11.1 17.7-18.5

162

5.

Conclusions

External charges on a surface act as a set of SP: an external triggering, such as a laser beam, could force the electrolytic system to realize the same conditions causing the rise of events perhaps proving the occurrence of L E N R . T h e electrode potentials appropriate to the cathode-electrolyte interfaces (i.e. cathode falls) are related to the interfacial plasmon energies. This picture creates a link between the electrochemical interface structure and the electrodynamics processes occurring at the interface.

References 1. 2. 3. 4. 5. 6. 7. 8. 9.

A.M. Brodskii, Electrokhimiya 22(2), 270 (1986). W.H. Weber and G.W. Ford, Opt. Lett. 6(3), 122-124 (1981). A.K. Sarychev, V.A. Shubin, and V.M. Shalaev, Physics B 279, 87-89 (2000). H. Raether, Surface Plasmons on Smooth and Rough Surfaces and on Gratings (Springer-Verlag, Berlin Heidelberg, 1988). V. Fano, J. Opt. Soc. Am. 3 1 , 213 (1941). A. Otto, Z. Phys. 216, 368 (1968). A.Z. Zangwill, Physics at Surfaces (Cambridge Press, Cambridge, London). A.K. Vijh, Electrode potentials and interface plasmons in the metal/gaseous electrolyte (i.e. plasma) interphasic Region, Mat. Chem. Phys. 14, 47-56 (1986). A.K. Vijh, J. Chem. Phys. 71, 812 (1975).

PRODUCTION METHOD FOR VIOLENT TCB JET PLASMA FROM CAVITY FARZAN AMINI Department

of Mechanical Engineering, Farab Company, Mirhadi St. Vali-e-Asr Ave., Tehran, Iran E-mail: farzanaminiQyahoo. com

No.

30,

The present paper aims at studying transient cavitation bubbles (TCB) jet plasma when such phenomenon like load rejection happens in a hydropower plant; this phenomenon creates a significant cavity at downstream. This process generates abundant tiny bubbles at the micro or nanolevels. The cavity collapses more violently; therefore, higher energy density in the cavity contents is produced. The level of collapsed energy and frequency is controllable by the use of air injection. The load rejection tests at a specific operating regime are utilized to investigate the released energy, which is much more than that of regular TCB experiments.

Nomenclature AQ Cp Cpa Ha Hs Hu K Leq p'v p'L p'0 P Pai Pc PQ Q r rc rv R i?H Re R'0 vc

sectional area of draft t u b e exit pressure coefficient area-mean pressure recovery coefficient atmospheric pressure Suction head vapor pressure polytropic index equivalent length of foot portion saturated vapor pressure at liquid temperature liquid density initial liquid pressure at equilibrium pressure area mean static pressure at inlet section inner pressure of cavity static pressure at the exit of draft tube flow r a t e radial position radius of cavitation rope core radius of Rankine vortex radius of pip wall dimensionless bubble radius Reynolds number initial equilibrium bubble radius cavitation volume 163

164

U' We

characteristic speed for normalization Weber number

Greek symbols F circulation a cavitation number p density 1. Introduction One of our hydropower plants (Masjed - E - Soleyman, Iran) has four Francis turbines. Two units on the right side (looking downstream) share a common penstock and a common long tailrace tunnel, and the other two units on the left also share a penstock and tailrace tunnel. Upon commissioning of one unit, the hydraulic transient in the draft tube during load rejection above 75% was excessive. It was apparent that the guide vane closing law that had been adopted would result in water column separation during load rejection at full power. Tests with a slower closing rate showed that the risk of column separation was reduced, but a violent surge developed in the draft tube close to maximum over speed. The energy level and cavity volume that are produced are much more than those of regular transient cavitation bubbles (TCB) experiments, and therefore, we should expect more intense effects than a regular TCB jet produces. 2. Load Rejection Test When the generator is disconnected from its load, the rotational speed increases due to the hydraulic torque on the turbine. The governor senses the higher speed and causes the turbine distributor to close rapidly to prevent the rotational speed from reaching excessive values. The rapid closure of the distributor causes the spiral case pressure to rise and the draft tube pressure to drop as a result of water hammer effects. The risks during load rejection include: excessive pressure in the penstock; an excessive pressure drop in the draft tube; and an excessive rotational speed inducing shaft vibrations and loss of bearing oil. Water hammer calculations were done to see if better break point and closing rates could be found. They indicated that load rejection at full power could be safe with a slower first closing stroke and a lower break point. Tests with the new settings caused a sharp pressure surge in the draft tube (Fig. 1). This surge propagated to the spiral case and penstock and caused big dynamic loads on the mechanical assemblies of the turbines. It is due to a sudden collapse of the draft tube vortex cavity or to a burst of self-excited instability at the particular unsteady operating conditions of the unit. These unsteady conditions typically occur at around 50% of best efficiency energy coefficient, 30% of best efficiency discharge coefficient, and a low cavitation coefficient.

165

f °lw/

+

1.

%

log of the acoustic wave

bar

— Opening SM

%

—Speed

— Tcbgale

— Draft lube

— Penstock

Figure 1. A severe surge during an emergency shut down. T h e initial conditions of test and results of load rejection are as follows: Initial conditions of test (1) (2) (3) (4) Test

Head water level: 367.7 m. Tail water level: 222.4 m. Opening before G C B off 86.7%. Power before G C B off 250 M W . results

(1) Maximum speed rise: 150.3%. (2) Minimum draft tube pressure: 0.03 bar. (3) Maximum draft tube pressure: 7.01 bar. The measurement equipment in this experiment has a sampling time of 0.01s. Pressure transducers measuring - 1 . 0 to 10 bar located a t the following parts: (a) T w o a t draft t u b e cone. (b) One at draft t u b e exit. (c) One a t head cover. Also one pressure transducer measuring —1.0 to 25.0 bar located at the spiral case. T h e flow in the draft t u b e is complex because the turbine often operates outside

166

-5

0

5

10

15

20

26

30

35

Figure 2. The decreasing of the draft tube pressure peak upon load rejection with the increase air quantity.

its best efficiency point. The first and best-known surging problem is caused by the helical vortex cavity that causes pressure fluctuations in the range of 50-70% of the output at the best efficiency point. The draft tube cavity is filled with water vapor, and air if the turbine has provision for air admission in the center of runner. Air admission was proposed as a method of damping or suppressing the surge, as shown in Fig. 2. The frequency of this partial load pressure fluctuation is often referred to as the "Rheingans frequency," and it is approximately one-third of the rotational speed of machine. The runner and draft tube design as well as operating conditions influence the frequency and amplitude of fluctuations. Currently, available theoretical approaches are not able to model this phenomenon accurately. In turbine model tests with provision for the observation of draft tube flow at the partial load conditions, the cavity is visible at low sigma values (low suction pressure) as a helical void rotating in the same direction as the runner (Fig. 3). For operation at full power, the helical cavity evolves into an axially symmetrical cavity with rotation in the direction opposite to the runner rotation. This may be accompanied by pressure fluctuations and possible auto-excitation. 3. Violent T C B Jet Plasma The TCB jet implant is formed when phenomena like load rejection happens, and it creates a significant cavity that collapses more violently than the stable cavitation bubbles; therefore, higher energy density in the bubble contents is produced. The implanted jet plasma is high-density fluctuating energy plasma, and we expect this energy plasma to increase. The high-density plasma is produced by the plasma jet, which is pinched by the changing magnetic forces that are produced through the high velocity plasma electrons. The TCB "jet" is stabilized by this pinch effect. The jet plasma high-density changing energy contains the deuterons from the dissociated D2O that are implanted in the target lattice, and that remain in place long enough, a few ps, to produce transient fusion conditions before diffusion makes it impossible for the deuterons to fuse. 1 ' 2

167

Figure 3.

Cavity under runner in model test.

4. Cavity M o d e l The natural frequency cavity of draft tube vibrating system with cavitation region is expressed as the following relationship: 3 /s

AQrc 1 2w y pLeqVc

(1)

See the "Nomenclature." All parameters except the cavitation volume Vc in the above equation can be determined. Observation of the cavitation vortex rope in a draft tube indicates that its radius decreases gradually from the inlet to the elbow. In operating condition where a single, cavitation vortex rope is observed, we see the root of the rope usually locates at the center in the inlet section of a draft tube. Thus, the flow field can be regarded as axisymmetric at the inlet. The distribution of circumferential velocity is assumed to be that of the Rankine vortex. Then, the velocity and static pressure distributions are expressed as follows: ® Force vortex region: r c < r < r v . rT

(2)

27rr 25 pT2(r2

rc2)

Pe-

rn

168

Free vortex region: r v < r < R. Vu=^,

P

(4)

2irr'

2 prVi i V pr2(r2v-r c; c) =^ ( +pc 2 ^ 2- ^ ) 2 + ^r;" 42' 8ir V r r / 87r r

(5)

As a representative averaged pressure at the inlet section is required for determining the radius of cavitation rope r c , we use the area-mean pressure recovery coefficient defined as follows:

^-pM

(6)

+ Vv&p

where (7)

TTJ?2'

Vum p W 2 / r2c

P

= ^_,

pY2 ( 1

\

(8) 3

+

f

T

iA

- = ^ M l ^ ~ J "^Ul " 16^ " 4 ^ ]

+P

-

(9)

Substituting Eq. (9) into Eq. (26), and using the following equations: Kl

Ha-Hs-Hv

~

Po P5

ul,2g

(10)

'

h + Ha-Hs.

(11)

We have r4 8r 4

i? 2 r 2 4r 4

/i?2 3 \ Irl 8

1 R\ TZ ( Q I n - - Ki [£-) 2 rv / \TR

+ Cp,

TRJ

+

1 4

0. (12)

In violent bubble collapses, as observed in caviting flows, the bubbles can break up into many smaller fragments. Following the recent work of Brennen, depending on either Reyleigh-Taylor instability or micro-jet formation mechanisms, a simple bubble fission model is introduced to explore the rebound structure after fission and the energy dissipated in the process.4 As mentioned a bubble fission model to describe the rebound structure of the fission fragments, thereby, the energy dissipated due to bubble fission, using a modified Rayleigh-Plesset equation. It is difficult to determine the number of product bubbles that would come out following bubble fission.

iW + fn-Vi + ^ + o f e ^ ' - V i + l'

169

Where Cp =

Vo

(14)

WLU'2

Re = PLU'R'O

(15)

ME

and We =

PLU'2R'O

(16)

According to Eq. (12), during load rejection test, the volume of the cavity is highly dependent on the speed and position of wicket gates, and the rate of change of wicket gate position causes an initial pressure drop for cavity surroundings followed by an increase in that pressure. Therefore, cavity bubbles are affected according to Eq. (13), breaking into smaller fragments. In the transition time, Fig. 1 shows that the energy dissipated due to fission when the number of fission products is large. This process generates many tiny bubbles at the micro or nanolevels, which is one of the characteristics of hydroturbines.

50.00 47.50 6545 00 6 0 42.50 40.00 5537.50 5 0 35.00 4 5 32.50 4 0 30.00 3527.50 25.00 3 0 22.50 2 5 20.00 2 0 17.50 1 515 00 12.50 1 010 00 057.50 005.00 >• % - * - ~ „- *r - - , S&^<J,fiuio< 2.50 -0 50.00 -1 tv ) 5 10 15 20 25 30 35 40 45 50 55 60 65 70 75 80 85 90 •«*• Penstock [bar] — Draftjubel [bar]^Draft„tube2 [bar]™ Speed_U4[%] «~S.M. opening_U4[%] •— Headcover press, [bar] — Flap gate pressure [bar] — Air press, vessel [bar] Air press, a. valve [bar] Deflection [mm]

_"

Figure 4. gates.

_

,_ _

200.0 190.0 180.0 170.0 160.0 150.0 140.0 130.0 120.0 110.0 100.0 90.0 80.0 70.0 60.0 50.0 40.0 30.0 20.0 10.0 0.0

Several examples of TCB jet plasma generation by opening and closing of the wicket

5. Conclusion A helical cavity, which is formed in hydropower plants during load rejection, can collapse, and violent TCB jet plasma can be implanted. It appears possible to

170

simulate these phenomena (load rejection). Its energy is achievable and controllable. T h e level of collapse energy and frequency is controllable by the use of air injection. It is possible to generate T C B jet plasma when the wicket gates open and close several times during load rejection.

Acknowledgment T h e author would like to t h a n k J. Rothwell from LENR-CANR.org for his editorial and technical comments.

References 1. R. Stringham, Cavitation and fusion, in: Tenth International Conference on Cold Fusion (2003). 2. R. Stringham, Pinched cavitation jets and fusion events, in: The Ninth International Conference on Cold Fusion, Condensed Matter Nuclear Science (Tsinghua University Press, Beijing, China, 2002). 3. X. Wang, M. Nishi, and H. Tsukamoto, A simple model for predicting the draft tube surge, in: XVII IAHR Symposium, Section on Hydraulic Machinery and Cavitation, Beijing (1994). 4. M. Tunc and F. Delale, Energy dissipation due to fission of cavitating bubbles, in: Fifth International Symposium on Cavitation (Osaka, Japan, 1-4 November 2003).

N E W RESULTS A N D A N ONGOING EXCESS HEAT CONTROVERSY

L. KOWALSKI Montclair State University, Montcalir, NJ, USA E-mail: kowalskil@mail. montclair. edu G. LUCE AND S. LITTLE EartchTech Inc., Austin, TX, USA E-mail: [email protected] E-mail: UttleQearthtech. org R. SLAUGHTER Advanced Energy Industries, Fort Collins, CL, USA E-mail: rslaughterQcompuserve. com

Mizuno-type cells (glow discharge plasma electrolysis) were used to measure excess heat generated at several potentials between 250 and 650 V. No significant amounts of excess heat were detected. That conclusion contradicts findings of several researchers.

1. I n t r o d u c t i o n This report describes results of two separate experiments, one conducted in the EarthTech laboratory (Austin, T X , USA) and another in the laboratory of Richard Slaughter (Boulder, CL, USA). T h e purpose was to either confirm or refute reality of excess heat in a plasma electrolysis cell. Our experimental setup was similar to t h a t of Fauvarque et al.1 It is a jar with an electrolyte (K2CO3, 0.2 M) containing two electrodes: a cylindrical anode (platinized niobium) and a tungsten cathode (welding rod). A constant difference of potential, for example, 400 V, is applied to electrodes and a glowing layer of gas is formed around the cathode. Three parameters are measured during each test: the electric energy delivered to the cell, E, the amount of heat lost through water evaporation, Q i , and the amount of water lost through conduction and radiation Q2. T h e difference between Q i + Q2 and E, if any, is called excess heat. As in Ref. 1, our experimental results are reported in terms of the coefficients of performance ( C O P ) . T h a t coefficient is simply the ratio (Qi+Q2)/£171

172

2. Experimental Results According to Ref. 1, the COP, at 350V, is approximately 1.35. Our results, 2 ' 3 shown in Table 1, conflict with that conclusion. Table 1.

Coefficients of performance at several voltages

Volts

250

250

300

300

300

355

350

350

400

650

COP

1.00

0.99

0.97

1.00

1.00

1.02

1.03

0.98

1.05

1.05

The first nine results are based on experiments performed in Texas 2 ' 3 , the last result is based on experiments performed in Colorado. 4 The Colorado setup was similar, in principle, to that in Texas except for the power supply (see Appendix 1). An important observation concerning both experiments can be seen in Appendix 2. The Colorado experiment was simply a 21 beaker, mounted on a balance, with two electrodes. Another difference between our two experiments was that the diameter of the anode in Texas was 6 cm while in Colorado it was 3 cm. The range of potential differences in Colorado was from 500 to 700 V. The mean value of COP in that region turned out to be 0.90±0.2. The last value 1.02, shown in Table 1, resulted from eight separate tests. The standard deviation calculated from these tests turned out to be 0.11. It is interesting that foaming and splashing in Colorado was so insignificant that an experiment could be conducted in an open beaker. We believe that this was due to the differences between the power supplies used in two experiments. 3. Discussion Favarque et al. report observing COP's up to 1.4 in their experiments. Similar values were observed by other researchers. Clearly we have not replicated such results. How can this be explained? By experimental errors (measuring E, Qi, and Q2), or by unrecognized, but significant differences in experimental setups. Conditions under which experiments were performed might also have been different. Our anodes, for example, were made from platinized niobium while the anode used in Ref. 1 was made from platinized titanium. Instruments used to measure E were also very different. Accurate measurement of the electrical input power during plasma operation is complicated by the highly erratic current. In Texas, for example, the average current drawn by the cell was 2-3 A but the waveform peaks frequently exceeded 10 A. A sophisticated Clarke-Hess instrument was able to recognize overloads and signal them by flashing. On a less sophisticated instrument such conditions might be overlooked and will lead to underestimation of the average power being delivered to the cell. Overloads were observed during the initial testing; they were eliminated by placing a large filter capacitor between the Clarke-Hess instrument and the cell, as described in Ref. 8. Possible errors in measuring Qx and Q2 are discussed in Ref. 3.

173

Let us mention that appearances of the cathode glow discharge in Texas and in Colorado were quite different. In the first case, we occasionally observed white light flashes coming from large regions inside the cell, in the second only a steady yellow light was seen from a small region surrounding the cathode. Intense white light coming from large regions inside the electrolyte can also be seen on the Internet pictures of similar experiments performed by other researchers. Another difference worth mentioning was the fact that a typical current (for a given voltage) in Texas was about four times higher than in Colorado. The plasma differences between Texas and Colorado experiments were probably due to the arc suppression abilities of the Colorado power supply (see Appendix 1). Why is excess heat observed in some recent experimental s e t u p s 1 ' 5 - 7 and not in others? 8 Are the discrepancies due to experimental errors or to unrecognized, but essential, ingredients present in some setups and absent in others? It is difficult to answer such questions. Scientific disputes are not resolved by voting but a large number of confirmations of excess heat, by qualified researchers in many countries, should not be ignored. The existing controversy would be eliminated if a highly reliable portable excess heat generator could be built. Such generator would then be studied in different laboratories. How else can a consensus be reached? Referring to the issue Jed Rothwell9 wrote: "This is more art than science. Direct, hands-on learning may be the only way to grasp these things; Mizuno himself does not know what is going on in many ways. Building devices on the basis of described protocols does not seem to be sufficient." That is a very good point. A tentatively accepted theoretical model would certainly synchronize our efforts to make sense out of what is going on in the CMNS field. Trying to confirm or to refute claims made by individual researchers is certainly much less effective than testing various aspects of a tentatively accepted model. P.S. ( 1 2 / 2 / 0 5 , by Ludwik Kowalski) Unfortunately, one important detail, about the protocol used by Fauvarque et al, was not specified in Ref. 8. As I learned from Pierre Clauzon (at the ICCF12) the voltage applied to the cell must change gradually, typically in 20 V increments every minute or so. During that time, the cathode was said to be preconditioned to produce excess heat. Clauzon said that they also failed to confirm reality of excess heat without preconditioning. Appendix 1: Power Supply in Colorado Experiment The power supply used in Colorado was Pinnacle. 10 Although the supply was designed for other purposes, it seems to be ideal for glow discharge experiments. Its typical applications include dc sputtering with RF bias, basic magnetron sputtering, cathode-arc deposition (sputter etching and DC-biased RF sputtering). The special features of the Pinnacle are as follows: (1) High line to load efficiency 91%. (2) Power factor >0.9 for loads greater than 1.2 kW.

174

(3) (4) (5) (8) (9)

Quick response to changes in the load. Extremely low-stored energy in the output filter. Fast arc-suppression. Ability to preset joules to be delivered to the load. Provides up to 20 kW of continuous power (we did not exceed 2kW).

The supply provides very accurate power measurements and the ability to control how the power is delivered to the cell. Pinnacle can be used as a source of constant voltage, constant current, or constant power, depending on what is chosen. The other two parameters are then determined by the load. The output voltage, current, or power will hold to within ± 1 % as long as the load impedance stays within the voltage and current limits of the unit. Our tests were performed by using the constant voltage mode, in the voltage range between 400 and 800. The low-stored energy of the output filters of the Pinnacle allows the regulation system of the supply to rapidly respond to changes in the cell impedance. The lowstored energy also prevents the supply from dumping large amounts of energy into the cell as its impedance changes. The low-stored energy is probably one reason that we did not experience the violent reactions in the electrolyte. The other reason was probably the built-in arc suppression. The pinnacle has several methods of arc suppression. The one we used is called "micro-arc suppression." When an arc of less than 10 (is occurs, the stored energy is diverted from the cell and the growing arc is extinguished. The voltage is restored, approximately 5 ^s later. This ability is used in industry to maintain steady even plasma that are required for precise deposition of material on the manufactured product. This arc suppression in combination with the low-stored output energy of the Pinnacle was most likely the reason that we were able to increase the potential difference to over 700 V without the violent reactions in the electrolyte. The arc suppression might also be a reason that our results are different from those reported in Ref. 1. According to Ref. 9, Mizuno says "anyone can generate plasma with hundreds of volts. The trick is to generate it and then gradually reduce input power to the minimum." In one of his papers he writes: "Some researchers have attempted to replicate the phenomenon, but it has been difficult for them to generate large excess heat. They have tended to increase voltage to a very high value, around several hundred volts, but they measured no excess heat." Mizuno also indicates that when the cell begins to produce excess heat the conditions inside the cell are placid. These are the same conditions that we observed in Colorado. We recognize that the cost of the Pinnacle would make it prohibitive for most experimenters. There are, however, less expensive techniques for arc suppression that could be added to power supplies. It is likely that arc suppression will help to minimize the power delivered to the cell, at a given voltage. This might be an important precondition for the generation of excess heat, as indicated by Mizuno.

175

Appendix 2: On Water Condensation Inside Cells A critical reader might notice that Fauvarque et al.1 used an open beaker while the cell used in Texas had a lid on top of it. Can this possibly be a reason for the discrepancy between the outcomes of the experiments? The fraction of steam condensing in a cell with a lid is certainly larger than in a nearly open cell. The rate at which the mass is lost is used in the calculation of COP. Therefore, a critical thinker might say, the difference in the reported values of COP is not surprising. This issue was discussed in Ref. 3. The conclusion was that no significant errors are expected from condensation of water inside the electrolyte, provided the non-evaporative losses are also measured, as in Ref. 1. But that was only a logical conclusion based on certain assumptions. Here is how the conclusion was experimentally validated in Colorado. (a) One liter of water was placed into a 21 beaker standing on a scale, as in Ref. 1. An ohmic heater was used to sustain boiling. The cell had no lid. The mass lost in 350 s was found to be 40.1 g. (b) The cell was then covered with a plastic plate. That plate had eight holes (about 1cm diameter each) plus a hole for the ohmic heater cable. The amount of water lost in 350 s turned out to be 26.1 g. This confirmed the obvious - condensation is enhanced by covering a cell. (c) A pair of plasma experiments was performed - one with a nearly open cell and another with a nearly covered cell. The calculated COP turned out to be 1.00 when the cell was closed (to prevent anticipated splashing that did not materialized) and 1.07 when the cell was essentially open. This pair of tests, by the way, was conducted at 700 V. Pairs of tests at 600 and 550 V also showed that the values of COP are nearly identical and very close to unity. Appendix 3: On Reporting Negative Results After finishing Colorado experiments, one of us (L.K.) called a friend and talked about the discrepancy between our results and results reported by other investigators of plasma electrolysis. This prompted him to write the following message: "I am a retired physics teacher interested in all three CMNS phenomena: CF (cold fusion), CT (cold transmutations), and EE (excess energy). We know that there are two kinds of experimental results: unreliable and reliable. Unreliable data are obtained when experiments are being set up and when we are not yet sure that things work properly. Once the initial difficulties are overcome researchers think that results are reliable. Suppose that reliable experimental data were obtained in 10 experiments. Two of these experiments confirmed the expectations and eight did not confirm them. How should such situation be handled? What should a scientific conference report contain, only two positive results or all results? I know that our natural tendency

176

is to focus on the most interesting new results. But is this appropriate? I do not think so. Negative results should not be confused with unreliable results ..." But the situation is complicated by the fact that some researchers might be hesitant to publish negative results. They might fear that negative statements, taken out of context, can be quoted by pathological skeptics criticizing the field. In our opinion, such fears are not justified; benefits from sharing all reliable results far outweigh negative consequences of self-imposed secrecy. Unscrupulous critics, such as Dr. Richard Park, should not be feared by honest researchers. The issue of publishing negative results goes to the heart of scientific methodology. Here is what Ed Storm wrote about publishing negative results (a private message, 11/19/05): "I would like to throw out some counter thoughts. I think publishing negative results is a waste of time unless these results reveal a useful pattern. For most phenomena, millions of ways are available that will fail to generate the desired results. In contrast, many fewer methods will give the desired results. When isolated negative results are reported, they provide no guidance because they are only a few of so many possible ways to fail. The negative results must be shown to relate to a pattern or a general characteristic. For example in CF, if the H2O content of the electrolyte is too high, the results will be negative over a wide range of concentration. Unless this fact is related to a positive result obtained when the H2O content is low, the observations have little value. My point is that people reporting negative results should be required to show an understanding of their meaning just as people reporting positive results must show what their results mean. However, this does not mean that negative results can be used to deny the possibility of positive results. The two kinds of results have very little relationship to each other until the positive results are well understood, because as I said at the start of these comments, many ways exist for a real result to fail." We do not agree with this. Negative results are worth sharing and discussing. In this report, for example, one of us (R.L.) speculated that our negative results might be associated with the absence of arcing (collecting data when arcing was not too intensive in Texas and suppressing arcing electronically in Clorado). Is it possible that arcing superimposed on the quite glow discharge is an essential component of a device generating excess heat? R.L. plans to answer this question experimentally in the near future. We think that negative results are worth sharing because, like positive results, they guide our attempts to understand what is going on. At one point, two of us (R.L. and L.K.) were discussing the magnificent Naudin's report: http://jlnlabs.imars.com/cfr/html/cfdatas.htm The scatter plot called "efficiency..." shows results from a large number of experiments that were similar to ours. We noticed that in all 22 experiments (performed at 200 V or above) the excess heat was larger than 20% of the input energy. That is a highly significant result; the voltage-dependence trend seems to be consistent with what was reported in Ref. 1. That is how the issue of "publishing positive results only" came about. Negative results were not mentioned. We assumed that

177 the impressive 22 d a t a points represent 100% of reliable experiments. But what if this were not true? We would be much less impressed if these 22 d a t a points represented only 30% of all reliable experiments. Negative results, if any, are important indications of encountered difficulties. P.S. Subsequently Ed wrote: "You may quote me and even use my name. However, your counter argument to my comment missed the point I was making. As I said, "I think publishing negative results is a waste of time unless these results reveal a useful pattern." T h e "useful pattern" is the important aspect of my comment. In your reply, you showed t h a t your negative results were being used to reveal a useful pattern, i.e. t h a t the nature of arcing was a possible important v a r i a b l e . . . During my present study of the F - P effect, I have had many "negative" results. However, I know t h a t certain variables are important and must be controlled. For example, no excess energy is possible unless the D / P d ratio in the surface is very high, which is a difficult condition to achieve. Therefore, I a m investigating the processes t h a t affect this composition. If I report all the negative results without relating t h e m to the important variables, I would be wasting everyone's time. References 1. J. Fauvarque, P. Clauzon, and G. Lalleve, Abnormal excess heat observed during Mizuno-type experiments. Laboratoire d'Electrochimie Industrielle, Conservatoire National des Arts et Metiers: Paris (2005). Available as: (http://www.lenrcanr.org/acrobat/FauvarqueJabnormalex.pdf) 2. See (http://www.earthtech.org/experiments/Inc-W/Fauvarque) 3. See (http://blake.montclair.edu/~kowalskil/cf/2671ittle.html) 4. See (http://blake.montclair.edu/~kowalskil/cf/270slaughter.html) 5. T. Mizuno, D. Chang, F. Sesftel, and Y. Aoki Generation of Heat and Products During Plasma Electrolysis, in Eleventh International Conference on Condensed Matter Nuclear Science, (Marseille, France, 2004). Downloadable from the library at (http://www.lenr-canr.org) 6. D. Cirillo, A. Dattilo, and V. Iorio, Transmutation of metal to low energy in confined plasma in the water (electrochemical plasma cell), in Eleventh International Conference on Condensed Matter Nuclear Science (Marseille, France, 2004). Downloadable from the library at (http://www.lenr-canr.org) 7. Jean-Louis, Naudin et al. Several illustrations and references are downloadable from (http://jlnlabs.imars.com/cfr/index.htm) and from (http://jlnlabs.imars.com/ cfr/html/ cfrtpwr.htm) 8. Scott R. Little, H.E. Puthoff, and Marissa E. Little, Search for excess heat from Pt electrolyte discharge in K2C03-H20 and K2C03-D20 electrolysis. Downloadable from (http://www.earthtech.org/experiments/Inc-W/Mizuno.html) 9. Jed Rothwell, private communication (November, 2005). 10. The Advanced Energy Industry Inc, Fort Collins, Colorado, 80525 (http://www.advanced-energy.com/upload/Pinnacle%20Series%20DC% 20Magnetron%20Power%20Supplies.pdf)

OBSERVATION OF SURFACE D I S T R I B U T I O N OF P R O D U C T S B Y X-RAY FLUORESCENCE S P E C T R O M E T R Y D U R I N G D2 GAS P E R M E A T I O N T H R O U G H Pd COMPLEXES

YASUHIRO IWAMURA, TAKEHIKO ITOH, MITSURU SAKANO, NORIKO YAMAZAKI AND SHIZUMA KURIBAYASHI Advanced

Technology Research Center, Mitsubishi Heavy Industries 1-8-1 Kanazawa-ku, Yokohama 236-8515, Japan E-mail: [email protected]

Ltd.,

YASUKO TERADA Japan Synchrotron

Radiation

Research Institute, Hyogo 679-5148,

1-1-1 Kouto, Japan

Sayo-cho,

Sayo-gun,

T E T S U Y A ISHIKAWA Coherent

X-Ray

Optics Laboratory, Sayo-gun,

RIKEN Harima Institute, Hyogo 679-5148, Japan

1-1-1 Kouto,

Sayo-cho,

In-situ measurement of transmutation of Cs into Pr was performed, and the surface distribution of Pr was investigated using X-ray fluorescence spectrometry (XRF) at SPring-8, a large synchrotron X-ray facility. The in-situ measurement indicated that Pr emerged and Cs decreased at some points after Di gas permeation, though any Pr cannot be observed before Z>2 gas permeation at all the points on the Pd complex surface. Using small size X-ray beam in 100- and 500-fim 2 , we obtained two-dimensional XRF spectra for three permeated samples, from which we detected Pr. Pr was detected again by the two small X-ray beams as expected. The amount of Pr varied greatly at different locations of the Pd surface, however, a clear correlation between surface structures and distribution of Pr has not seen up to now. Experimental results suggest that nuclear transmutations do not occur uniformly but some uncertain factors, presumably condensed matter effects in the present P d / D / C a O system, have a large effect on the rate or the process of the reactions.

1. Introduction Low-energy nuclear transmutations in condensed matter have been observed in Pd complexes which are composed of Pd and CaO thin film and Pd substrate, induced by £>2 gas permeation through Pd multilayer complexes. We already reported transmutation reactions of Cs into Pr, Ba into Sm and Sr into Mo, respectively.1_5 Figure 1 shows schematic of our method. Our experimental method can be characterized by the permeation of D2 gas through the Pd complex and the addition of an element that is specifically targeted to be transmuted. Permeation of deuterium is attained by exposing one side of the Pd complex to D2 gas while maintaining 178

179

the other side under vacuum conditions. On the D 2 gas side of the Pd complex, dissociative absorption causes the D 2 molecules to separate into D atoms, which diffuse through the Pd metal toward the vacuum side, where they emerge from the Pd metal, combine and are released as D 2 gas.

D permeation

^ i ^

^ j ^

^l^

ii

Cs, Ba, etc.

t i I

D flux

I

Vacuum

Figure 1.

/i

i 1

Schematic of our experimental approach.

The second feature is the addition of an element targeted to be transmuted. Our sample is a Pd complex composed of bulk Pd on the bottom, alternating CaO and Pd layers, and a Pd thin film on top. After fabricating a Pd complex, Cs, Ba, Sr, or the other element is deposited on the surface of the top thin Pd layer. We can observe transmutation of the added Cs or Ba. In other words, with this composition, we can provide a deuterium flux through the Pd complex on which a target element is placed as a target to be transmuted. We perform elemental analyses of the given elements after D 2 gas permeation by exhausting the D 2 chamber. In this paper, in-situ measurement of transmutation of Cs into Pr and surface distribution are described. X-ray fluorescence spectrometry at SPring-8 (http://www.spring8.or.Jp/e/) was used for this study. Transmutation reactions of Cs into Pr were confirmed by the in-situ measurement. Surface Pr distribution data were obtained and they showed that the amount of Pr changed greatly depending on the locations of the Pd surface. 2. E x p e r i m e n t a l Fabrication of Pd complex is basically the same as before. 1-5 A Pd was washed with acetone and annealed in vacuum (<10~ 7 torr) at 900°C for 10 h. It was then cooled to room temperature in furnace and washed with aqua regia to remove impurities on the surface of the Pd plate. The surface of the plate was covered by layers of CaO and Pd, which were obtained by five times alternatingly sputtering 20 A thick CaO and 200 A thick Pd layers. Then a 400 A thick Pd layer was sputtered on the surface of the CaO and Pd layers. These processes are performed by Ar ion beam sputtering method or magnetron sputtering method. After forming a Pd complex, Cs was deposited on the surface of the thin Pd layer. Cs was deposited by electrochemical method or ion implantation method.

180

D2 gas inlet

Figure 2.

Experimental setup for in-situ measurement.

Figure 2 shows the experimental setup for in-situ measurement. Synchrotron orbital radiation X-ray (5.97 keV) is introduced into the permeation chamber through a Be window and attacks on the surface of Pd complex sample. X-ray intensity is about from 1012 to 10 13 photons/s. Cs-L and Pr-L lines can be detected by a Silicon Drift Detector (SDD). The SDD is covered by a CI filter for suppression of Pd-L X-ray. We made D2 gas permeated through a Pd complex with Cs for 10-14 days. D2 gas pressure is about 170 kPa and the temperature was 70°C. X-ray fluorescence spectrometry was performed during D2 permeation in-situ at the beginning and the end of experiments. Surface distribution of Cs and Pr can be measured by the experimental setup shown in Fig. 3. The synchrotron radiation X-ray is divided by slits and we get rectangular micro X-ray beam. In this study, we use 500 and 100 /im beams. The Pd complex sample is attached on an X-Y stage that can be moved by stepping motors, two-dimensional XRF spectra can be obtained by this setup. Surface images can be taken by a microscope that is equipped for this two-dimensional XRF spectrum analysis. We can obtain the information about correlation between distribution of elements and surface images. 3. Results and Discussion First of all, we describe the results of in-situ measurement; sample name is SP24. Initial (before D2 gas permeation) and final (after D2 gas permeation) XRF spectra are drawn in Fig. 4. Cs was deposited by the ion beam implantation method

snt _

^

si. _ _

a**. ^

z

^ ^ ^ B w | i samp,e

^

i

H

X^ray fluorescence £ M

f ^

**"•"•**"-•- ^ S L „ mam Figure 3.

^

^ & £

^

l

m

Si**"

iST"

Experimental setup for the measurement of surface distribution of Cs and Pr.

181

Energy (keV)

Figure 4. Confirmation of transmutation of Cs into Pr using ion beam implanted sample (SP-24) by in-situ measurement.

(voltage: 5kV, dose: 2.5 x 10 1 4 /cm 2 ). In this case, we use 1mm 2 X-ray beam. As shown here, Cs peaks decreases and Pr peak emerge after D2 gas permeation at the shown point. It can be seen that transmutation of Cs into Pr occurred at this point. However, no Cs was changed and no Pr was seen except this point in the case of SP-24. Another example of in-situ measurement is shown in Fig. 5. Electrochemical deposition 1 was applied to this sample (SP-33). Pr was detected at points 2, 3, 8, and 9, although no Pr was detected at the points 4-6, 10-12. We could not see initial Cs at the points 1, 7, 13-15 because Cs distribution is not uniform if we applied electrochemical Cs deposition method. Initial and final XRF spectra at point 2 are shown in Fig. 2. Cs peaks decreased and a Pr peak emerged after D2 gas permeation. The ratio of minor peak of Cs-L to major peak of Cs-L is always constant, so we can judge that the peak near 5keV is attributed to Pr-L X-ray. This result also demonstrates that transmutation reaction of Cs into Pr occurs in this experimental system. Let us move on to the next point. Figure 6 shows Pr detection by XRF method performed in 2003. FG1 was fabricated by the Ar ion beam sputtering method and permeated for 97 h by D2 gas at 70°C. FG2 was made by the magnetron sputtering method and permeated for 96 h by D2 gas at 70°C. Pr-L lines were clearly in both foreground samples, while no Pr peak could be seen in the background sample. Pr surface distribution measurements were done for FG1, FG2, and SP-24 by small size X-ray beams in 100 and 500jum2.

182

/f6j&&

;.• 500

CO

co

400

Q.

CO

"5 CNJ

300

ar,

200

1 1 1 ) 1

I I

Distribution of Pr

_ : ,.., | | , | , | , , | |

A

Initial /

C S x

- j /

A f\

i

O

100 -

0 3.

11

10

6

5

4

3

2

1

9

8

7

15

14

13

2,3,9,8: Pr detected 4-6,10-12: No Pr 1,7,13-15: No initial Cs

c O

12

Final i

4.2

4.4

4.6

4.8

5.2

5.4

Energy (keV) Figure 5. Confirmation of transmutation of Cs into Pr using electrochemically deposited sample (SP-33) by in-situ measurement.

Mapping data of Pr for FGl analyzed by 500 fjm X-ray beam is shown in Fig. 7(a). Pr could be detected from all the points (400 points) in the analyzed region in 10 mm x 10 mm. Detection of Pr is consistent with the above XRF measurement in 2003. In addition to Pr, we detected the other peaks for 27 points. A peak around 4.5 keV can be seen at point 284. Levels of Pr seem to be almost uniform for these points. We can estimate that these peaks correspond to about 5 x 10 13 atoms/cm 2 by the comparison with XRF spectra using a reference sample

2

3

4

X-ray energy (keV) Figure 6. Detection of Pr by XRF in 2003 (FGl and FG2; D 2 permeated samples, BG; No permeated sample).

183

F^

£0

3 22 3 !4 ?7 •

Za

^ 4

At*

TO S i J-

2 ££644 &$7%2

S

x^

** 7? il

K

!••

1

44

•^TO

w ;^ 55 ,; iZ* i44r4

"5

« £5

s

^ 7 W<,

4^

9?

T^1

Eg! r ?

i! 2*

u0

^77 SW gfgfs * s A

^

44 ^?

K?

1

44

S^J v^? ^4v * ? ; « # 44 ^y.

•:;•-•

^

v4

rr

4*4 1 2 i

K*3

5fc

^

llj_i L j i

?a •;«v

A;

15 i 14*

TO

4 ^ 7 TO? TO

S-'

ijl

10 mm

fz

1 TO

4< £ L U C-iLi *-*!

10 mm V///I

Detection of Pr only; 373 points (93%)

l:-'-^l Deleclion ol Pr and unidentified element; 27 points (7%)

(a)

Energy (keV)

(b) Figure 7. Surface distribution of Pr for F G l using 500 (im X-ray beam; (a) Mapping of Pr and unidentified element, (b) X R F spectra for the points 281-285, (c) surface image of F G l for the points 282-286.

in which Pr was already implanted. Figure 7(c) shows corresponding surface image taken by a microscope. It seems that there are no specific or special features for the point. 284 under this measurement condition. Mapping data of Pr for FG2 analyzed by 500 fim X-ray beam is shown in Fig. 8(a) P r was observed at 61% points (74 points) in the analyzed region in 5.5 mmx 5.5 mm. Detection of Pr is consistent with the 2003 XRF measurement shown Fig. 6. In this case, we could not see any "unidentified peaks" shown in Fig. 7 (FGl). No Pr was

184

5.5 mm

108 107 106

105

120 119 118 117

^WMmmm.'M 5 aasa S I I

132 131 130

129 128 127 126

144 143 142

141 140 139 138 137

125

124

123

122

136 135 134

5.5 mm

Detection of Pr only; 74 points (61%) I

I No detection 47 points (39%)

Figure 8. Surface Distribution of Pr for FG2 using 500 /fin and 100 /im X-ray beams, mapping of Pr by 500 /un beam.

detected in 39% of the points. XRF spectra for points 75-79 by 500 /an beam are shown in Fig. 9(a). The strengths of Pr seem to be slightly changed depending on measured points, however, no clear difference seems to be seen as shown in Fig. 9(b). XRF spectra using 100 /im beam for the point 27 are illustrated in Fig. 9(c) and the surface image for the corresponding region is shown in Fig. 9(d). The "unidentified peak" emerged at the point 5-1 in the point 27, although we could not observe the "unidentified peak" if we used a 500 /an beam. This fact suggests that the "unidentified" element was so localized and so small that the signal from the element was buried when we used large beam (500/an). It also seems there are specific or special features for the point 5-1; or if there are specific structures, they might be much smaller than this image. Based on the XRF spectra, La, Ba, and Ti are candidates for the unidentified peak. At the present stage, we cannot completely exclude the possibility that the peak is derived from a localized impurity. Further investigation by other measurement methods is necessary. Sample SP-24, originally measured in-situ, was analyzed by small size X-ray beams in 100 and 500/an 2 5 months after the permeation experiment. Pr could be observed again in the same region as the in-situ measurement. The surface distribution of Pr for SP-24 by 500 /an X-ray beam is shown in Fig. 9(a). Pr was observed only at six points and the "unidentified" peak was observed at two points even though we used 500 /an X-ray beam. As for SP-24, reaction rate is lower than FGl and FG2. At present, the authors cannot explain completely the difference of

185

Energy (keV)

(a)

77

(b)

Energy (keV)

(c)

(d)

Figure 9. Surface Distribution of P r for FG2 using 500/im and 100 /im X-ray beams, continued: (a) X R F spectra for the points 75-79 by 500 pm beam, (b) surface image of FG2 for points 75-77, (c) X R F spectra using 100 /ini beam for the point 27, (d) surface image of FG2 for the point 27.

reaction rates between these three samples. It should be investigated further, since clarifying the factors that make influence on the transmutation rate is an important and valuable task to increase transmutation rate. Figure 9(b) and (c) shows surface distribution of Pr and XRF spectra obtained by 100/an X-ray beam for point 13-4 shown in Fig. 9(a). The amount of Pr changed greatly depending on the locations of the Pd surface. Pr is localized at the specific points shown in Fig. 9(c). Surface image for the corresponding region is shown in Fig. 9(d). No clear correlation between the localized Pr and surface image could be observed. These experimental results suggests that transmutation reaction rate varies depend on the Pd surface region. And if we postulate that the unidentified peak is derived from a transmuted element, transmutation pass might be changed depend-

186 ^ i

» i

,.,

«

M " V

;.L;: ...,

"

•

>

-

_

.-o ta

Ml

0

Detection ot Pr only; 6 points (3%)

£]

Detection of Pr and unidentified element; 2 points (1%)

•

No detection; 192 points (

(a)

X

1

2

4

3

e

5

13 -4

1 2

- P0nl 4-4 (nxW>Pr«>toe«on) -PWnt»4(Pr<M0ctkxi) -Pcfet*4(NoPr)

3 4 100 nm

5 6 100 |im

I

Much Pr detection Pr detection

] NoPr

4

4.5 Energy (KeV>

(b) (c)

(d) Figure 10. Surface Distribution of Pr for SP-24 using 500/im and 100 /mi X-ray beams, (a) mapping of P r by 500 jim beam, (b) mapping of P r by 100 /im beam a t point 13-4, (c) X R F spectra depending on location obtained by 100 mn beam, (d) Surface image of SP-24 corresponding to X R F spectra.

ing on location. Some uncertain factors, presumably relating to condensed matter effects in the present Pd/D/CaO system, must make a lot of effects on the rate or the process of the reactions. In order to make clear the uncertain factors, it would be necessary to use smaller X-ray beam, although it would take much more time for XRF measurement. 4. Concluding R e m a r k s One of our experimental apparatus was carried to SPring-8 for the purpose of in-situ measurement and we obtained clear Pr signals after D2 gas permeation by the X-ray fluorescence method. According to the micro X-ray beam measurement, we noticed that Pr was localized greatly. At present, the correlation between products and the surface structures is not clear. Further investigations are necessary, for example, using smaller X-ray beam or analyzing these samples by the other methods.

187

Acknowledgments T h e authors would like to acknowledge Professor A. Takahashi, Professor J. Kasagi, Professor T. Okano, Professor K. Fukutani, Dr. F . Clelani, Dr. K. Grabowski, Professor M. Melich, Dr. C. Catalina, Dr. C. Carmine, Professor K. Okuno, Dr. Z. Yoshida, Dr. Y. Nagame and Professor S. Iio for their valuable discussions. T h e authors also acknowledge for the support of T E E T (The T h e r m a l and Electric Energy Technology Foundation). X R F experiments in this work were performed at the BL37XU in the SPring-8 with the approval of the J a p a n Synchrotron Radiation Research Institute (JASRI) (Grant No. 2004B0456-NXb-np, 2005A0250-NXb-np, 2005 A0409-NXb-np-Na).

References 1. Y. Iwamura, M. Sakano and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4648 (2002). 2. Y. Iwamura, T. Itoh, M. Sakano, S.Kuribayashi, Y. Terada, T. Ishikawa and J.Kasagi, Proc. ICCF11, Marseilles, France, Oct. 31—Nov. 5 (2004), World Scientific, Singapore, pp. 339-350. 3. Y. Iwamura, T. Itoh, M. Sakano, S. Sakai and S. Kuribayashi,. Proc. ICCF10, Cambridge, USA, 24—29 August (2003), World Scientific, Singapore, pp. 435-446. 4. Y. Iwamura, T. Itoh, M. Sakano and S. Sakai, Proc. ICCF9, Beijing, China, 19-24 May (2002), pp. 141-146. 5. Y. Iwamura, T. Itoh and M. Sakano, Proc. ICCF8, 21—26 May (200 ) Lerici, Italy, SIF Conf. Proc. 70, 141-146.

D I S C H A R G E E X P E R I M E N T USING P d / C a O / P d MULTI-LAYERED CATHODE

S. N A R I T A , H. Y A M A D A , D . T A K A H A S H I , Y . W A G A T S U M A , S. T A N I G U C H I A N D M. I T A G A K I Department

of Electrical

and Electronic Engineering, Iwate Morioka, Iwate 0208551, Japan E-mail: narita@iwate-u. ac.jp

University,

J^-3-5 Ueda,

We performed the discharge experiment in deuterium gas atmosphere using cathode with multi-layered structure of P d / C a O / P d , and P d / C a O complexes on which Cs was deposited, and the possibility that the transmutation of Cs to Pr just as being observed in the recent permeation experiment was investigated. In this study, we have not seen the clear evidence for Pr production. There are still problems in the characteristics of discharge method to induce the reaction significantly. In addition to the study of such specified transmutation process, we surveyed all the elements qualitatively and check newly produced elements as well as anomaly in the isotopic abundance for the elements detected, and found some candidates of isotopes supposed to be produced during the experiment.

1. Introduction For the study of low-energy nuclear reaction in condensed matter, the discharge method is thought to be one of the effective ones and the advantages have been shown by several researchers. We have performed discharge experiment exposing Pd or Pd deuteride in high-purity deuterium gas changing the experimental conditions; the pressure of deuterium in the chamber, electrode shape, duration time and so on. In such experiments, we have demonstrated that anomalous gamma radiation with energy around ^100 keV, and it was suggested that some short-lived radioisotopes were produced. 1 However, the reproducibility of the phenomena was quite low and we have not specified the origin of the radiations. Besides the discharge experiment, there is a well-established technique for lowenergy transmutation study, that is, deuterium permeation method using multilayered Pd/CaO complex sample. In the method, the transmutation from Cs to Pr, Sr to Mo, and Ba to Sm was observed with good reproducibility. 2 ' 3 Although the reaction mechanism has not been clarified theoretically, it has been claimed that sufficient D flux in the permeation through the sample and Pd/CaO multilayered structure of the sample, especially for existing CaO layer, are necessary for triggering the phenomenon in the method. In this study, considering those experimental results, we performed discharge experiment in deuterium gas using Pd/CaO multi-layered cathode on which Cs 188

189

is deposited and searched for peculiar phenomena, which suggests that occurring nuclear reactions especially for Pr production by the transmutation from Cs, just as observing in the permeation experiment. In addition, we investigated the possibility of other element production and the isotopic abundance of the elements detected can be an evidence of nuclear reaction. According to recent reports, laser irradiation to hydrated/deuterated metal sample is supposed to initiate and/or amplify the nuclear effect in condensed matter, even the power is just a few 10 mW. 4 , 5 Then, we also tested the effect of irradiating the laser light to the cathode sample during discharge in this experiment. 2. Experiment We tested two sets of experimental conditions. One is the so-called our conventional glow discharge under low-deuterium pressure with foil type anode. The other set is corona discharge (partially breakdown discharge). This is under higher pressure with needle type anode. The energy of deuterium ions irradiated to the cathode is supposed be lower than that in glow discharge. In terms of the motion of D ions on the sample surface, this condition is thought to be more similar to permeation's. We used two different types of samples for each experimental condition. One is the sample with Pd and CaO thin layers on Pd substrate (type-1). The other is five alternate thin layers of Pd and CaO on the Pd substrate (type-2), which has the same structure as that used in the permeation experiment by Iwamura et al.2 These types 1 and 2 samples were used for the glow discharge experiment and the corona discharge experiment, respectively. The sample was prepared in the following procedure. The Pd foil (12.5 x 12.5 x 0.1mm 3 ) was washed with acetone and aqua regia. For type-1 sample, 10 nm CaO and 40 nm Pd layers were formed on the Pd foil by Ar ion beam sputtering. For type-2 sample, 2 nm CaO and 20 nm Pd layers formed alternately on Pd substrate by sputtering, and there are five sets of layers. The fifth, most surface, Pd layer was made thicker, it was 40 nm. On sputtering, the thickness of CaO and Pd layers was adjusted by sputtering time. After making thin layers, Cs was deposited onto the sample by electrolysis. In the electrolysis, the plastic cell was used and the sample was set as cathode and the anode was platinum foil. The electrolyte was a few mM CS2CO3. The applied voltage was 1V and the electrolysis time was several 10 s. After sample preparation, it was placed in the discharge cell as the cathode. The discharge cell is shown in Fig. 1. The cell made of Pyrex glass has a spherical shape with a volume of ~ 1500cm 3 . The thickness of the glass is 5 mm. The cell is connected to a vacuum system through the port so that we can drive out the gaseous impurities in the cell and control the pressure inside the vessel. Au foil (0.1mm in thickness) or Pd needle (0.2 mm in diameter) was used as anode. The former was used for glow discharge experiment, and the latter was used for corona discharge. Under the discharge, it is possible that the elements on the cathode surface are diffused by sputtering, so that small amount of elements produced by the nuclear

190

Valve

Figure 1.

Discharge cell.

reactions (if it happens) can be flown away. In order to detect such elements, a high-pure Au foil (5 x 10 x 0.1 mm 3 ) was placed 2 cm away from the cathode. One of the surfaces of each foil faced to the cathode to receive the elements sputtered. The Au foil is called "Au side-foil" hereafter. After the discharge, the cathode sample was taken out from the cell and the elemental composition was analyzed by the inductively coupled plasma mass spectrometry (ICP-MS) and atomic emission spectrometry (ICP-AES). These are used for measuring Cs and Pr density and also detected the elements contained as well. The sensitivity of ICP-MS is so high that it can detect the element with density above 0.1 ppb. The ICP-AES is less sensitive and it was mainly used for checking the elements detected by ICP-MS in qualitative analysis. In pre-processing ICPMS and ICP-AES, the multi-layered cathode sample was immersed in 1 cm 3 of ultra pure nitric acid for 30 s, and the elements on/in the sample were dissolved in it. Then it was diluted by adding pure water to be totally 50 cm 3 . This sample solution was analyzed by ICP-MS and ICP-AES. We evaluated the quantity of each element by the density of the elements measured in this solution In addition, the surface composition of Au side-foil was analyzed by time-offlight secondary ion mass spectroscopy (TOF-SIMS). In this analysis, we checked Pr signal and any other elements detected by ICP-MS and ICP-AES. TOF-SIMS is capable of analyzing all the elements including their isotopes, then, we surveyed over all elements and investigated the anomaly in the isotopic abundance. Also, we analyzed the reference sample which was prepared by the same process as the

191

standard sample was but not exposed to the discharge. Comparing the elemental composition of those two samples, we specified the candidates of products by nuclear reaction. For testing the effect by laser irradiation, we utilized semiconductor laser (690 nm in wave length and ~20mW in output power), and we investigated the difference in the phenomena for runs with or without laser irradiation. Table 1 shows the summary of run conditions. Four types of conditions were tested in this study. The run Nos. 1 and 2 were for glow discharge condition, and run Nos. 3 and 4 were for corona discharge condition. Table 1.

Experimental conditions

Run No.

Cathode

Anode

D2 pressure

Voltage

Current

Time (h)

Laser

1 2

Type-1

Au foil

lTorr

400—600 V

~lmA

~170 ~170

On Off

3 4

Type-2

Pd wire

1 atm

~10,000V

~4mA

~70 ~70

On Off

We now consider the D fluence to the cathode during the discharge. In permeation experiment, it is thought to determine the conversion rate of Cs to Pr transmutation, and a sufficient deuterium flux is an important factor to obtain a significant yield. Here, we assume that the current is determined mainly by D ions and the discharge area on the sample is ~ 1 cm 2 , about 1022 D ions are irradiated to the cathode during the discharge. From the results of the permeation experiment, Iwamura et al. have estimated the cross-section of transmutation of Cs to Pr and its conversion rate assuming the deuterium flux permeation through the sample being equivalent to deuterium beam irradiation. 6 They found that the conversion rate is proportional to average flow rate and they obtained ~0.3 for irradiating ^ 3 x 10 23 deuterium atoms. Considering our experimental conditions (Table 1), roughly speaking, the fluence estimated in our case is comparable value which gives ~10% conversion rate of Cs to Pr in permeation experiment. By ICP-MS analysis for the reference sample, the Cs concentration on the sample was measured to be 10-100 ppb (it cannot controlled uniformly in the current method and varied run by run), then we may expect the Pr density in the same analysis 1-10ppb. 3. Results and Discussion 3.1. Transmutation

of Cs to Pr

Table 2 shows Cs and Pr density measured by ICP-MS for each run. No Pr signal was found for every run. Also the Cs signal is nothing either or very small. It might be due to the sputtering effect in the discharge. The effect is apparent in glow discharge condition. No Pr signal was found in ICP-AES results, and this was expected because the Pr density should be below its sensitivity, considering the

192

initial density of the Cs on the sample and the conversion rate estimated from the D fluence. Table 2.

Cs and Pr density analyzed by ICP-MS

Run No.

Condition

Laser

Cs (ppb)

Pr (ppb)

1 2

Glow discharge

Off On

N/D N/D

N/D N/D

3 4

Corona discharge

Off On

2.5 15.4

N/D N/D

The Au side-foils were analyzed by TOF-SIMS. Figure 2 shows the spectra of the mass around Cs and Pr for the Au side-foil used in glow discharge experiment. The top figure is for laser-off run (run No. 1) and the bottom one is for laser-on (run No. 2). In both spectra, no clear signal on mass 141 corresponding to Pr mass was found. There are peaks of Cs on mass 133 and it is supposed to be diffused from the cathode sample. As mentioned above, the concentration of deposited Cs was not uniform. This must be a main reason why the intensity of Cs was different in these figures. The peaks on the each nominal mass were thought to be the signal of fragmentation of molecular ions. Figure 3 shows the mass spectrum for the Au side-foil used for corona discharge with and without laser irradiation. No Pr signal was found either. There is a peak around mass 141 in the bottom figure, but the mean value of the peak is far from true Pr mass. We did not observe Pr signal for every experimental condition (discharge type, sample structure, and laser irradiation). One of the possible reasons was that the Pr yield was quite few because D fluence and/or Cs concentration were insufficient. In order to enhance the D fluence, we should consider modifying the system so that we can supply much higher current. In the current method, we cannot control the Cs concentration on the sample. We should also modify the method in the Cs deposition. Moreover, the sputtering effect in the discharge seems to be a serious problem, so the changing sample structure and its layout should be modified. 3.2. Possible

Transmutation

Products

Table 3 shows the corresponding elements to the signals found in qualitative analysis by ICP-MS and ICP-AES. In this table, only the elements, which are not detected in the reference sample are listed. Some candidates as transmutation products were found in corona discharge experiments (runs 3 and 4). For the experiment without laser irradiation, candidates of Ga, Ag, Sn, and Ba were found in IPC-MS and Te was found in ICP-AES. Since the sensitivity of ICP-MS is much better than that of ICP-AES, Te signal might appear also in ICP-MS analysis if it really existed. However, it can happen that really existing element is only found in less sensitive device due to the characteristics of analyzing devices. So, it is kept in the list as possible product here. For laser-on run, Ga, Ag, Sn, I, and Ba were found.

193

T a b l e 3 . C o r r e s p o n d i n g e l e m e n t s for t h e signals d e t e c t e d b y I C P - M S or ICP-AES Corresponding element Run No.

Condition

Laser

1 2

Glow discharge

Off On

3 4

Corona discharge

Off On

ICP-MS

ICP-AES

Ga, Ag, Sn, Ba Ga, Ag, Sn, I, Ba

Te —

We now checked if these elements are found on the Au side-foil by TOF-SIMS. In this analysis, Ga cannot be checked because G a + ion is used as primary ion in TOF-SIMS. For laser-off run, isotopes of Ag ( 107 Ag and 109 Ag), Sn ( 112 Sn, 116 Sn, 117 Sn, 118 Sn, and 119 Sn), Te ( 120 Te and 130 Te), and Ba ( 130 Ba and 132 Ba) were identified. Ag isotopes were detected with natural abundance, and it is possible that these signals are overlapping of 106 PdH and 108 PdH compounds. For S, Te, and Ba isotopes, the abundance is quite different from natural ones. Then, for laser-on run, Ag ( 107 Ag and 109 Ag) was found with natural abundance and S ( 112 Sn, 116 Sn, and 118 Sn) and Ba ( 130 Ba, 134 Ba, 135 Ba, 136 Ba, and 138 Ba) were found with anomalous abundance. The signal of Iodine was not detected. Although we observed '

•

•

•

7500

£

5000

2500

1 1... i... i...i. ,.L..L ,..l.

a

0 132 133 134 135 136 137 138 139 140 141 142 •

:

;

i

.

i

| . U .

:

"

'

, . I . . | M

• • | 1

, , ..

Counts

400

200

1.

.,,,. » , : . , « I : » n 1 132 133 134 135 136 137 138 139 140 141 142 i -

<

i

,

Mass F i g u r e 2. M a s s s p e c t r u m m e a s u r e d b y T O F - S I M S for A u side-foil u s e d in glow d i s c h a r g e e x p e r i m e n t . Laser-Off ( T o p ) a n d L a s e r - O n ( B o t t o m ) .

194

1000

tn

§

500

j...li..,|j...ll,,.ll..i J.... 0 d. I . M U 132 133 134 135 136 137 138 139 140 141 142 -i i i i | u i i | M i t 11 n i 11 i n j i M \ 1 i u i 11 n i 11 i 11 11 111-

4000

2000

0.

J I

it, . I.

LL ,i

l.i , J

JT

J

132 133 134 135 136 137 138 139 140 141 142 Mass Figure 3. Mass spectrum measured by TOF-SIMS for Au side-foil used in corona discharge experiment.

anomaly in abundance for some isotopes, the signal with large mass number can be affected by the fragmentation of molecular ions. Therefore, we should still consider the possibility of miss-identified and miss-counted of the signal corresponding. We cannot give a conclusion only with the current information, and further study is necessary. 4. Summary We performed the discharge experiment under two different types of condition, i.e. the glow discharge and the corona discharge, with multi-layered Pd/CaO cathode to investigate the nuclear transmutation. Depositing Cs to the multi-layered cathode, we tried to induce transmutation of Cs to Pr just as observing in permeation experiment, but we did not see the evidence of Pr production with some analysis methods. Some problems in the experimental conditions still remain, and those should be solved in the next step. The possibility of production of some elements was shown in the corona discharge experiment. Further study to identify such candidates correctly by various methods, are necessary. Irradiating the laser to the deuterated metal is interesting idea in terms of improving the efficiency for the low-energy nuclear reaction in condensed matter. We made the first trial to investigate the effect irradiating the semiconductor laser to the cathode sample in the discharge experiment, and we could not obtain any symptom showing the effect in this study.

195 We will continue to investigate the possibility of inducing a selective transmutation by discharge method and also t r y to obtain the evidence of nuclear reaction in this method. These results may help clarify the low energy nuclear reaction in condensed matter.

References 1. S. Narita et al, Proc. JCF5 (2004) pp. 14-18. 2. Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4650 (2002). 3. Y. Iwamura, T. Itoh, M. Sakano, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi, Proc. ICCF11 (Marseilles, France, 2004). 4. D. Letts, Proc. ICCF10 (Cambridge, USA, 2003). 5. V. Violante, Proc. ICCF11 (Marseilles, France, 2004). 6. Y. Iwamura et al, Proc JCF5 (2004) pp. 60-64.

P R O D U C I N G T R A N S M U T A T I O N E L E M E N T ON MULTI-LAYERED Pd SAMPLE B Y D E U T E R I U M P E R M E A T I O N

H. Y A M A D A , S. N A R I T A , S. T A N I G U C H I , T . U S H I R O Z A W A , S. K U R I H A R A , M. H I G A S H I Z A W A , H. SAWADA A N D M. I T A G A K I Department

of Electrical

and Electric Engineering, Iwate University, Morioka 020-8551, Japan E-mail: yamadahi@iwate-u. ac.jp

Ueda

4-3-5,

T. ODASHIMA Department

of Chemical

Engineering, Ichinoseki National Takanashi, Ichinoseki 021-8511,

College of Technology, Japan

Hagiso,

Time-of-flight secondary ion mass spectroscopy (TOF-SIMS) was employed for elemental analysis of surface of multi-layered palladium sample with small amount of cesium. Substances with mass number 135 and 137 were newly detected by TOF-SIMS after deuterium permeation at 70°C. The result suggests production of an element with mass number 137 which would be produced from cesium by same low-energy nuclear reaction.

1. Introduction The phenomena on nuclear reactions at low temperature in solid-state have been widely investigated for these 17years. Among several experimental methods for the reaction, the gas permeation method is one of the promising methods. Iwamura et al.1 have studied using this method with Pd film complexes, which consist of Pd layers, CaO layers and a bulk Pd. They have reported a low-energy nuclear reaction such as the transmutation of Cs into Pr in deuterium permeation experiment and have recently found a certain rule of nuclear transmutation, that is, 8 mass number and 4 atomic number increase in the process. The phenomenon has been observed with good reproducibility. While, we have been taking account of the possibility of nuclear transmutation not only in such Pd film complexes but also in plain Pd foil by hydrogen gas permeation at room temperature. We have performed an elemental analysis on the Pd foil and have reported increases in count intensity of several elements including Ag after hydrogen permeation. 2 The count intensity of Fe has been sometimes observed to increase significantly after the permeation of highly pressurized hydrogen gas through Pd samples of 0.1 and 0.3 mm thickness. This result would show a pressure effect on the reaction of transmutation. Furthermore, the isotopic composition of Ti and Cr has been observed to differ from the natural isotopic abundance of those elements. These results have suggested that several elements were produced 196

197

by a nuclear transmutation and that the reaction could occur in hydrogen system as some researchers have claimed in various experiments. 3-5 The aforementioned results suggest that there is a key to understand the reaction in terms of the mobility of proton or deuteron in Pd lattice. These reports caused us to study the phenomena systematically by the permeation experiment for deuterium as well as hydrogen using multi-layered Pd samples. Thus, in this present investigation, we have performed a deuterium permeation experiment using Pd samples6 including a multi-layered sample consisting of single couple of CaO and Pd thin films and a bulk Pd foil. On the basis of the reports on transmutation of 133 Cs into 141 Pr, production of elements with mass number ranging between 133 and 141 could be expected before Pr production. Therefore, we have focused our attention to this mass number range to search for the producing elements as a result of low-energy nuclear reaction. The amount of newly producing elements in this range would be so little; it is desirable to employ an instrument having a good sensitivity for a very small quantity of the elements on the sample with high resolution in mass number. Consequently, we have performed the element analysis using time-of-flight secondary ion mass spectroscopy (TOF-SIMS). 2. Experimental A base Pd foil (99.95% pure) of 0.1 x 12.5 x 12.5mm 3 in size was rinsed with acetone and pure water, and then washed by aqua regia to remove impurities on the Pd foil surface. Next, the Pd was annealed at 900°C for 8h, followed by being cooled to room temperature in furnace and washed again with aqua regia. Using the base Pd foil, we prepared three types of samples. The first one was a plain Pd sample just as the base Pd foil was. It had no deposition of any additional elements. The second one had small amount of Cs deposited on the base Pd foil. The last one had small amount of Cs on the uppermost of multi-layered Pd sample. The multilayered sample consisted of a couple of CaO and Pd thin films on the base Pd foil. The CaO and Pd thin films were formed on the Pd foil by Ar ion beam sputtering under the input energy of 30 W for 5min and 20 W for 1 min, respectively. After forming the thin films, small amount of Cs was deposited on the multi-layered Pd sample by an electrochemical method. In this method, the Cs was deposited by applying an electric field to 0.5mM CS2CO3 solution; a I V negative voltage was applied to the multi-layered Pd sample for 10 s. A Pt foil of 10 x 10 mm 2 in size was utilized as a counter-electrode. The thickness of CaO and Pd films formed were 2 and 40 nm, respectively. No deuterium gas was loaded to the samples before deuterium permeation experiment. Figure 1 shows the deuterium permeation system to investigate the transmutation of Cs into other elements of lager mass number. Whole the permeation system was constructed at Ulvac Techno, Ltd. in Japan. The surface inside of chamber was finished by electro polishing method to reduce amount of impurity molecules deposited on the surface as low as possible. A stainless steel sample holder for

198

N 2 gas

/T^ZHX}

Figure 1.

Apparatus for cold transmutation.

the deuterium permeation system is shown in Fig. 2. The vacuum chamber and the sample holder were baked at 200°C sufficiently before setting the sample. The chamber is usually filled with N2 gas under non-experiment condition. Just before the permeation experiment, the Pd samples were set into the sample holder in an air environment and it was placed at the vacuum chamber. Then, the chamber was filled with deuterium gas at a pressure 0.1 MPa; the thin Pd film side of multi-layered Pd sample was exposed to D2 gas. The other side of

D 2 gas

Sample

Sample holder

O ring

Figure 2.

Sample holder for deuterium permeation.

199

sample was evacuated by a turbo molecular pump to prevent the Pd sample being contaminated from the atmosphere. The deuterium permeated from the chamber through the Pd sample to the evacuated side by the pressure gradient for about 1 month. A heater was employed to keep the temperature of the chamber at 70°C during the experiment. After the permeation experiment, the heater is turned off and the chamber was filled with N2 gas, then the sample ("after permeation sample") was taken out from the holder. Before the element analysis, the sample was not treated for purging the deuteron atoms remaining in. The sample surface of gas-filled side was analyzed by TOF-SIMS (ULVAC-PHI: TFS-2100). TOF-SIMS has a good sensitivity for a very small quantity of the elements on the sample with high resolution in mass number although it is difficult to deduce the absolute quantities from its output data alone. The primary ion in TOF-SIMS was Ga + and we measured three randomly selected areas of 40 x 40/xm2. The spectra, given in this paper, were obtained after sputter cleaning of upper most surfaces of samples by the G a + for 10 s. In order to take into account the contamination from the environment, we prepared the control sample ("control sample") without flowing the deuterium gas, which was prepared by the same procedure for the permeation samples. Comparing the composition of the elements on the surface of "Control sample" with that of "after permeation sample", or comparing that of plain Pd sample with that of multi-layered Pd sample, we tried to specify newly produced elements during the deuterium permeation.

3. Result and Discussion A TOF-SIMS spectrum of mass number range 132-141 without deuterium permeation for Cs deposited on plain Pd foil is shown in Fig. 3. No marked 133 C S

_

_

_

_

_

_

;

4 i

_

_

_

_

_

,

/S

•f

["*"

i

12.5 x 12.5mm

" " . " . . I ' d — Pd foil: 0.1mm

4

-£ 400

o O 300 200 100

I S

69Ga2

i

1

O O O O O O O O O O O O O O O O O O O o i f i o i / i O L o o L n o m o m o L n o m o i f i o ( N w c ^ c o ^ - ^ i r i L r i t D c d f ^ r ^ o d c d c r i a i o d ' r ^

Mass Figure 3. TOF-SIMS spectrum of mass number range 132-141 without deuterium permeation for Cs deposited on plain P d foil.

200 25000 J3

Cs

*. 15000 c

Cs

^ Pd film-. 40nm ^ f — C a O film: 2nm -Pd foil: 0.1mm 12.5 x 12.5mm j i

o O

5000

Mass 136 (molecule)

Mass

Figure 4. TOF-SIMS spectrum of mass number range 132-141 without deuterium permeation for Cs deposited on multi-layered Pd sample.

J count, except Cs and Ga2 was seen in this spectrum for this control sample. A TOF-SIMS spectrum of mass number range 132-141 without deuterium permeation for Cs deposited on the multi-layered Pd sample is shown in Fig. 4. The sample was used for another control one and the schematic view of sample is shown in this figure. No marked count was again observed, even though only a few count due to a molecule contaminant at mass number 136 was detected. A TOF-SIMS spectrum of mass number range 132-141 after deuterium permeation at 70°C for the plain Pd foil is shown in Fig. 5, where no

500

69

450

Ga 2

400 350 c

o

o

300 250 200 150

• P d f o i l : 0.1mm 12.5 x 12.5mm

100

£

50

Mass Figure 5. TOF-SIMS spectrum of mass number range 132-141 after deuterium permeation at 70°C for plain Pd foil.

201

8000 133CS

7000 6000

Cs

Pd foil: 0.1mm 12.5 x 12.5mm

4000

Mass

Figure 6. TOF-SIMS spectrum of mass number range 132-141 after deuterium permeation at 70°C for Cs deposited on plain Pd foil.

marked count except 69Ga2 was detected in this mass number range. A TOF-SIMS spectrum of mass number range 132-141 after deuterium permeation at 70°C for Cs deposited on plain Pd foil is shown in Fig. 6. Three peaks at mass number 133, 136, and 138 can be seen in the spectra; these count peaks correspond to Cs, a molecule and Ga2, respectively. TOF-SIMS spectra of the multi-layered sample with small amount of Cs after deuterium permeation at 70°C are shown in Figs. 7-11. Figure 7 shows a spectrum

60000 133CS

arcs

/

^ 40000

c

^

O O 30000

Pd film: 40nm Cao film: 2nm Pd foil: 0.1mm

12.5 x 12.5mm

20000

CO

CO

CO

00

Ol CVJ CO

CM CO

CO CO

CO CO

CO CO

CO CO

o o

070-

CO

060

CO

050

10000

CO CO

CO CO

CO CO

CO CO

Mass Figure 7. TOF-SIMS spectrum around mass number 133 after deuterium permeation at 70°C for Cs deposited on multi-layered Pd sample.

202

100

80

OR

60

/ . . . . .

o O

^ P d f i l m : 40nm + — CaO film: 2nm

1

3

12.5 x 12.5mm

40

20

00

CO

CO

00 CO

CO

CO

CO CO

CO

CO

CO

CO

CO

CO

CO

CO

CO

CO

Mass Figure 8. TOF-SIMS spectrum around mass number 134 after deuterium permeation at 70°C for Cs deposited on multi-layered Pd sample.

around mass number 133, where only the counts corresponding to Cs is seen at mass number 133. Figures 8 and 9 show spectra around mass number 134 and 141, respectively. No marked count was observed in both the spectra. It was not likely that the element 1 4 1 Pr was produced using the multi-layered sample prepared. However, one can recognize a small peak at mass number 141; which may imply a very small amount of Pr production. To the contrary, we have found anomalous peaks at mass number 135 and 137, as shown in Figs. 10 and 11, respectively. The substance, corresponding to mass 100

80

60

—

. ylS

r

12.5x12.5mm o O

„,Pd film: 40nm Hdfoil:u.1mm

40

•**

Ajj»

Mass Figure 9. TOF-SIMS spectrum around mass number 141 after deuterium permeation at 70° C for Cs deposited on multi-layered Pd sample.

203 Mass 135 (~133CsD, - 135 Ba)

100 90 80

Cs

70

„Pdfilm:40nm J^CaOfilm:2nm *—Pd foil: 0.1mm 12.5 x 12.5mm

60 o O

50 40 30 20 10

Aj^o*fr»

^

^

^

^

V

Mass Figure 10. TOF-SIMS spectrum around mass number 135 after deuterium permeation at 70°C for Cs deposited on multi-layered Pd sample.

number 136, is considered to be a molecule. A small peak at mass number 135 may correspond to molecule CsD or an element such as 135 Ba. It should be noticed that the count intensity seen at mass number 137 is higher than that at mass number 135. This is the characteristic commonly observed in all the three measured areas. In general, amount of CsD formed is much more than that of CsD2 during the deuterium permeation experiment. Accordingly, the substance corresponding mass number 137 could not be CsD2. While, the compounds consisting of Pd, which

in in n n

in m

CO

O)

O

in n

in n

ID C D < D C O n cororo

T-

CJ

o

o

CD cd (b m co m

o

o

to to en m

o

o

to co

o

o

o

o

r ^ h ^ r ^ t ^ N cococococo

o o o o o o o o o LO 00 CM C3 C3 CO

CO CO

CO

CO CO

Mass Figure 11. TOF-SIMS spectrum around mass number 137 after deuterium permeation at 70° C for Cs deposited on multi-layered Pd sample.

204

might be formed during the experiment, cannot account for these anomalous counts at mass number 135 and 137. Because no peak appeared at mass numbers 134 and 138 even though Pd has large national isotopic ratios in mass number 105, 106, and 108. The candidate elements and molecules detected by TOF-SIMS in mass number range 133-141 are compiled into Table 1. Most of all the sections are blank. This means almost no count was detected at each mass number. Since no substance with mass number 137 was registered in a control multi-layered Pd sample and in a plain Pd sample with Cs after the permeation, the process of forming multi-layered sample and of depositing Cs seemed to present almost no amount of contaminant of mass number 137 to these samples. Thus, the substance with mass number 137 observed after deuterium permeation is unlikely to be contaminant but would be an element such as 137 La or 137 Ba. The results suggest an impotent role of alpha cluster in the transmutation process of 8 and 12 mass number increasing. Table 1. Candidate elements and molecules detected by TOF-SIMS at mass number range 133-141; blank means almost no count being observed Mass

Plain P d

133 134 135 136 137 138 141

Control P d + Cs

After permeation P d + Cs

Control P d + CaO + Pd + Cs

After permeation P d + CaO + Pd + Cs

Cs

Cs

Cs

Cs

Molecule

Molecule

Ba CsD Molecule Ba La

4. Conclusion Elements analysis on the Pd samples was performed after deuterium permeation experiment and for control Pd samples using TOF-SIMS. The TOF-SIMS has provided the marked count peaks at mass numbers 135 and 137 in spectra after deuterium permeation at 70° C, only when the multi-layered Pd sample with a small amount of Cs was used. The substance with mass number 137 could be 137 La or 137 Ba produced during deuterium permeation by some nuclear transmutation occurring on/in the uppermost of multi-layered Pd sample. The single couple of Pd/CaO thin films on Pd foil might contribute to induce production of an element with mass number 137. This would imply a transmutation of 4 mass number increasing before 1 4 1 Pr production. References 1. Y. Iwamura, T. Itoh, and M. Sakano, Jpn. J. Appl. Phys. 41, 4642 (2002). 2. H. Yamada, S. Narita, H. Onodera, H. Suzuki, N. Tanaka, T. Nyui, and T. Ushirozawa, Proc. 5th Meeting of Japan CF Research Society (2004), p. 69.

205 3. G. H. Miley, H. Hora, A. Lipson, S. Kim, N. Luo, C. H. G. Castano, and T. Woo, Proc. 9th International Conference on Cold Fusion (2002), p. 255. 4. T. Ohmori, H. Yamada, S. Narita, and T. Mizuno, Proc. 9th International Conference on Cold Fusion (2002), p. 284. 5. J. Tian, B. Liu, X. Z. Li, W. Z. Yu, M. Y. Mei, D. X. Cao, A. L. Li, Jing Li, Y. G. Zhao, and C. Zhang, Proc. 9th International Conference on Cold Fusion (2002), p. 360. 6. H. Yamada, S. Narita, S. Taniguchi, T. Ushirozawa, S. Kurihara, M. Higashizawa, H. Sawada, M. Itagaki, and T. Odashima, Proc. 6th Meeting of Japan CF Research Society (2005) p. 48.

E X P E R I M E N T A L OBSERVATION A N D C O M B I N E D INVESTIGATION OF H I G H - P E R F O R M A N C E F U S I O N OF IRON-REGION ISOTOPES IN OPTIMAL G R O W I N G MICROBIOLOGICAL ASSOCIATIONS

V L A D I M I R I. V Y S O T S K I I Kiev National

Shevchenko

University, E-mail:

Vladimirskaya St. 64, 01033 Kiev, [email protected]

Ukraine

A L L A A. K O R N I L O V A Moscow

State

University,

119899 Moscow,

Russia

A L E X A N D R B. TASHIREV Kiev Institute

of Microbiology,

Kiev,

Ukraine

JULIA KORNILOVA Scientific

Center

of System

Investigation

and Technologies,

Moscow,

Russia

The report represents the results of combined (Mossbauer and mass-spectroscopy) examinations of isotopes transmutation process in growing microbiological associations in the iron-region of atomic mass (50 < A < 60). It was shown that the effectiveness of isotopes transmutation during the process of growth of microbiological associations at optimal conditions is by 10—20 times more than the effectiveness of the same transmutation in "one-line" (clean) microbiological cultures.

1. I n t r o d u c t i o n a n d G e n e r a l Consideration Several years ago, we have studied and reported the process of transmutation of stable isotopes in growing "one-line" (one type, "clean") microbiological cultures like Escherichia coli or Deinicocus Radiodurans.1 It was shown that the transmutation process during the growth of such microbiological cultures had taken place but its effectiveness had been low and had equaled A « 1 0 _ 8 s _ 1 in the case of the reaction with light isotope Mn 55 + d2 = Fe 57 and A « 10~ 10 s _ 1 in the reaction with middle range mass isotopes Na 23 + P 3 1 = Fe 54 . The typical Mossbauer spectrum of "one-line" culture Saccharomyces cerevisiae T-8 grown in D2O with the presence of Mn 55 isotope 1 is presented in Fig. 1. The low amplitude of Mossbauer resonance (A J / J « 0.2%) in these experiments was the result of low absolute and relative concentration of created Fe 57 isotope in the culture. 206

207

b 0 i!!ii illilhiirlu'llihltlliiiilMllitn.iti A i i i 0.1 Jllllliff |P|(|||PlP|fiRfPI||||jlP 0.2

*\K

-3.2

MihMi\k\lmLiMk\\ti\ jpp|t p w' l ii|||||p tllfljftl

-1.6

-1.6

-3.2

Velocity, mm/s Figure 1. Mossbauer spectra of grown cultures in different identical flasks. romyces cerevisiae T-8 grown in D2O with presence of M n 5 5 isotope. 1

Culture Saccha-

There are two main reasons of low effectiveness of nuclear transmutation in "one-line" microbiological cultures: • Relatively low effectiveness of the investigated reactions is the result of the narrow interval of optimal functional individual characteristics of any "one-line" type of culture. Each of the "one-line" cultures needs individual specific conditions (temperature, hydrogen ion exponent pH, balanced contents of nutrient medium, etc.) for optimal metabolism during the whole period of growth. Such conditions are often absent in real experiments. • During the growth of "one-line" culture processes of auto-intoxication of nutrient media by metabolic products take place. It leads to the impairment of growth. In a contrast to these "one-line" cultures investigated microbiological associations include great number of types of different cultures. The base of used microbial catalyst-transmutator (MCT) compound is microbe syntrophin associations of thousands different micro-organism kinds that are in the state of complete symbiosis.2 These micro-organisms appertain to different physiological groups that represent practically the whole variety of the microbe metabolism and relevantly all kinds of microbe accumulation mechanisms. The state of complete symbiosis of the syntrophin associations results on the possibility of maximal adaptation of the micro-organisms' association to any external conditions change. These cultures are in a state of natural complete symbiosis and grow as a total correlated multisystem. There are a lot of different types of intraspecific

208

Figure 2. Symbolic scheme of different types of intraspecific and interspecific connections between arbitrary selected culture and different cultures in the volume of syntrophin association. The same connections are related to each culture.

and interspecific stimulated and symbiotic connections between different cultures in the volume of syntrophin associations (Fig. 2). This correlated microbiological multisystem adequately reacts to modifications of exterior requirements, to composition of nutrient medium and to biochemical properties of a system because of metabolism, growth and transmutation processes. The spectrum of their functional characteristics is very wide. It has been expected that it would lead to high effectiveness of stimulation of the transmutation process. This model is presented in symbolic form in Fig. 3. 2. Experiments on Transmutation and the Results of Mossbauer and Mass-Spectroscopy Investigation of Experimental and Control Biological Substances The report presents the results of combined (both Mossbauer and TIMS massspectroscopy) examinations of isotopes transmutation process in growing microbiological associations in the same iron-region of atomic masses (54 < A < 58). The general aim of investigation was to find biotechnology ways for effective isotope transmutation. During experiments microbiological MCT granules were used. Expected Mn 55 + d2 = Fe 57 reaction with heavy water in growing MCT was conducted in the system "D 2 0 + Mn 55 + MCT + additional isotope components". The control experiments were conducted in another system "H2O + Mn 55 + MCT + the same additional isotope components".

209

The growth of optimal cultures at concrete environment at fn

• ••!

JIUIUUUilLmnEtti mlUfituip

Directions of symbiosis and synergism to optimal cultures from all members of association

V?'"-IfHtllllHiiilHffrtBiUm • Metabolic shift at L

Concentration and growth parameters of different microbiological cultures in the same association at concrete environment

iiiuuiiaK^uifomHiuiujLMHinniiniii ^L

Initial chemical composition and biochemical properties of nutrient media at fn (the optimal conditions in brightly area)

Composition (spectrum) of microbiological association (different cultures in state of symbiosis)

(b) ' ';

1

One-line culture, extreme slowed growth

• Metabolic shift

Initial chemical composition and biochemical properties of nutrient media at fn (the optimal conditions in brightly area)

i

\ \ One-line culture, slowed growth

> ,'\

/

One-line culture, maximal growth

Figure 3. Change the directions of symbiosis and synergism in microbiological association (case a) to optimal growing cultures at change of chemistry composition and biochemical properties of nutrient media and environment. Change of type of optimal cultures is the result of metabolic shift of chemical composition and biochemical properties of nutrient media. The case b presents the process of growth impairment in "one-line" culture at metabolic shift.

Many different experiments under varying conditions were carried out. A typical series of experiments concerning nuclear transmutation of elements consisted in growing of certain microbiological culture in three disks simultaneously. The first disk contained full-compounded heavy-hydrous (D 2 0) nutrient medium with MnS0 4 , the second one — also heavy-hydrous (D 2 0) nutrient medium without

210

MnS0 4 , and the third one — light-hydrous (H 2 0) full-compounded (with 0.05% of MnSC^) nutrient medium. Such series of experiments were held for MCT during 20 days at temperature 25°C. After the completing of each series, the obtained biological substance was collected, cleaned in distilled H2O water and dried. The dried substance in the form of a unstructured granules (like peat) was separated using non-iron containing instrument, ground to a powder and placed at the same quantity in Mossbauer spectrometer. The mass of investigated dried biological substance in all cases was about 0.3 g. The results of Mossbauer investigation of both control and optimal dried biological substances are presented in Figs. 4 and 5. In these experiments different amplitudes of Mossbauer resonance ( A J m a x / J ) c o n t r o i « 1.1% and ( A J m a x / J ) t r a n s m u t ~ 3.1%) at the same masses of investigated dried biological substances were observed and measured. It is well known that the amplitude of Mossbauer resonance is proportional to the concentration of resonant nuclei (if this concentration is low). Registration of Mossbauer Fe 57 isotope in the biological substance that was grown in nonoptimal medium (see Fig. 4 for the control experiment) is the result of presence of natural Fe as admixture in the components of initial MCT compound. Earlier 2 we have informed that MCT compound is the special granules that include:

Figure 4. Mossbauer specter of microbiological MCT grown in the volume with presence of H2O and Mn 5 5 isotope (control): A J m a x / J f» 1.1% is the magnitude of Mossbauer resonance.

211

Absorption, %

1"

2-

3;

3.4%

4H

-

•

4

r

'

-

1

3

'

-

1

'

2

1

1 v (mm/s)

•

r

0

1

1

1

1

2

1

3

1

4

Figure 5. Mossbauer specter of microbiological MCT grown in the volume with presence of D2O and Mn 5 5 isotope (experiments on transmutation): A J m a x / J ~ 3.4% is the magnitude of Mossbauer resonance.

• concentrated biomass of metabolically active microorganisms (microbe syntrophin association); • organic sources of carbon and energy, phosphorus, nitrogen, etc.; • gluing substances that keep all components in the form of granules stab le in water solutions for a long period of time at any external conditions. The organic source of microelements contained some small quantity of natural Fe as admixture. In this case the registered Fe 57 isotope is the small part (2.2%) of natural Fe. In experiments on transmutation (see Fig. 6) the same MCT compound with the same organic sources of microelements was used. But the result (presence of Fe 57 isotope) was different - (concentration of Fe 57 isotope in control biological substance less by three times in relation to transmutated biological substance). So, the difference of quantity of Fe 57 isotope in transmutated and control dried biological substances follows from the difference of Mossbauer absorption ( A J m a x / J ) t ransmut - (AJmax/J) control ~

2%,

(AJmax/J)t ransmut

/ ( A J m a x / J ) control ~ ^*: and is the direct result of fusion reaction Mn 55 + d2 = Fe 57 during growth of the same microbiology MCT compound in optimal medium.

212

X/Fe 56 (relative concentration of isotopes)

(a)

X/Fe 56 (relative concentration of isotopes)

1

• •

• •

0.15

0.15

0.05

1

0.1

0.1

1

t

"1"'

Iki

0.0

Figure 6. Mass-spectrum of iron-region of microbiological associations (dried biological substances) that were grown in control nutrient medium with H2O and Mn 5 6 (case a) and in experimental nutrient medium with D2O and the same quantity of Mn 5 5 isotope (case b). Here X = F e 6 4 ; Mn 5 5 ; Fe 5 7 . The process of increasing (f) of concentration of Fe 5 7 isotope is accompanied by decreasing (J.) of concentration of Mn 5 5 isotope.

The total number of created Fe 57 nuclei is about 10 17 nuclei per 1 g of grown and dried biological substances that is by 10-20 times more in comparison with the maximal number of created Fe 57 nuclei in "one-line" grown and dried cultures. 1 The total mass of created Fe 57 isotope is about 10~ 5 g per each g of dried biological substance. The effectiveness has increased, in particular, because the association has grown during 20 days. "One-line" culture cannot grow so long in heavy water because self-intoxication of the medium by the metabolism products (in our former experiments 1 the "oneline" E. coli culture has grown during 72 h). The effectiveness of such transmutation (the coefficient of transmutation) is the following: A « iV(Fe 57 )/iV(Mn 55 )At « (0.5,..., 1)10"

(synthesized Fe 57 nuclei per s and per single Mn 55 nucleus).

For verification of these results additional examinations of isotopes ratio of the same dried biological substances (both control and transmutated) were conducted by TIMS ("Finnigan" MAT-262) spectroscopy. The results of TIMS massspectroscopy investigation are presented in Fig. 6 and in Table 1. Table 1. Parameters of mass-spectroscopy investigation of control and transmutated cultures

Isotope, natural concentration

Natural isotopic ratio (in relation to Fe 56 )

Mn 55 , 100% Fe 56 , 91.7% Fe 57 , 2.2%

— 1 Fe 56 /Fe £

= 41.7

Concentration in dried biological substance in control experiment: H2O-t-MnSC-4-f nutrient medium. Counts/s (normalized)

0.024 ± 0.002

Isotopic ratio in control biological substance

Concentration in dried biological substance in experiment on transmutation: D 2 0 + MnS0 4 + nutrient medium. Counts/s (normalized)

Isotopic ratio in the experiment on transmutation:

Mn 5 5 /Fe 5 7 = 6.6 1 Fe 5 6 /Fe 5 7 = 42.5

0.13 ± 0.012 1 0.051 ± 0.003

Mn B5 /Fe 57 = 7.7 1 Fe 5 6 /Fe 5 7 = 19.5

213

3.

Conclusions • T h e results of examination of created Fe 5 7 isotope are approximately the same in the cases of Mossbauer resonant gamma-spectroscopy and TIMS mass spectroscopy (increasing of concentration of created Fe 5 7 isotope by 2-3 times). • T h e effectiveness of isotopes t r a n s m u t a t i o n during the process of growth of microbiological associations at optimal conditions is by 10-20 times more t h a n the effectiveness of the same t r a n s m u t a t i o n in "One-line" (clean) microbiological cultures. • T h e structure and half-width of Mossbauer spectrums of control and transm u t a t e d microbiological association are identical. So, the process of transmutation does not change spatial structure of growing biological culture. Created and n a t u r a l Fe are identical in the biochemical sense! • Decreasing of additional M n 5 5 isotope in t r a n s m u t a t i o n flask is synchronized with the creation of Fe 5 7 isotope in the same flask. It is one of acknowledgement of nuclear synthesis in growing biological system!

References 1. V.I Vysotskii and A.A. Kornilova, Nuclear Fusion and Transmutation of Isotopes in Biological Systems. MIR Publishing House, Moscow (2003). 2. V.I.Vysotskii, A. Odintsov, V.N. Pavlovich, A.B.Tashirev, and A.A.Kornilova, Experiments on controlled decontamination of water mixture of long-lived active isotopes in biological cells. Proc. IGCF-11, Marseilles, France, pp. 530-536 (2004).

R E S E A R C H INTO LOW-ENERGY N U C L E A R REACTIONS IN CATHODE SAMPLE SOLID W I T H P R O D U C T I O N OF EXCESS HEAT, STABLE A N D R A D I O A C T I V E I M P U R I T Y NUCLIDES

A.B. K A R A B U T FSUE

"LUCH" 24 Zheleznodorozhnaya St, Podolsk, Moscow E-mail: [email protected]

Region

U2100,

Russia

Results on measurements of excess heat power, impurity nuclides yield, gamma and X-ray emission in experiments with high-current glow discharge (GD) in D2, Xe, and Kr are presented. The cathode samples used in the experiments were made of Pd, V, Nb, and Ta. In experiments with Pd cathode samples in D2 GD, the recorded excess heat power amounted to 10-15 W and the heat efficiency (the output heat power in relation to the input electric power) was up to 130%. Excess heat power up to 5 W, and efficiency up to 150% was recorded for deuterium pre-charged Pd cathode samples in Xe and Kr discharges. Production of impurity nuclides with atomic masses less than and more than that of the cathode material was registered. Considerable deviation from the natural isotopic ratio was observed for the registered elemental impurities. X-ray emission was measured in H2, D2, Ar, Xe, and Kr GD during the GD operation and after the GD current switch off (up to several hours afterward) with the help of thermo-luminescent detectors (TLD), X-ray film and scintillator detectors with photomultipliers. The energy of recorded X-ray emission distributed in the range 0.5-10 keV. Weak gamma-emission (up to 1000 events per second) was registered in certain experimental conditions. The Xray spectra include both (bands of) the continuum and multiple lines with energies ranging 0.1-3.0 MeV. The possible mechanism for production of the excess heat power, elemental impurities, gamma, and X-ray emission is also considered.

1. Introduction Measurements of the excess heat, isotopic impurities, heavy particles emission, and soft X-ray emission in high-current density glow discharge have been carried out for years. Further experimental evidence is required to elaborate a reliable theory explaining the phenomena under discussion. The present research is focused on this problem. 2. Excess Heat Measurements by Flow Calorimeter The measurements were carried out using the glow discharge device (GDD) consisting of a water-cooled vacuum chamber, the cathode, and the anode assemblies (Fig. 1). The cathode design allowed the placement of the cathode samples made of various materials on the cooled surface. Three components of the device (the cathode, anode, and chamber) had independent water-cooling channels. Each cooling 214

215

Figure 1. Experimental glow discharge device (flow continuous calorimeter). (1) vacuum discharge chamber, (2) cathode holder unit, (3) cathode sample, (4) anode unit, (5) input and output of water cooling system, (6) out channel of X-ray emission, (7) 15 fim Be shield, (8) X-ray detector of the different kinds, (9) heat insulation cover, and (10) windows in heat insulation cover.

channel incorporated thermal sensor (at the input and output) connected differentially and a water flow meter. The device was placed into a thermal insulation package, comprising the flow calorimeter. The pulse-periodic electric power supply was used. The thermal (signals from thermal sensor and the flow-meter) and the electric parameters (the GD current and voltage) were recorded using a data acquisition board. The values obtained were processed by a computer. The excess heat power PEH value was determined by PEH = (PHC + ^HA + Pnch) - Pei ± AP e r r o r , where Pei is the GD input electric power; PHC, -PHA; and PHCh represent the output heat power carried away by the cooling water from the cathode, anode and chamber, respectively; AP e r r o r stands for the systematic error of the power measurement for the given measuring system. Calibration of the measurement system was carried out in the following way: a water-cooled electric resistive heater wrapped into an insulating package was placed among the thermistors inside each thermal power measuring channel. The amount of the consumed cooling water corresponded to that inside the GDD. The resistive heater was powered by a pulse-periodic power supply. The heater electric parameters were identical to those of the GD. The measured heat power of the resistive heater was equated to the heater measured electric power. The calibration relationship was estimated at different values of the input electric power.

216

The Pd samples used in tests with Xe and Kr GD were not deuterium precharged. The measurement system allowed to record the GD input electric power and the thermal power output by the cooling water with accuracy of 0.6 W at the absolute value of the electrical power up to 120 W (relative error ±0.5%). In this set of the experiments the current density did not exceed 100 mA/cm 2 . At such values of the discharge current in D 2 , a continuous loading of D 2 into Pd ran up to saturation. The experiments were carried out with Pd cathode samples in D 2 GD, and with deuterium pre-charged Pd cathode samples in Xe and Kr discharges. The amount of the loaded D 2 was estimated by the pressure drop in the chamber. D 2 was periodically supplied into the chamber to maintain the required pressure. The amount of deuterium loaded into palladium was determined by the volume of the gas absorbed from the discharge chamber. When saturation was achieved, the value of the D/Pd ratio was close to 1. t(W) 8 7

#-PdD-D ©-PdD-Xe B-PdD- Kr

6 5 4 3 2 1 0

i

i

i

2

4

6

J 8

I L J I 10 12 14 16 p

l m

' e l . input l v v >

Figure 2. Excess heat power in relation to the input electric power. Pd cathode sample, d = 9 mm; Deuterium pre-charged Pd cathode samples in Xe and Kr discharges. (1) Optimal (1100-1300 V) Glow Discharge voltage and (2) not optimal glow discharge voltage.

Heat measurements were carried out for Pd cathode samples in GD while changing the following parameters: GD current density, voltage, duration of current pulses, and the time between current pulses (from the power supply). The absolute value of the excess heat power and thermal efficiency grew with increasing the power input into the discharge (Fig. 2). Relatively high values of the excess heat power and thermal efficiency were achieved for deuterium pre-charged cathode samples in Xe and Kr discharges. No excess heat power production was observed in the cathode samples made of pure Pd (not deuterium pre-charged) in Xe and Kr discharges (Fig. 3, curve 3). Two typical groups of the results can be noted: relatively large values of the excess heat power and efficiency coefficient (curve 1) and the group the results with lower values of the excess heat power and efficiency coefficient (curve 2). The large

217

^heat out'°el.input (%)

170 160 150 #-PdD-D ©-PdD-Xe 0-PdD-Kr * - P d _ Kr

140 130 120

__ __ — * ©

._/ ^ *

%

03 ^

110 100 90 0

J 2

I 4

I 6

I 8

I I I I 10 12 14 16

L el.input

(W)

Figure 3. Dependence of the output heat power to the input electric power ratio of the input electric power. (1, 2) Deuterium pre-charged Pd cathode samples in D2, Xe, and Kr discharges, d = 9 mm. (1) optimal (1100-1300 V) glow discharge voltage, and (2) not optimal glow discharge voltage, and (3) non-deuterium-charged Pd cathode.

values of the excess heat power and efficiency coefficient were observed under the modes when the GD operational voltage ranging 1000-1300 V (Fig. 5). The three-channel system of separate measurements of the output excess heat power (for the anode, cathode, and chamber) allowed to define the structure of the excess heat power output in the GD. Large efficiency values were achieved in experiments with high relative heat release on the cathode. This data prove that the excess heat power was produced mainly on the cathode (Fig. 4). Thus, it was experimentally shown that the excess heat power production was determined by two processes: (1) deuterium should be loaded into the medium of ,(W)

•*-PdD-D ©PdD-Xe E-PdD-Kr • - Pd-Kr

I 0

I

I

I

I

10

12

14

16

Pe,,npu,(W)

Figure 4. Dependence of the cathode output heat power of the input electric power. (1) Deuterium pre-charged Pd cathode samples in D2, Xe and Kr discharges, d = 9mm, optimal (11001300 V) Glow Discharge voltage, (2) Non-deuterium-charged Pd cathode, in Kr discharge.

218

1

170

"heat out' °el.input

«-PdD-D o-PdD-Xe H-PdD-Kr

\'°)

160 150 140 130 120 110 100 .1 0.8

I

I 1.0

I

I 1.2

I

I 1.4

I

I L 1.6 Ue, (keV)

Figure 5. Dependence of the output heat power and the input electric power ratio of the GD voltage. Deuterium pre-charged Pd cathode samples in D2, Xe, and Kr discharges.

the solid crystal lattice and (2) the crystal lattice should get initial excitation, so that high-energy long-lived excited levels were created in the cathode solid. These excited conditions could be created by an additional source (e.g., by a flow of inert gas ions). 3. Registration of Impuruty Nuclides Presently, the release of excess heat power is accounted for by 4 He production and the on-going reactions of transmutation accompanied by the impurity nuclides yield. We had registered 4 He in the early experiments. 1 Some of Pd cathodes together with the reference samples were analyzed at the Rockwell International Laboratory (Oliver's group). A small increase in the 3 He concentration and a large increase in the 4 He concentration was found in the discharge treated Pd samples. The results of two experiments are represented in Table 1. This is the third independent evidence of 4 He presence in the nuclear reaction. The impurity elements content in the cathode samples were analyzed before and after the experiments with high-current GDD. In the early experiments, we had analyzed the charge number of the impurity elements (X-ray fluorescent spectrometry) and the atomic mass number (secondary ionic mass spectrometry). This results were approximately equal (Table 2). Table 1. The relative content of produced 3 H e and He in the cathode sample after Glow Discharge experiment. The cathode-plasma forming gaze forming system is Pd-D2; current: 35 mA; time of the experiment: 4h. 1NO.

1 2

rieafterdischarge /

Up to 10 times Up to 2 times

ileinitial

tieafterclischarge/

Up to 100 times Up to 35 times

rleinitial

219 Table 2. The content of produced impurity nuclides in the cathode sample after Glow Discharge experiment. The cathode-plasma forming gaze forming system is Pd-D2; current: 35 mA; time of the experiment: 4 h. Analysis made by X-ray fluorescent spectrometry method. Impurity element Content (%)

Na 0.07

Mg 0.01

Al 0.04

Ca 0.04

Si 0.015

Ti 0.01

Br 0.03

Sr 0.07

Y 0.4

Mo 0.15

Tc 0.2

The following methods were used: secondary ionic mass spectrometry (for Pd samples), and secondary neutral mass spectrometry (for V, Nb, and Ta samples). These techniques were used to analyze the impurity content in the cathode samples material before, and after, the experiment. The Pd cathode samples were analyzed for impurities after their exposure to D2 discharge. The cathode samples made of mono-isotopic metals (V, Nb, and Ta) were studied after the exposure to D2 and H2 at the same GD operational regimes. The difference in the content of the impurity elements before, and after, the experiment was defined as storage of the elements during the experiment. The procedure for determining the impurities by the method of the secondary ion mass spectrometry included the following stages: (a) removal the upper 1.5-nm-thick defect layer by plasma etching, (b) scanning the first and the second layers in 5 nm increments, while determining the content of the impurity nuclides, and (c) removal of a layer with the thickness of 700 nm and repeated scanning of the third and fourth layers in 5 nm increments while again determining the content of the impurity nuclides (Fig. 6). The maximum quantity of impurity nuclides was registered in Pd samples after exposure to D2 discharge. Elemental impurities with masses approximately half the Pd mass or close to Pd mass were recorded in the 100 nm thick near-surface layer in amount up to some tens percents. The main impurity elements (isotopes) with more than 1% content included: 7 Li, 1 2 C, 15 N, 20 Ne, 29 Si, 44 Ca, 48 Ca, 56 Fe, 57 Fe, 59 Co, 64 Zn, 66 Zn, 75 As, 107 Ag, 109 Ag, 110 Cg, m C g , 112 Cg, 114 Cg, and 115 In (Table 3). The impurity content in the cathode sample volume was defined at different depths. 800 nm

Figure 6. Registration procedure for the impurity contents in the cathode samples (methods SIMS and SNMS). 1-dirty superficial layer, 2, 3-analyzed layers 1, 2 scans, 4-surface of the cathode samples, 5-removal of a metal layer, 6, 7- analyzed layers, 3, 4 scans.

220 Table 3. The impurity nuclides content in the cathode sample surface layer after Glow Discharge experiment. The cathode-plasma forming gaze system is Pd-D2; current: 100 mA; time of the experiment: 22 h. Analysis made by SIMS method. An Impur. nuclide 6

Li Li U B

7

12C 13C

20 Ne 42 C a 44

Ca 45 Sc 46

T i

47Ti 48 T i 52 56

Cr Fe

57pe 59 66

Co Zn

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

4 scan 800nm, content

(%)

(%)

(%)

(%)

0.075 0.84 0.14 0.93 0.19 0.14 0.72 2.0 0.74 0.57 0.25 1.1 0.62 2.9 5.5 1.0 0.21

0.21 0.45 0.18 0.47 0.05 0.14 1.08 3.1 0.86 0.52 0.31 1.1 0.31 3.1 3.53 1.4 0.54

0.22 0.53 0.31 0.63 0.15 0.27 1.14 3.2 0.91 0.72 0.14 1.23 0.41 2.6 3.25 1.0 0.43

0.16 0.47 0.18 0.54 0.06 0.16 0.8 2.6 0.8 0.7 0.14 0.66 0.1 2.7 3.16 1.5 1.0

An Impur. nuclide 71

Ga Ge 75 As 77 Se 78 Se 79 Br 80 Se 82 Se 85 Rb 72

88Sr 90

Zr Cd 112 Cd 113 Cd 114 Cd lu

115In

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700nm, content

4 scan 800 nm, content

(%)

(%)

(%)

(%)

4.0 5.1 6.2 3.4 4.5 3.0 4.0 3.4 2.2 3.1 2.4 2.8 3.4 4.0 4.7 2.2

4.9 4.4 4.9 3.9 3.45 2.4 3.4 3.0 3.4 4.4 1.5 3.0 3.2 1.8 3.9 2.5

5.6 5.1 7.4 4.8 5.8 2.8 2.5

3.4 6.0 4.7 4.0 1.4

3.3 4.2 2.3 3.0 4.2 2.8 3.3 2.3

2.3 3.2 3.6 6.0 5.8 3.4 5.1 3.6

Noticeably smaller quantity of impurity nuclides was produced in V, Nb, and Ta cathode samples. In V samples, the masses of impurity nuclides exceeded by two or more times the V mass. Thus, it may be assumed that two V nuclei and one H2 and D2 nucleus, correspondingly, participate in the transmutation reactions. Similar pattern was observed with Nb samples. The production of light impurities Table 4. The impurity nuclides content in the cathode sample surface layer after Glow Discharge experiment. The cathode-plasma forming gaze systems are V-H2 and V-D2; current: 100 mA; time of the experiment: 4h. Analysis made by SIMS method. V-D

V-H An Impur. nuclide

"Ru 102 Ru 103 Rh 104pd 106pd 108pd ln

Cd

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

(%)

(%)

(%)

ND 0.66 0.25 0.16 0.15 0.45 0.05

ND 0.73 0.14 0.04 0.02 0.04 0.16

ND 0.4 0.02 0.3 0.02 0.06 0.01

An Impur. nuclide 99

Ru Ru 103 Rh

102

104pd 106pd 108pd lu

Cd

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

(%)

(%)

(%)

0.42 0.74 0.19 0.22 0.29 0.21 0.15

0.11 0.51 0.23 0.2 0.16 0.24 0.2

0.02 0.4 0.34 0.37 0.12 0.12 0.07

221 Table 5. The impurity nuclides content in the cathode sample surface layer after Glow Discharge experiment. The cathode-plasma forming gaze systems are Nb-H2 and Nb-D2; current: 100mA; time of the experiment: 4h. Analysis made by SIMS method. Nb-H An Impur. nuclide 99

Ru Ru

102

104 p d 106pd 108pd

noPd 118 Sn 120 Sn 139 La

Nb-D

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

(%)

(%)

(%)

0.08 0.14 1.02 1.97 1.26 1.0 0.12 0.34 ND

0.07 0.07 0.53 1.76 1.56 1.32 0.07 0.24 ND

An Impur. nuclide 99

0.07 0.05 0.47 1.59 1.65 0.79 0.19 0.16 ND

Ru Ru

102

104pd 106 p d 108pd

nopd 118 Sn 120 Sn 139 La

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

(%)

(%)

(%)

0.27 ND ND 0.26 0.32 0.27 ND ND 0.34

0.16 ND ND 0.26 0.35 0.25 ND ND 0.23

0.1 ND ND 0.17 0.28 0.31 ND ND 0.16

(including rare-earth nuclides) was registered for Ta. After exposure to H2 and D2 discharge these metals showed great variety (in form and quantity) of impurity nuclides. This may suggest nuclear origin of the phenomenon in question, since the chemical, and thermo-physical characteristics of H2 and D2 are practically the same. Alongside with formation of impurity nuclides with V, Nb, and Ta cathode Table 6. The impurity nuclides content in the cathode sample surface layer after Glow Discharge experiment. The cathode-plasma forming gaze systems are Ta-H2 and Ta-D2j current: 100 mA; time of the experiment: 4h. Analysis made by SIMS method. Ta-H An Impur. nuclide 23

Na Ca 63 Cu 65 Cu 99 Ru 40

106 p d 108pd 183W 184W 185

Re

186W 153Eu 163

173

Dy Y b

Ta-D

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

(%)

(%)

(%)

1.5 1.1 0.08 0.043 0.022 0.019 0.015 2.14 0.21 0.004 0.006 ND ND ND

0.74 0.74 0.07 0.023 0.006 0.017 0.017 2.42 0.27 ND 0.007 ND ND ND

0.36 0.51 0.03 0.19 0.005 0.024 0.016 2.4 0.27 ND 0.005 ND ND ND

An Impur. nuclide 23

Na Ca 63 Cu 65 Cu 99 Ru 40

106pd 108pd 183W 184W 185

Re

186W 153 163

Eu Dy

173

Y b

1 scan 10 nm, content

2 scan 50 nm, content

3 scan 700 nm, content

(%)

(%)

(%)

0.85 1.1 ND ND 0.015 0.009 0.006 1.5 0.21 0.027 0.045 0.004 0.0045 0.006

0.49 0.81 ND ND 0.004 0.004 0.004 1.75 0.16 0.027 0.04 0.012 0.006 0.012

0.24 0.39 ND ND 0.003 0.003 ND 1.8 0.14 0.03 0.04 0.005 0.004 ND

222

samples, considerable reduction (by tens of times) in the content of some light elemental impurities (which had been present in the samples before the experiment) was observed. 4. Gamma-emission Registration Weak gamma emission was registered in certain experimental conditions (specific geometry of the discharge chamber, cathode, and anode). The gamma emission was recorded over the whole volume of the discharge chamber. The gamma-emission registration was carried out using HPGe detectors and a multi-channel spectrum analyzer. The detector with the glow discharge device with the detector was placed into the shield made of lead with thickness of 10 mm. Gamma-emission ranging 0.1-3.0 MeV was observed during the GD operation and within 8 days after the discharge current switch off. In the course of long intervals between the experiments (up to some months) the repeated measurement of the background spectra was also carried out. The value of gamma - emission was determined taking into account the geometrical and physical efficiency of the detector and the registered background value. The value of gamma background fluctuation did not exceed 10% during the experiment (5 months). 2 3 p _ ^ 23

Ne -> 23 Na Ne ->24 Na - 24 Mg 39 3 9 g _ > CI -+ 39 Ar 59 Cr -V^Mn - 5 9 Fe --. 5 9 Co 67 Ni- ^ 7 Cu --+ 67 Zn 69 Ni- -^69 Cu --^69 Zn -^69 G a ^ 6 9 G e 73 Zn -^ 73 Ga - 7 3 G e 81 Ga ^ 8 1 G e ^ 8 1 As --.81 g e ^ 8 1 B r 83 Ge ^ 8 3 As -- 8 3 Se -^83 B r ^ 8 3 K r 84 As- - 8 4 Se -^ 8 4 Br -H• 8 4 K r 87 As- - 8 7 Se --+87 Br -,87 fo ^ 8 7 R b 9 3 B r .- 9 3 Kr -^ 9 3 Rb -^93 g r ^ 9 3 Y ^ 9 3 & 94 Kr ^ 9 4 Rb ^ 9 4 Sr -4 94 Y ^ 9 4 ^ j . 99 Rb - + " Sr -_^99 y _> 99 Zr ^ " Nb - > " Mo 100y ^ 1 0 ° Zr ^ 1 0 ° Nb ^ 1 0 ° Mo 101y ^ 1 0 1 Zr -^ 1 0 1 Nb _ ^ i o i M o ^ i o i T c ^ i 2 4 p _ ,2i

105Nb ^105 115

Rh ^

115

M Q

^105

Pd ^

115

T(,

^105

Ag -^

115

R u

^105

Cd -^

115

R h

^105 p

d

In

The cathodes made of the different materials showed the value of inductive gamma-radiation after the GD current switch off. The intensity of the emission increased with the increase in dose of plasma ion radiation (D2, H2, Ar, and Xe) of the plasma forming gas for the cathode sample. The spectra of inductive gammaactivity include areas exceeding the continuous spectra (continuum) and the lines imposed on them. In this case the value exceeding the area of gamma line over

223 A/j

1 %

d

•

i" !

400

i i i

I I

600

/'

'f fk

200 W L & H - T A .1. 1

-Je.

-, 1

0

200

IW!^KH , &'MS ^ M *

600

400

800 E(keV)

Figure 7. Gamma emission spectrum recorded by Ge-Li detector from the GD device after, the discharge current switch off. Pd cathode placed in D2 discharge. The part of the spectrum area ("d" - area) is presented in greater detail (see Fig. 8.).

background (a) is not a large factor a (a = 2.5-5). The value for the continuum is a = 8-10. The gamma spectra obtained during the GD operation and after the GD current switch off were processed with the help of a database to identify gamma lines of radioactive nuclides.2 For each /^-transition 30 or 40 gamma lines were identified. For a single /3-radioactive decay chain (one atomic mass of radioactive nuclides) 100-200 gamma-lines were identified. The gamma emission spectrum registered after the GD current switch off contains gamma lines of short-lived (3- radioactive chains (Figs. 7 and 8). Presumably after the GD current switch off there appear certain conditions for initiating nuclear reactions. The total number of radioactive atoms was determined taking into account the values of gamma-line areas, the value of the detector efficiency, and the ,1

Ru, 306.8 'Br, 334.0 E E aaSr, 307.0 , , , — m,n 336 2 2% i«Tc, 309.5, ' -MO,

250

42

Ca^312.6

12,

200

107

^Rh, 374.3 374.9

101Tc, 408.7 84 Br, 408.2 105 Rh, 407.6

r

!3

Na, 440.0 Zn, 438.6

i9

Cd, 481.0 'Cd, 478.7

348.5 ' " N b , 373.9

Pd, 348.2

r°lNb

83

ln, 313.7 I

150 100 50

a

Br, 345.2 Pd, 344.5 115 Ag, 342.7

105

300

400

E, (keV)51

Figure 8. Part of gamma emission spectrum indicating identified gamma-lines The duration of the discharge operation was 10,000 s. The duration of the gamma spectrum registration was 60,000 s after the discharge current switch off. The background spectrum (60,000 s duration) was subtracted from the operational spectrum. The lines are identified as related to excited nuclei of beta-decay chains.

224

value of the quantum yield. The /3-radioactive chains with masses of A = 23, 24, 39, 59, 67, 69, 73, 81, 83, 84, 87, 93, 94, 99, 100, 101, 105, and 115, make the main contribution into gamma-radiation (operating time for radioactive nuclides is up to 10 5 atoms). 5. X-ray Emmission Registration The initial excitation energy up to several keV is needed to trigger the assumed nuclear reactions within the cathode sample solid (the density of the interactive nuclei corresponding to that of the solid). The existence of such excited energetic levels is evidenced by intensive X-ray emission from the cathode sample solid medium observed in the experiments. The recording of the X-rays was carried out using thermo-luminescent detectors (TLD), an X-ray film and scintillator detectors with photomultipliers. l The high intensity of the X-rays made it possible to obtain an optic image of the emission area. This was done by a pinhole camera (with 2.0 mm diameter hole as an optic lens). The image shows that the cathode area measuring 9 mm diameter (Fig. 9) and especially its central part is the most luminescent. The pinhole provided a spatial resolution of the X-ray emission. The X-ray emission registration by the pinhole was performed without any induced magnetic field, and, with lateral 0.3 T magnetic field induced in front of the pinhole (to deflect the charged particles flow from the cathode). Absence of noticeable difference between the two images (Fig. 9b and c) shows that the pinhole recorded the X-ray emission.

Figure 9. The diagram of the X-ray image registration using the pinhole. The objective with 2.0 mm diameter closes by the 15(im Be shield. The system Pd-D2, the discharge current: 150 mA; voltage is 1850 V; the exposure time: 10,000 s. (a) X-ray image registration without superimposition of the cross magnetic field; (b) X-ray image registration with superimposition of the cross magnetic field 0.3 T. The image is positive. (1) anode, (2) discharge plasma area, and (3) cathode.

The evaluation of the X-ray emission was made with reference to the change in the radiation dose absorbed by thermo-luminescent detectors covered with Be foils of varying thickness. The experimentally determined value of the X-ray energy increased from 1.2 to 1.5 keV when the thickness of the Be shield increased from

225 Table 7. The characteristic of X-ray emission from different cathode samples in Glow Discharge experiment. Material of cathode Glow discharge voltage (V) Glow discharge current (mA) X-ray energy during passing the discharge current, J3x—ray (keV) X-ray energy without current, J^X-ray (keV)

Al Sc Ti Ni 1650 1540 1730 1650 130 130 170 150 1.54 1.26 1.45 1.91

Mo Pd Ta Re 1420 1650 1600 1520 210 138 138 125 1.48 1.98 1.62 1.36

Pt Pb 1650 1610 138 138 1.47 1.36

1.68

1.33

1.75

1.5

1.46

1.96

1.71

1.62

1.38

1.45

15 to 300 /jm. X-ray emission as a function of time was studied with scintillator detectors and photomultipliers (PM). For different cathode materials the X-ray energy values obtained with the help of scintillator detectors, PM and 15 and 30 /iin-thick beryllium foils amounted to Ex-ra,y ~ 1.0-2.5 keV (Table 7), which showed good agreement with the TLD data. The X-ray spectra were determined using the curved mica crystal X-ray spectrometer fixed (positioned) on an X-ray film (Fig. 10). The X-ray wave length was evaluated by the expression: m x A = 2 x d x sin#, where A is the wave length, d stands for the distance between crystallographic planes of the mica crystal, 2 x d = 2nm; 9 represents Bragg divergence (angle); m stands for the diffraction order. The spectrum was registered both as bands of the continuum with energies ranging 0.6-10.0 keV and as spots resulting from the emission of series of high-density mono-energetic X-ray beams (with energies up to 0.6-10.0 keV) characterized by small angular divergence. The energetic position within the spectrum depended upon the cathode material used (was specific for a given cathode material) and was similar to characteristic X-ray spectra. Of particular interest was the persistence of the X-ray spectrum registration for several hours after turning off the GD current. Presumably, some long-lived excited levels with energies up to several keV are formed in the cathode solid-state medium, and after the GD current is cut off, the excitation persists maintained by the X-ray emission. The spectrum band ranging in energy 1.2-1.3 keV was defined for Pd cathode samples in D2 and Kr GD (during its operation, and after, the discharge current switch off) (Fig. 10). This result is in good agreement with the maximum value of excess heat power at 1000-1300 V GD voltage. 6. Discussion Experiments on anomalies in high-current glow discharge carried out for several years allow to outline the basic processes and conditions of their occurrence. (1) Excess heat production. Excess heat was produced in the volume of the solid-state medium of the cathode sample under the following conditions: • Deuterium should be loaded into the solid-state cathode medium.

226

Pd-D

^ ? # ^ r : < r : . ; r •; • „ "#.,

20 10

5 0 40

:io

2.0

18

15

v

20 10

5.0 4.0

JO

1.4

y VVj-

v

Pd_Kr

Pd-Xe

* -\ 3.6 " "'

20

18

16

1.4

- ^ ^Tgrggjgip

?0 10

5 0 4.0

3.0

2.0

1.8

1.6

1.4

^x-ray (keV)

Figure 10. The outline of X-ray spectrum registration from the Pd cathode sample using the curved mica crystal spectrometer. (a5 b, c, d) during the GD operation, the exposure time is 18,000 s. (a) during the GD operation in D2; (b, c, d) the Pd cathode samples are non deuteriumcharged, (b) GD in Ar, (c) GD in Kr, (d) GD in Xe, (e) the spectrum registered after the GD in D2 current switch off.

® Initiating excitation of the energy levels of the crystal lattice of the cathode material was necessary. ® This initiation could be achieved by a foreign source (e.g., by a flow of inert gas ions). ® The production of the excess heat power occurred mainly in the nearsurface layer of the cathode sample with the thickness up to 1/im (where the impurity nuclides were found). The volume density of the excess heat power showed a value up to 105 W/cm 3 . (2) Production of elements (isotopes) as an induced impurity of the basic cathode material.

227

• The production of impurity nuclides occurred in the volume of the solid-state cathode medium, presumably, as a result of nuclear transmutation reactions. • The emission of high-energy heavy ions was not recorded in the experiment. This allows to assume, that the nuclear reactions energy was not released as a kinetic energy of the formed impurity nuclides. The impurity nuclides may be assumed to form as nuclear isomers (the nuclei being in the excited state). The results of the experiment showed that the relaxation of these excited nuclear levels through the gammaradiation channel was strongly suppressed. (3) Excitation of the energy levels in the solid-state cathode medium. • Formation of the excited energy levels in the crystal lattice was evidenced by recording the X-rays from solid-state cathode. • X-rays were observed as bursts of short duration (presumably up to 1 0 - 1 3 s). Each burst contained up to 109 X-ray quanta with the energy of 1.5-1.8 keV. The bursts were recorded in amount of up to 105 bursts per second during the GD operation and within 100 ms after turning off the GD current. • Hypothetically, the mechanism of forming this radiation was the following. When bombarding the cathode surface by the discharge plasma ions in the solid medium, excited energy levels with the energy of 1.5-2.5 keV and lifetime up to 100 ms were formed. Looking into the concrete physical mechanism of forming these levels requires some additional research. It is possible to assume the existence of one of the two possible physical phenomena: (1) excitation of internal electronic - nuclear system without ionizing the external electrons; (2) oscillatory deformation of the electron-nuclear system of the solid ions. The core of electronic shells was displaced from a nucleus with forming a dipole (optical polar phonon). • The relaxation of the excited energy levels of the solid medium occurred through the emission of X-rays and, perhaps, fast electrons. • Hypothetically, the relaxation of the excited levels occurred simultaneously from micro mono-crystals that make up the solid medium. In other words, the totality of the excited ions of the micro mono-crystal relaxed simultaneously and gave the X-rays burst. (4) Nuclear transmutation reactions. The excited energy states with the population density of n ex ; t (cm - 3 ) and a characteristic temperature of Texit ~ 1-5-1.8keV, and more (up to 20,000,000 K, and more), were formed in the solid with every pulse of the glow discharge current. These energy states existed for the characteristic time Texit (up to 100 ms and more). Such medium, in which the temperature of the crystalline lattice did not exceed some hundreds Kelvin, we call a non-equilibrium medium.

• Occurrence of non-equilibrium nuclear transmutation reactions was made possible in such medium. Probability of running these reactions (and accordingly the value of the excess heat power) was determined by the criterion: ^exit X T ex it /* (^exit -* T e x itjmiii'

This criterion was a modified Lawson's criterion used for estimating the positive heat output at inertial thermonuclear synthesis. • The population density was defined by the parameters of the discharge duration and the cathode sample geometry. The characteristic lifetime of the excited states was defined by the balance between the processes that produce excitation of the energy levels (when passing a pulse of the pumping discharge current), and, relaxation processes of these levels (by emitting the X-rays). Thus, for obtaining large quantities of the excess heat power it was necessary to create a high population density of vibration- dipole energy states n ex it and to suppress the X-rays emission (for increasing a lifetime of the excited states Tex;t). (5) The following types of the nuclear transmutation reactions resulting in formation of the stable nuclides are possible: A + m B ^ [AB]*, A + A + m B ^ [2AB]*, [AB]* - ^ F * - ^ F + Heat, [AB]* -> C * +D* - • C + D + Heat, where A is Pd or the nucleus of another element; B stands for deuterium or hydrogen; [AB]* represents short-lived intermediate compound nucleus; m = 1, 2, 3 , . . . , C*, D* are the nuclear isomers of nuclides with masses less than that of Pd; C,D are stable nuclides, F stands for a nuclide with mass more than that of Pd. First a composite compound-nucleus in the excited state is formed. Then one of the two possible modes is realized: (a) The compound-nucleus could lose its excitation and form a stable nucleus, being heavier than Pd; (b) the compound nucleus could fission into two nuclear fragments with masses less than that of Pd. In doing so, the two nuclei should be in excited isomeric states (experiments showed that the nuclear reactions energy was not produced as a kinetic energy). (6) To determine the specific physical mechanism for these reactions requires some additional research. One possible type of reaction for forming the impurity nuclides can be long-range (resonant) nuclear reactions. The mechanism of such long-range reactions can be explained using as an example a specific transmutation reaction for Pd + D (Fig. 11a) and Pd + 2D (Fig. l i b ) .

229

The formation of significant 13 C nuclide and 93 Nb was recorded in the experiments. Assumedly, the reaction can proceed in the following way. 104

Pd+2D

[Pd;D]n

.13

C

93

Nb +7.820 MeV.

According to the laws of momentum and energy conservation, the formed nuclide 13 C should receive the energy of 6.8609 MeV. The nuclide 93 Nb should receive the energy of 0.959 MeV. The nuclear excited state (nuclear isomer) with the energy of 6.864 MeV and excited level width of 6 keV exists for 1 3 C. The excited level with the energy of 0.94983 MeV exists for 93 Nb. The difference between the energy received by nuclide 13 C and the energy of one of the excited nucleus equals to 3.f keV. At the excitation energy of the crystalline lattice of 1.5 keV, and width of the excited energy level of 6.0 keV, these conditions resulted in a high probability for occurrence of the long-range (resonant) nuclear reaction. 105

Pd + 2 2 D - • [Pd2D]* -^ 9 3 Rh + b Li + 11.794 MeV.

According to the laws of momentum and energy conservation, the formed nuclide Li should receive the energy of 8.880 MeV. The nuclide 93 Nb should receive the energy of 0.959 MeV. The nuclear excited state (nuclear isomer) with the energy of 6.864 MeV and excited level width of 6 keV exists for 1 3 C. The excited level with the energy of 0.94983 MeV exists for 93 Nb. The difference between the energy received by nuclide 13 C and the energy of one of the excited nucleus equals to 3.1 keV. 6

. = 7820 keV

11794keV

5a

~

HiLi*ex.lev. 6Lin.r

fc

13Cn.r

r^j I >

3.1

CD

n Ul

^

<

O CD

CD CD

[PdD]*

Nb stable

• >

CD O

+

686

rt

1 93

I

5/2

CD

ev.

13

'

C stable

[Pd2D]*

103

Rh stable

6

Li stable

Figure 11. Assumed plan of carrying out long-ranged (resonant) nuclear reactions, (a) for Pd D transmutation reaction and (b) for Pd + 2D transmutation reaction.

The totality of the experimental results allows to assume that the energy of the excited nuclear levels of the formed nuclides converts into heat. The specific physical mechanism of such conversion requires additional research.

230

7.

Conclusions

T h e results obtained (the glow discharge device producing the excess heat power up to 5 W / c m 2 at an efficiency up to 150%) allow the development of a demonstration source of heat power. The technology for development of multi-element cathode fuel elements with plasma anodes has been worked out. The development of new nuclear engineering is possible based on non-equilibrium nuclear t r a n s m u t a t i o n reactions in the solid-state medium. This type of engineering can be called "Third way" in nuclear engineering in comparison with the nuclear engineering based on uranium nuclear fission, and thermonuclear synthesis.

References 1. A.B. Karabut, Ya.R. Kucherov, and I.V. Savvanimova, Nuclear product ratio for glow discharge in deuterium, Phys. Lett. A, 170, 265, 1992. 2. Richard B. Firestone, Table of Isotopes, 8th Edition, Vols. 1 and 2, Appendix G - 1 , John Wiley & Sons, Inc., New York, 1996.

I N F L U E N C E OF P A R A M E T E R S OF T H E GLOW D I S C H A R G E ON C H A N G E OF S T R U C T U R E A N D T H E ISOTOPE COMPOSITION OF THE CATHODE MATERIALS

L B . SAVVATIMOVA A N D D.V. G A V R I T E N K O V Federal State Unitarian Enterprise Scientific Research Institute "Luch", Zheleznodorozhnaya, 24 Podolsk, Moscow region 142116, Russia E-mail: [email protected]

Results of examinations of changes in structure, element, and isotope composition of cathodes after the glow discharge exposure in hydrogen, deuterium, argon, and xenon are submitted. The voltage of the discharge was less than 1000 V and the current was 5-150 mA. Samples before and after ions bombardment in the glow discharge were explored by the methods of mass spectrometry: the secondary ions (SIMS), the secondary ions with additional ionization of neutral sprayed particles (SNMS), spark (SMS), and thermo-ionization (TIMS), and also methods of energy dispersion X-ray spectral analysis (EDX). The alpha-, beta-, gamma- emission, and gamma- spectrometry for radioactive uranium specimens were also carried out before and after experiments in the glow discharge. Changes in structure, isotope, and element composition of the cathode samples depend on current density, integrated ions flow (fiuence of ions), kind of irradiating ions and other experimental conditions. Attempts are made to estimate qualitatively and quantitatively the role of each of the parameters on intensity of the observed changes in cathode composition. It is shown that the maximum changes in structure, chemical and isotope composition of the cathode material occur in "hot points," such as craters from microexplosions, phase segregations, blisters and other new formations. Various methods of the analysis revealed that the basic elements Mg, O, Si, Al, and Ca with quantities up to per cents and more were prevailing in these zones and not found out before experiment. The greatest changes of the isotope relations were observed for iron, calcium, silicon, chromium after experiments with pulsing current. EDX method finds out the elements missing in the samples before experiment such as cadmium, strontium, tin. The isotopes with mass number 59 (Co 100%), 55 (Mn 100%), 45 (Sc 100%) are also not found in initial samples and background measurement by TIMS method. Results of changes in the element and isotope composition, which are found by various methods of the analysis, are compared with possible reactions of fusion-fission. It is noted that under different experimental conditions on various cathode materials similar groups of prevailing elements are find by various methods of the analysis.

1. Introduction As is known, the ionic processing of materials results in changing surface properties. It has been shown earlier that physical-mechanical properties, element, and isotope compositions in plasma of a glow discharge change. 1_9 The majority of the "additional" elements found after ion irradiation and not found before irradiation is distributed at the boundaries of grains 1 and in 231

232

local spots. 3 ' 4,9 They make up from the 10th fractions of a percent up to several percents. Thus in initial samples the content of separate impurity elements did not exceed 10~ 3 -10~ 4 at.% and EDX analysis could not reveal it. Groups of such elements as Sc, Ti, V, Ag, Cd, In, P, CI, Br, Ge, As, Kr, Sr, Y, Ru, and Xe have been found in Pd after irradiation by ions of all the types (D, H, Ar, and Ar+Xe), but in various quantities. 2 Elements with atom numbers Z = 26-31 (Fe, Cu, Zn, and Ga) were observed by the method of energy-dispersion X-ray spectral analysis (EDX) preferentially after irradiation by deuterium ions. As a result of EDX and radiography, it was supposed that nuclear transmutations occur more intensively on local sites. 1 - 4 Distinctions in the characteristic spectrums corresponding to various combinations confirmed the nuclear processes in local zones. 3 ' 9 Considerable changes of the isotope relations were observed for 10 B / n B , 1 2 C/ 1 3 C, 6 0 Ni/ 6 1 Ni/ 6 2 , 4 0 Ca/ 4 4 Ca, and 9 0 Zr/ 9 1 Zr. 3 Change of the isotope relation in i 09 / 107 Ag from 3/1 up to 9/1 was observed in different series of experiments. 3 ' 9 In this paper, the changes of structure, element, and isotope composition of palladium for various parameters of the discharge are compared. The role of the current sort in transmutation intensity is shown. The possible types of nuclear reactions for pairs of the elements observed in the cathodes after experiments are shown. 2. Methods of the Analysis and Parameters of Glow Discharge The installation had a vacuum discharge chamber with a cathode and an anode. The chamber was evacuated up to 10~ 2 Torr, and then it was filled by working gas up to 3 10 Torr. Deuterium, hydrogen, argon, and xenon were used as working gases. Samples were irradiated by currents with density of ~10-50mA/cm 2 and at discharge voltage of 50-1200 V. The discharge burning exposure was 1-40 h, diameter of samples ~20mm, thickness ^100 /xm, the irradiated area - about 1 cm 2 . Multilayer cathodes consisting of several foils approximately 100 /jm thick each for acquisition of data on change of the element and isotope composition on depth were used. The examinations procedure in detail is described in Refs. 3 and 9. The measurement system allowed recording current, discharge voltage, gas pressure, sample temperature, temperature of the inlet, output of the cooling water in the cathode, anode, and cooling jacket. Changes in the element and isotope composition were analyzed by EDX methods and mass spectrometry. The element composition of the cathode materials was studied on scanning electronic microscope Hitachi S-840 with Link Analytical LS - 5 for a spectral analysis, later the structure of the surface and the sample composition were studied by electronic microscope JEOL JSM 6460-LV using INCA for X-ray spectral analysis. The content of elements was estimated using programs INCA (Version 4.02). Time of the spectra recording is 2 min. The accelerating voltage of 10 kV for the analysis of lighter elements and 30 kV for heavier elements were used. The analyzed zone size was about 1 /im 2 for the probe analysis in point, and when scanning on the area it was up to ^250 x 200 /im 2 . Sensitivity of the method

233

was ~ 1 0 - 2 atom.%. Depth of an analyzed layer made up about 1 /xk. Elements 0 , F, S, Na, Mg, Al, Ti, Cr, and Fe are analyzed on Ka, Mo and Br - on La, W - on Ma of characteristic spectrums lines. Concentration of the ("additional") impurity elements was determined using the majority of main lines of the characteristic X-ray spectrum. Initial samples and samples after experiments in deuterium glow discharge are analyzed. Places with structural defects and new formations such as swellings (blisters), craters, areas of micromeltings, needle structures, and sites of surface without special changes after irradiation in glow discharge plasma were explored. The isotope composition of the samples at high temperature was determined by the method of the thermo-ionization mass spectrometry on mass spectrometer "Finnigan"-262. The sample temperature in this analysis usually exceeded 1800°C. The majority of complex compounds should break up (dissociate) at such a temperature while the secondary ionic mass spectrometry can give many composite complexes. 3. Changes in Structure of Surface, Element, and Isotope Composition It is shown that changes of structure, element, and isotope composition depend on the following: (a) (b) (c) (d) (e)

Doses of irradiating ions (Tables 1-3).1 Density of ions current (Tables 4 and 5). 3 ' 4 Irradiating ions kind (Tables 4 and 5). 3 ^ 5 Current sorts: direct or pulsing (Tables 6, 12, and 13). Places of "hot points" analysis and new formation (Tables 8-12).

Each of the above process parameters (a-d) influenced on the process intensity and its reproducibility. The role of "hot points" in the change of structure, chemical, and isotope composition3-"5 and the groups of the elements dominating in these "active sites" are analyzed by various methods. 1 ' 2 ' 5 In this paper special attention is paid to structural change in new formations (in zones of craters, growth formations, and blisters) and to the effect of current (direct and pulsing). 3.1. Dependence

of "Additional"

Elements

Quantity

on Dose

Changes of the isotope and element composition of the samples irradiated by deuterium ions after different exposure time (dose) were analyzed by several methods. Table 1 comprised the data received by method of secondary ionic mass spectrometry after 30 min bombarding of palladium by deuterium. Table 2 includes the results of EDX data, and Table 3 has the same samples data obtained by method of spark mass spectrometry. The increase in the content of Li (Table 1) by a factor of 50-450 (rows 1 and 2), n B by a factor of 70 (row 4) can be a result of nuclear process under conditions

234

of low-energy actions in glow discharge plasma with the participation, for example, of hydrogen or deuterium, or processes of heavier elements fission. The increase in the content of Zr by a factor of <~570-340 (rows 15 and 16), V by a factor of 100 (row 5), Cr by a factor of 160 (row 6), Fe by a factor of 2-4 (rows 8 and 9), and Ni - 5-30 (rows 10 and 11) can also be a result of nuclear transmutations. The experimental time of this series was ~30min. The increase of the impurity elements at the backside was observed only for Li. "Dot" aggregations of Zn, Co, Br, and Mg located preferentially on boundaries of subgrains, with a density of ~ ( 1 - I 0 ) x l 0 6 cm~ 2 (for Zn the density of such places made up ~ ( l - 2 ) xlO 6 cm" 2 , for B r ^ ( 2 - 4 ) x l 0 6 c m - 2 ) 1 are found during scanning the surface of a sample. The comparison of the new elements quantity shows that an increase in experimental time (fiuence) by a factor of 10 times (data EDX) leads only to an increase in Mo which is an element of construction (the a pressure holder of the sample, screening a part of surface during sample irradiation). Therefore, it is not surprising that irradiation time increase leads to Mo quantity increase. The quantity of other "additional" elements (Br, Sr, and Te which are absent in the sample before experiment) does not change largely with an increase of experimental time (a dose of irradiation) by a factor of 10. The reason for such an effect can be both preferred formation of these elements in the sample at the initial stage of the discharge burning, having significant quantity of Table 1. Changes of isotope and element composition of impurity atoms on surface of palladium after bombarding by deuterium ions (SIMS). 3 No.

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16

Mass number

6 7 10 11 51 53 54 56 57 60 61 63 87 88 90 91

Element

Li* Li* B* B* V* Cr Fe, Cr Fe Fe Ni Ni Cu Sr* Sr* Zr* Zr*

Content (arb. un.) After experiment

Before experiment

Irradiated side

Back side

0.02 0.02 0.01 0.10 0.30 0.60 2.20 22.20 11.00 0.10 0.20 1.40 0.10 0.50 <0.10 <0.10

1.00 9.00 0.01 7.00 30.00 96.00 15.00 55.00 45.00 3.00 10.00 60.00 1.00 0.10 57.00 34.00

0.15 0.28 0.01 0.01 0.20 1.00 2.00 20.00 12.00 0.20 0.20 1.00 0.10 0.20 0.00 0.10

Thickness of the samples ~ 100 jira. Depth of analyzed layer was ~ 100 A. Method of the analysis secondary ionic mass spectrometry. Li, B, V, Sr, and Zr were not present at the discharge chamber earlier. The source of possible impurity is absent.

235

different defects on its surface and possible preferable sputtering of lighter elements at the following experimental stage. Another reason for the absence of growth of the "additional" elements quantity with an increase in discharge burning time can be participation of the forming elements in the secondary reactions. It is impossible to exclude the contribution of irradiated surface screening by sputtered. However, the analysis of the same samples by spark mass spectrometry method does not confirm the explanation of the results obtained by the surface screening by molybdenum precipitation because an increase of other elements such as 7 Li, n B , K, Rb, In, and Nb in a longer experiment was observed both on irradiated and on the backside of the same sample. Table 2. No.

1 2 3 4 5 6 7 8 9 10 11

Additional atoms on palladium surface after glow discharge in deuterium (EDX). 1 The additional atoms

Na Mg Al Si**

Ca Ti* Br* Sr* Y* Mo** Tc*

The nuclear number

11 12 13 14 20 22 35 38 39 42 43

Dependence of quantity of impurities on duration of experiment ( x l C T 2 at. %) 4h

40 h

7.0 ± 0.3 1.0 ± 0.3 4.0 ± 0.3 1.5 ± 0.3 4.0 ± 0.3 1.0 ± 0.3 3.0 ± 0.6 7.0 ± 0.6 40.0 ± 1.0 15.0 ± 1.0 20.0 ± 1.0

3.0 ± 0.3 2.0 ± 0.3 2.0 ± 0.3 < 0.3 3.0 ± 0.3 1.5 ± 0.3 2.0 ± 0.6 6.0 ± 0.6 20.0 ± 1.0 40.0 ± 1.0 10.0 ± 1.0

*Source of possible pollution is absent. **Source of possible pollution is the parts of the construction. Sonde diameter was 1 /im. EDX method used SEM "HITACHI-800" with "Link Analytical" device. All the peaks corresponding to Ti, Br, Sr, Y, and Tc on X-ray spectrums were observed after experiments. Ti, Br, Sr, Y, and Tc were never present in the discharge chamber before experiment. Ti, Br, Sr, Y, Tc, Zn, and Co are absent before experiments in spectrums of this Pd.

A 500-3000-fold increase in Zr content (rows 20 and 21) can be a result of possible nuclear processes under low-energy actions in glow discharge plasma. One can assume that a 10-20-fold increase in Indium content (series 28) can also be an effect of stimulated nuclear processes with the participation of palladium and, for example, hydrogen, deuterium, or boron (mass numbers 10, 11). The assumption of preferred sputtering of light elements forming during experiment can confirm the data of Table 3 obtained by SMS method. One can see an increase in 10 B content by a factor of 2 on the sample backside with 4-hour irradiation and an increase in n B by a factor of 10 on the sample backside after 40-h experiment, and only by a factor of ~ 3 on the irradiated side of samples (40 h). Increasing Al, 115 In, and 93 Nb correlate with an increase of the discharge time both on the irradiated and on

236

backside of the sample. Similar changes are also observed for 90 Zr isotope on the surface irradiated by palladium ions where the increase is ^500 times after 4-hour discharges and 1200 times for 40 h. On the backside, the quantity of 90 Zr increases by a factor of ~4.4. The quantity of 91 Zr isotope increases ~1000 and ^1200 times with a 10-fold increase in discharge time. The 80 Se increasing was ~100 times on

Table 3. Quantity of the impurity atoms on palladium surface after deuterium ions irradiation at glow discharge (SMS). 1 No.

Mass number

Element

Content before ( x l 0 — 4 at. %) (X100 ppm)

Additional element content in Pd for different experiment duration ( x l O - 4 at. %) 4h Upper

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28

6 7 10 11 23 27 28 29 30 32 39 41 47 48 49 50 78 80 85 90 91 93 98 100 103 107 109 115

Li Li B B Na Al Si** Si** Si** S K K Ti* Ti* Ti* Ti* Se* Se* Rb* Zr* Zr* Nb* Mo** Mo** Rh* Ag* Ag* In*

0.06 0.06 0.07 0.07 0.44 6.00 9.00 7.00 6.00 7.00 3.00 3.00 1.20 1.40 1.30 1.70 0.23 0.30 < 0.03 < 0.05 < 0.05 < 2.00 0.40 1.80 7.00 1.00 1.00 <0.04

0.15 0.33 0.30 4.40 96.00 18.00 21.00 18.00 14.00 9.00 12.00 1.80 580.00 680.00

40 h Lower

0.40 0.15 0.20 1.00 10.00 9.00 11.00 4.50 2.00

0.23 0.20 0.01 25.00 50.00 40.00

1.00 60.00 2.50 3.25 3.40 0.20 0.20 0.05 0.05 0.05 2.00

4500.00 21.00 63.00 50.00 0.48

1.80 21.00 3.00 1.50 0.04

Upper

Lower

0.90

0.50

0.20 2.00 300.00

0.70 6.00 25.00 3.00 10.00 66.00 2.00 4.50 9.00

15.00 3.50 12.00 18.00

130.00 130.00 0.20 0.20 90.00 60.00 61.00 7200.00 2880.00 25.00 1.00 0.80

3.50 2.60 4.00 33.00 51.00 0.22 4.00 3.00 7.00 3.20 2.50 0.16

*Possible source of impurity is absent. **Possible source of Mo and Si impurities are construction parts. Depth of analyzed layer ~ 10 (im. Sensitivity of the method is 10 —4 at. % ( l p p m ) . The quantity of each isotope is brought to 100 %. Ti, Se, and Ru, In were not present before discharge experiments. The "Upper" sample was irradiated by ions and contacted with deuterium plasma. "Lower" sample was not irradiated by deuterium ions and did not contact deuterium plasma.

237

backside for 40-hour experiment. Authors could not explain a significant increase in n B , 115 In, 93 Nb, 80 Se II 91 Zr on the backside of the sample by other non-nuclear processes. 3.2. Dependence of Quantity of "Additional" Density and Ions Kind

Elements

on

Current

Current density (ions flow) and ions type are also important parameters. The quantity of the impurity elements formation in the cathode material after discharge experiments depends on them. The data of other series experiments for quantities of Ag in Pd at various density of ions flow with different ion content are shown in Tables 4 and 6. Table 4. Sample number

Current (mA)

Change of quantity of Ag in Pd glow-discharge cathode (SMS) 4 Ions type

Ag+ 2 (ppm)

Analyze place*

Increasing (times)

Isotope mass 107 Initial

0

1666

35

1667**

35

109 1

D2

1668

25

H2D2

1670

25

H2

1671

25

D2

1.7 x 10 3 5j) x 10 3 2.1 x 10 <1.5 x 10 1 1.1 x 10 2 <2.0 x 10 1 <2.0 x 10 1 5/7x 10 2 2 M x 10 2 10 1.2 x 2 9/7 x 102 10 4.5 x 10 3 2.6 x 2 10 1.8 x

2.2 x 10 1 5.2 x 10 3 2J2 x 10 3 < 5 7.7 x 10 1 <2.0 x 10 1 <2.0 x 10 1 5Ji x 10 2 7 4 x 10 2 1.3 x 10 2 l O x 10 3 4.5 x 10 2 2 7 x 10 3 1.9 x 10 2

-2.5 x 10 2 -1.0 x 10 2 -4.0

-2.5 x 10 1 - 3.5 x 10 1 - 5.0 - 5.0 x 10 1 -2.0 x 10 1 -1.2 x 10 2 -9.0

*1, 2, 3 depth of analyzed layer is 10 /jm: (1, 2) the upper irradiated sample; (3) unirradiated lower sample. **1668 - discharge in hydrogen, and then in deuterium. ppm: impurities particles per million.

One can see that the maximal Ag increase after deuterium discharge at greater density of current (35 mA) in the near-surface layer of 10 um was 250 times (from 20 ppm in an initial state up to 5000 ppm after irradiation by deuterium). The following layer ~10 um thick only showed ~ a 100-fold Ag increase. A lower increase (~120 times) of Ag content was observed at smaller current density (25 mA). A less increase was observed in hydrogen at greater current density. It can be explained by easier output of hydrogen implanted into palladium lattice at a higher temperature of the sample (and accordingly by a smaller hydrogen content in palladium lattice), i.e. by closely related velocities of hydrogen implantation

238

and hydrogen desorption under these conditions. An essential increase of Ag content in the lower sample (~4 times) was observed only for the sample preliminarily irradiated by hydrogen and then by deuterium. This might be a result of simultaneous running of both non-nuclear (sputtering, diffusion separation) and nuclear processes (fusion and fission, secondary interaction of nuclear reactions products). Table 5 shows experimental data on B, Ni, and Zr. An increase of boron, nickel and zirconium isotopes was observed only at irradiation by deuterium and preferentially in the near-surface layer. Table 5. Sample number

Change of In, Ni, and Zr quantity in Pd cathode at deuterium discharge (SMS). Current (mA)

Gas

Isotope ( x l O - 4 at. % (ppm))

Analyzed layer B

Initial

0

1666

35

D2

25

3.3. Dependence

D2

Zr

10*

11

58

60

61

62

90

91

1 1

<2.7 21

<0.4 19

10 280

<5.5 300

<40 480

<14 500

<1 25

5 16

2

<2 <2.8

<2.5 <1,8

60 26

69 17

<52 <36

75 <15

8,5 <1

5 <2,4

25 <1.5

22 1.1

190 31

180 28

560 <80

660 <25

30 0.9

31 <5

3 1671

Ni

I

of Change in Pd Composition

on Current

Type

3.3.1. Change of the isotope and element composition of Pd sample under direct current discharge (TIMS) Isotope and element composition change for two different Pd samples (Table 6) arranged one above the other are given as an example, and the difference in isotopes ratio in them is shown. Light elements remains in the lower sample screened from direct ions irradiation. So, Al was found to be 10 times more in lower sample, Mg was also observed to be 4 times more in the lower sample, 29 mass (Si) was observed in the lower sample too. But 22 Ne (9.25%) isotope was observed in the upper Pd foil while 20 Ne (90.48%) was practically never observed. The absence of the isotope with maximum abundance is observed for 1 6 0 and 14 N while 1 8 0 and 15 N were very often observed. The following features in the isotope composition of the upper sample irradiated and the lower sample screened were observed: • Absence of isotopes correlation in Ca and Ti with the natural abundance. • Sc in the irradiated sample - 1200 counts per second (cps) in the lower one - 95 (cps). Sc was not available in the initial sample and the background analysis.

239

Cr and Fe were not available in the discharge chamber parts (water-cooled stainless steel holder was placed under eight Pd foils 100 //m thick each and one molybdenum foil 0.1 mm thick). Cobalt and manganese have not also been found in initial Pd and in background measurement. Cr, Fe, Co, and Mn were observed in the second sample in smaller quantities. Therefore, Mn intensity in the upper sample was 4000 cps and only ~30 cps in the lower Pd sample. Cobalt quantity was found to be ~380 cps in the upper sample and 20 cps in the lower sample, 52 Cr was ~10000 and ~3400 cps, respectively. Only 44 Ca, 24 Mg, and Al were found to be in bigger quantities in lower Pd sample as compared with the upper sample.

Table 6. Isotope and element composition of Pd samples irradiated by deuterium ions under direct current discharge (TIMS). Mass

Element

14 15 16 18 22 24 25 26 27 28 29 30 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59

N O Ne Mg

Al Si

Ca

Sc Ti

Natural abundance (%)

N\ CPS, 1610(1)

N2 CPS, 1610(2)

-

90.6

-

0.37

2.0 x 101

99.8

-

0.20

1.0 x 101

9.32

6.0 x 101 1

78.99

1.0 x 10

10 11 100

-

-2.0 x 101

-1.0 x 101 +2.8 x 101 +1.0 x 101

-

1.0 x 103 2

92.23

2.5 x 10

4.68 3.09

-

0.65

1.8 x 103

0.14

4.3 x 103

2.09

1.0 x 101

100 8.0 7.3

1.2 x 103 5.0 x 101 3.0 x 101

5.5

1.2 x 102 1.0 x 101

Ti, Cr

5.4; 4.3

4.6 x 102

V Cr Cr

99.8

4.6 x 102

83.8

1.0 x 104

9.5

7.0 x 102

Fe,Cr

5.8; 2.37

2.0 x 103

Mn Fe Fe Fe Co

100

4.0 x 103

91.7

1.5 x 104

2.2

1.5 x 103

73.8

1.0 x 101 3.8 x 101 1.0 x 101

A (A^-Ni)

0.28

3.8 x 102

100

3.8 x 102

1.0 x 104 1.0 x 102 1,5 x 102 3.0 x 101 1.5 x 102 1,5 x 102 6 x 102 9.5 x 101 6.5 x 101 5.5 x 101 4.0 x 102 4.5 x 101 2.0 x 102 5.0 x 102 3.4 x 103 3.0 x 102 2,6 x 102 3.0 x 101 2.5 x 103 5.5 x 101 3.0 x 101 2.0 x 101

+9.0 x 103 -2.4 x 102 +1.5 x 102 +3.0 x 101 -1.65 x 103 -4.15 x 103 +5.9 x 102 -1.1 x 103 +1.5 x 101 +2.5 x 101 +2.8 x 102 +3.5 x 101 -2.6 x 102 +4.0 x 101 -6.6 x 103 -4.0 x 102 -1.7 x 103 -3.0 x 103 -1.2 x 104 -1.4 x 103 -3.5 x 102 -3.6 x 102

1610(1)—irradiated sample (JVi); 1610 (2)—screened sample located under irradiated sample (N2)

240

A change of the isotope ratio in samples after carrying out deuterium bombardment was observed from several percent up to hundreds. 1,2 The quantities of "additional" elements were from 0.1 at.% up to ~ 5 at.%. The most considerable difference in the isotope ratio was observed for Mg, Si, K, S, Ca, and Fe isotopes after deuterium discharge. A comparison of the chemical composition and isotope ratio on palladium samples after experiments in deuterium discharge with direct current and pulsing current by thermo-ionization mass spectrometry is shown in Tables 7-10. One can see from Table 8 that the quantity of Mg (24-26) and Si (28-30) isotopes in the lower layers of the sample are higher; therefore it is impossible to explain this fact by "impurity" from the surface.

Table 7.

Change of Fe, Cr, and Ti isotope ratio with direct current by TIMS (No. 1610).

Sample number*

Element

Isotopes

Natural abundance (Nn)

Ratio after experiment (Nexp)

j^**

1 2

Fe

56/57

91.72/2.2 = 41.7

1.5 x 10 4 /1.5 x 10 3 = 10 2.5xl03/5.5xl01 =46.4

4.17 0.90

1 2

Cr

52/53

83.8/9.25 = 8.8

1 . 0 x l 0 4 / 7 . 0 x l 0 2 = 14.3 3400/3.0 x 10 2 = 11.3

0.62 0.78

1 2

Ti

48/47

7 3 . 8 / 7 . 3 = 10.12

1.2 x 10 2 /3.0 x 10 1 = 4 4 . 0 x l 0 2 / 5 . 5 x l 0 1 = 7.3

2.50 1.40

1 2

Ti

48/46

73.8/8 = 9.82

1 . 2 x l 0 2 / 5 . 0 x l 0 1 = 2.4 4 . 0 x l 0 2 / 6 . 5 x l 0 ] = 6.15

3.80 1.50

1 2

Ti

48/49

73.8/13.42 = 13.42

1.2 x 10V10 1 = 12 4.0xl02/4.5xl01 =8.9

1.10 1.50

*(1) An irradiated sample, (2) the sample located under irradiated one. ** K = Nn/Nexp: natural ratio/ratio after experiments.

3.3.2. Change of isotope and element composition in palladium at deuterium discharge under pulsing current These results (Tables 9 and 10) apply to the experiments with pulsing current frequency of ~ 1.35 x 10 3 Hz, pulse length duration of 70 ^s and a weak magnetic (magnetic field was ~ 4 T). Average current is ~ 10-15 mA, current in an impulse is ~ 100-150 mA. A very essential increase (1000 times) of the isotopes ratio in pulsing current experiments essentially for isotopes of iron takes place. The contribution of heavy isotopes for such elements as Ni (~ 11-16 times) and Cr (~ 8 times) also decreases. For Ti and Ba the contribution of a heavier isotope increases 2-3 times. It is important to note that changes in ratios of lead (1 ± 0.1) and gallium (1.5 ± 0.1) isotopes after the experiments are not practically observed.

Table 8. Mass number

Element

Change of Fe, Cr, and Ti isotope ratio with direct current by TIMS (No. 1694).

Natural abundance

exp

Before

(%)

(cps*)

After exper. (cps)

Natural isotope ratio

(Nn) 1 24 25 26 28 29 30 40 42 43 44 45 46 47 48 56 57 59

2 Mg

3 78.99

10 11 Si

92.23 4.67

3.1 Ca

0 0 0 0 0 0

96.86

0.6 0.15

Sc Ti

4

2.0 100 8 7.3

3 x 103 2 x 102 1 X 103

0 65 95

Fe

73.8 91.7

1 X 103 2.8;<10 3

Co

2.2 100

50 0

5

6 2

50/8 X 10 0/67 0/38 1 x 10 2 / > 1 x 10 2 6.3 x 102/1 x 103 2.2 x 102/5 x 102 1 x 10 6 2 x 10 B ~ 4 x 10 3 ~ 5 x 10 3 2 x 10 2 1.3 x 10 3

Isotopes ratio after exp. (A exp .)

K

A (cps)

7

8

9

24/25 25/26 24/26 28/29

~ ~ ~ ~

8 1 8 20

24/25 25/26 24/26 28/29

~ ~ ~

28/30 40/44 44/42 44/42

~ ~ ~ -

30 50 3 13.3

28/30 40/44 44/42 44/42

~ ~ ~ ~

48/46 ~ 6.2

12

~0.7

+ 8 x 10 2

1/0.5 1/0.5 0.16

~2 ~8

+67 +38

1 x 10 2

0.5 5

~60 ~10

+ 1 x 10 2 + 1 x 10 3 + 5 x 10 2

2.5 x 1 0 ~ 2 1.25

1,2 x 10 2 ~10.6

48/46 ~ 5.46

~1.14

0 7 x 10 3 4.5 x 10 3 2.5 x 10 2 1.5 x 10 3

+1,97 x 10 6 +3,8 x 10 2 + 4 x 10 3 + 2 x 10 2 +1235

-95 56/57 ~ 41.7

*cps: counts per second. **A, cps: difference of counts per second after and before for the columns 5 and 4. K: factor of change in natural isotopes ratio to isotopes ratio after experiment (Nn/Nexp). Column 5: data of the second scanning of the same sample are through dash.

56/57 ~ 18

-2.3

+ 6 x 10 3 +1.7 x 10 3 + 2 x 10 2 + 1.5 x 10 3

242 Table 9. Change of isotope and element composition in palladium at deuterium discharge under pulsing current (TIMS, # 1799). Element

Ne

Ni Ni Fe Cr Ti Ga Ba

Pb

3.4. "Additional" Analysis

Mass number

20 21 22 58 60 61 62 56 57 52 53 48 47 69 71 138 137 136 135 134 206 207 208

Elements

Quantity

Natural abundance

(%)

After experiment (cps)

90,5 0,27 9,32 68.1 26.2 1.25 3.6 91.7 2.2 83.8 9.5 73.8 8 60 40 71.7 11.3 7.85 6.6 2.4 23.6 22.6 52.3

2.0 3.0 5.0 1.5 6.5 3.0 1.3 1.6 4.0 4.8 4.5 2.0 1.0 3.0 1.8 3.0 1.9 1.2 2.2 2.5 4.0 4.8 1.0

on Different

x x x x x x x x x x x x x x x x x x x x x x x

10 1 10 1 10 1 10 2 10 2 10 1 10 2 10 2 10 3 10 2 10 2 10 2 10 1 10 2 10 2 10 3 10 2 10 2 10 2 10 2 10 1 10 1 10 2

Methods

of

One can see that most essential changes of the element composition in rather considerable areas of surfaces and in the local microzones characterized by some different structural changes (Table 11 with EDX data and Figs. 1-4) were observed. TIMS method can show very thin changes in the surface layers, but these measurements will concern all areas of the analysis. If we carried out spark mass spectrometry analyses, we found considerably smaller quantities, about 10~ 4 atomic percent. However, the analyzed layer depth was ~10 /iin. Therefore, the depth of X-ray spectral analysis is ^10 times less, and the depth of TIMS analysis is ~100 times less than for SMS. Taking into account the analysis depth of spark mass spectrometry and correlate it with TIMS data and (or) EDX method, it is possible to assume that TIMS data in the thin surface layer was also ~ 0.1-0.6 at. %. Thus, each method of the surface analysis is important and should be taken into account. Therefore, the analysis of the samples before and after experiments was carried out, at least, by two different methods (e.g., EDX and TIMS).

243 Table 10. Isotope ratio change in 'additional" elements of Pd sample after pulsing current experiment. Element

Isotopes

Natural isotopes ratio (Nn)

Ratio after experiment

Si

28/29 28/30 20/21 20/22 58/60 58/61 58/62 56/57 52/53 48/47 138/137 138/136 138/135 138/134 208/207 208/206

93.2/4.7 = 22.6 93.2/3.1 = 29.8 90.5/0.27 = 33.5 90.5/9.32 = 9.7 68.1/26.2 = 2.6 68.1/1.25 = 55 6 8 . 1 / 3 . 6 = 19 91.2/2.2 = 41.45 83.8/9.5 = 8.82 73.8/8 = ~ 9 71.7/11.3 = 6.35 71.7/7.85 = 9.13 71.7/6.6 = 10.8 71.7/2.4 = 29.8 52.3/22.6=2.31 52.3/23.6 = 2.22

10/75 = 0.13 10/20 = 0.5 20/30 = 0.67 20/50 = 0.4 1.5 x 10 2 /6.5 x 10 2 = 0 . 2 3 1.5 x 10 2 /3 x 10 1 = 5 1.5 x 10 2 /1.3 x 10 2 = 1.15 1.6 x 10 2 /4 x 10 3 = 0.04 4.8 x 10 2 /4.5 x 10 2 = 1.066 2 x 10 2 /10 = 20 3 x 10 3 /1.9 x 10 2 = 15.8 3 x 10 3 /120 = 25 3 x 10 3 /2.2 x 10 2 = 13.63 3 x 10 3 /2.5 x 10 2 = 12 1 x 10 2 /48 = 2.0 1 x 10 2 /40 = 2.5

Ne Ni

Fe Cr Ti Ba

Pb

(Nexp)

K**\ A factor of change in natural isotopes ratio to isotopes ratio after experiment

j{**

1.7 6.0 5.0 2.4 1.1 1.1 1.6 1.0 8.0 5.0 4.0 3.6 8.0 2.5 1.1 9.0

x x x x x x x x x x x x x x x x

10 2 10 1 10 1 10 1 10 1 10 1 10 1 10 3 10 1 10"1 10"1 lO"1 10-1 10 1 10° 10"1

(N„/Ncxp).

The "geometric" factor shows the influence of boundary conditions (Fig. 3a and b). The maximal surface change was observed at the interfaces between radiated and unirradiated (screened) areas. The screened areas had the insignificant change in topological structure and chemical structure. Table 11. Dependence main elements on palladium surface for various methods of analysis of the same sample. Element

Atomic % (EDX)*

TIMS (cps)**

Mg Fe Al Ga O Ca

3.1 ± 0.2 6 ± 0.2 3.7 ± 0.2 2.4 ± 0.4 50 ± 1.5 2.7 ± 0.3

-

Ti

4.3 ± 0.3

-

~ 5.0xl03±2.5xl02 ~9.0xl05±2.5xl03 ~ 7.0xl03±2.5xl02

-

~ 2.2 x 1 0 3 ± 1 x 10 2 (42, 43, 44 isotopes)

* The volume of analysis by X-ray spectral method (EDX) on electronic microscope JEOL JSM ~ I/un . ** TIMS: thermo-ionization method; cps: impulses (ions) per second in the sample after experiment minus the account in the initial sample. Using TIMS method, analyzed a Pd strip 1-2 mm thick and 20 mm in length, including a zone under the screen. The field volatilizes tens of angstrom unit from the sample surface during the analysis.

244

* **

Fig. 1. Blisters on Pd surface after 22-hour deuterium discharge exposure. Marks on the figure are 10, 50 and 100/mi, respectively.

'^pp*

„ \

4

a. Needle formations on the boundary

b. Broken cocoon.

c. Micro explosion "crater"

Fig. 2. New formations on Pd surface after deuterium bombardment. Marks on the figure are 10, 20 and 20/xm, respectively.

As can see in Table 13, the composition (in quantity and element content) of each element in the 1 /im-diameter point do not coincide (do not equal) with all analyzed Fig. 4a area 250 x 200/mi 2 . The sample (1610/2) is one upper in eight foils-multilayer sample in this experiment. Upper sample was partly melted during experiment. However, heat balance was not estimated in this experiment. The separate elements content, analyzed of 1610/2 area ~ 300x220 /im 2 , with elements content on the 1/xm diameter area were compared. Data of Table 13 showed same difference in additional elements content and close values for main elements for homogenious place of the surface.

a. of radiated and unirradiated areas

b. radiated area on the left

Fig. 3. New formations on the boundary (a) of radiated and unirradiated areas (b) radiated area on the left Fig. 4c. The screened area from glow discharge radiation. Marks on the figure are 100 and 500 /zm, respectively.

245 Table 12.

Chemical composit:ion change in new formations areas (Fig. 2c).

Element

Atomic percents Point 1

O Al Mg Si Ti Ga Mo Pd

Point 2

Point 3

Point 4

60.1 ± 1.2 0.5 ± 0.3

2.1 ± 0.9

Point 5

Point 6

21.5 ± 1.2

52.3 ± 1.5 0.8 ± 0.2 1.5 ± 0.5

1.4 ± 0.5 4.3 0.5 1.6 33.1

97.9 ± 0.3

± ± ± ±

0.3 0.4 0.2 0.7

1.7 ± 0.6 3.4 ± 0.6 93.5 ± 0.9

1.6±0.9 4.2±0.8 94.2±0.9

1.5 ± 0.6 2.6 ± 0.5 74.4 ± 1.1

1.1 ± 0.3 40.7 ± 1.0

3.5. Conformity Between Changes in Element Composition Palladium and Structural Changes (Method EDX)

of

The most essential changes of structure are observed with an increasing in discharge time. For example, numerous swellings - blisters (Fig. 1) and various growth

'"

1 ** * *S§%

"r <*+

?

V

\ *V V . - /

%

^ « ^ — *

1

<:V ^\;,

'

>

•

>

^

' *

;

#

^

b.

a.

Fig. 4. (a) Pd surface after deuterium irradiation by dose ~ 8 x 10 2 1 sm" - 2 (Pd # 1610, 30 mA, 400±20 V, P ~ 5 Torr, 4 h in H ^ D . Set included eight foils. Three P d foils were partially melted), (b) Crater on the end of crack on back side of sample, (c) Screening zones. Table 13. Additional elements in Pd after deuterium bombardment (EDX. atomic percent). Element

o Na Mg Al Si Ga Mo Pd W

At. % , Fig. 4a (1610/1) Point 1 (1 jum)

All areas

13.3 ± 0.2

55.9 ± 1.2 1.2 ± 0 .2 0.7 ± 0.1 0.9 ± 0.1 0.4 ± 0.1 0.8 ± 0.1 0.82 ± 0.1 39.13± 0.2

1.4 ± 0.3 1.3 ± 0.2 2.0 ± 0.2 1.2 ± 0.1 80.4 ± 0.4 0.3± 0.05

At. % , (1610/2) Point 1 (1/im)

All areas

1.25 ± 0.3 0.27 ± 0.3 0.49 ± 0.2 2.32 ± 0.25 0.53 ± 0.16 95.0 ± 0.3 0.12 ± 0.1

0.95 0.53 0.25 2.32 0.47 95.36 0.12

± ± ± ± ± ± ±

0.3 0.17 0.1 0.2 0.16 0.25 0.08

246

formations are observed: needle-shaped growth and formations similar to cocoons (Figs. 2 and 3). Especially considerable changes of structure were observed on boundaries of the irradiated and unirradiated areas (Fig. 3). Examples of the structures forming after irradiation by low-energy ions and the element composition in these areas are explored in details (Figs. 3 and 4 and Tables 12 and 14). 4. Discussion: Transmutation Effect Earlier it was shown that the irradiation by ions with energy <1 keV at glow discharge causes complexes of defects (dislocations and their aggregations, pores) depending on type of bombarding ions, temperature of irradiation and fluence of ions. The ions implantation with such energies can occur to depths of no more than several atomic layers. However, the radiation type defects under conditions of stress concentration gradient were formed.14 In this case, the gas atoms are implanted to depths up to several millimeters. In addition, voids in volume of cathode material irradiated with low-energy ions are formed.13 Earlier Matveenko (IAE "Kurchatov Center") showed (applied to the first wall of a thermonuclear reactor) that pressure in the pores under hydrogen ions energy of <1 keV could reach some hundreds of atmospheres. The appearance of new elements absent in the sample and constructive parts of the apparatus before was found in the samples irradiated on glow-discharge cathode. An increase in the quantity of the impurity elements hundreds and thousands of times was revealed. Besides a change in the isotope ratio of elements from tens of percent up to hundreds of times 3 was observed. The analysis of the samples irradiated in glow discharge for more reliable results was carried out by several methods: a mass spectrometry and X-ray microanalysis in several Institutes of the country (including GIRedMet, IPhChAN, Tomsk Polytechnic Institute, "Lutch"). The greatest changes of the isotope and element composition were observed in "hot points": places of microexplosions, craters of plasma microdischarges.9 It is difficult to say what process is primary-microexplosions, microdischarges on structural inhomogeneities, growth formations, and phase inserts; or formation of new elements and phase segregations in places of microexplosions is the result of elements transmutations in the micromelting zones. New elements formation as the result of DD-reactions at the cracks edges with oxide films, so-called accelerating effect, is possible too. It might be the consequence of "overvoltages" incipient on "spikes" formations (cone-shaped or needle-shaped) and resulting in instantaneous micromeltings or microexplosions. In these cases, processes similar to the processes in constructional materials of the nuclear reactors with the formation of micromeltings zones ("thermal" peaks) are possible, too. It is difficult to estimate the priority of these processes. Every possible, the ions concentration gradient and temperature gradient can contribute to the change of cathode structure. Ivanov 11 showed that a formation of pulsing microplasma discharges (unipolar arcs) on structural irregularities (heterogeneities), impurities segregation and oxide films in the surface material layer was possible.

247

Examination of the radioactivity change, the isotope and element composition of the uranium samples (uranium component decrease and thorium component increase by gamma-spectrometry, mass spectrometry and EDX) in glow discharge showed the opportunity of stimulation of nuclear transmutations processes under low-energy actions. 7 ' 8 It is impossible to explain the increase of integrated a, /?, 7 uranium emission and the change of ratio of uranium energy peaks and its daughter elements (231>234Th and 234 U) after experiments in glow discharge by impurity pollution from medium (environment) or by some other effects. The maximum quantity of additional elements at glow discharge experiments should be observed under equivalent conditions for heavier ions (e.g., an argon) if "additional" elements appearance is a result of cathode sputtering or redistributions of these elements in volume of the ion irradiated material. These quantities should grow according to masses and ionic radiuses of bombarding ions in the following sequence: a minimum quantity for the hydrogen irradiated samples, a greater quantity—for deuterium irradiated samples, and a maximum quantity for heavyions irradiated samples (argon and xenon), respectively. We observed a maximum quantity of additional elements and their maximum variety at deuterium discharge. Smaller quantities of these elements and a smaller variety of them were observed at hydrogen discharges and minimum of variety for argon and xenon. 2 One can see that the peak effect on characteristic spectrums was for experiments in deuterium. Dependence of additional elements quantity on ions current density and on temperature of process is very significant and ambiguous. In this case, it is difficult to take into account the action of plurality of simultaneously proceeding processes. Probably, both new additional elements formation and preferable sputtering of lighter elements simultaneously occur under low-energy ions irradiation. The accelerated (speeded) surface diffusion, the impurity components segregations near dislocations and other defects are also take place. A series of experiments 4 showed a dependence of the element composition change on current density and working gas composition (medium) (Tables 4 and 5). So, a maximal increase of Ag quantity was observed for the greatest current density of 35 mA/sm 2 (250 times or from 20 up to 5000 ppm). A comparison of the discharge in hydrogen, deuterium and the discharge with preliminary irradiation in hydrogen and then in deuterium showed, that additional quantity of Ag appearance was minimal (up to 200 ppm). The isotope and element composition changes essentially depend on such parameter of process as current sort. The isotope changes obtained by TIMS method for experiments with direct current are given in Tables 7 and 8 and with pulsing current in Tables 9 and 10. A significant change was observed for 56 / 57 Fe (-1000) in pulsing current experiment, this change being significant not only on value of ratio, but also on absolute value. So, for a sample after experiment with pulsing current Af(AT57Fe-Ar56Fe) = 3840 cps, and the natural iron 56/57 isotopes ratio is about 40, 56/57 isotope ratio after experiment is ~0.04. The 56/57 isotopes ratio for Sample 1610 at direct current was ~10. It means that the ratio decreases 4 times due to an increase of the contribution of 57 Fe (a heavier isotope). Thus, a change in the

248 56/57pe j s o t 0 p e r a tio by a factor of more than 100 for comparative experiments with pulsing current and direct current was observed. For the same Sample 1610 the isotope ratio of 4 8 / 4 7 Ti increases ~2.5 times and 48 46 / Ti increases almost ~3.8 times due to a decrease of contribution of a heavier isotope (the most spread 4 8 Ti isotope). The 5 2 / 5 3 Cr isotope ratio also decreases due to a decrease of contribution of heavier isotope 53. Thus, it is impossible to explain this effect by sputtering of a lighter isotope or by isotopes separation. Also it is impossible to explain it by diffusion coefficient. The 56 / 57 Fe isotope ratio in 1694 as compared with natural ratio of isotopes is ^2.3 (Table 8). The 4 8 / 4 6 Ti isotope ratio comparison is about ~5.46. Samples No. 1610 and No. 1694 had different experimental conditions. So No. 1610 was a multilayered compound and after experiment some melting areas and even cracks were found on it and No. 1694 was single-layered and its surface after experiment was more homogeneous. We would like to pay special attention to detection of isotopes with mass number 59 (Co), cps of which was ~10 3 cps, for 55 (Mn) ~10 3 cps, for 45 (Sc) ~ 102 cps. They were found in a plenty in the samples after experiment but they not were found in initial samples. The comparison of the quantity of the elements analyzed by method SMS with possible reactions of fusion-fission of nucleus is given in Table 15 in view of conformity of their masses, their spin and parity. The opportunity of simultaneous appearance of particular isotopes groups in samples is supposed, i.e. formation of such elements as Mg and Br (1); Mg and As (2); Si and As (3) in the same low-energy process in glow discharge. The variants of the reactions given in the table are possible from the results of the analysis. It is possible to see the presence of isotopes with mass numbers 26 and 80 as results of reactions (1-4), 19 and 88 - reaction (5), 50 and 56 - reaction (6) in one analyzed sample. It could be possible to explain the appearance of chemical elements in the samples irradiated by ions in glow discharge by such reactions, but the high Coulomb barrier makes the probability of such processes insignificant. Rodionov 12 paid attention to the fact that the Coulomb barrier is a classical concept and the representation of it at nuclear distances does not work. It means that the concept of the Coulomb barrier is not meaningful in quantum ensembles for low energies of interacting particles. It makes possible multinuclear reactions in low-energy processes. Therefore, it is supposed that Fe, Ni, and Ti can appear in the following reactions: a + ^

2

P d ^ T i + ^Fe*+20.1MeV,

(7)

o r ^ g T i + | | F e + 25.1MeV,

(8)

or -> ^ T i + SSFe + 26.5 MeV.

(9)

Table 14.

Additional elements in structure formations after deuterium experiments (atomic %, EDX)* Screened zone

Boundary zone

Element

Irradiated zone Point 1

oNa Mg Al

Si K S Fe Ni Ga Sr Mo Pd Cd Ac Pb Sn W

73.3+0.7 0.13+0.05 0.12+0.04 2.05+0.04 0.3+0.1

69.3+0.7 0.13+0.10 0.2+0.1 1.8+0.1 0.3+0.1

43.4+1.2 1.0+ 0.2 3.4+0.2 1.0+0.1

1.2+0.3

16.4+1.5

4.3+1.3

1.1+0.2

0.9+0.3

1.6+0.3

0.4+0.1

All zones

Point 2

Point 3

9

10

11

1.6+0.1

22.4+2.1 3.1+0.3 0.96+0.2 0.5+0.13 0.3+0.15

26.4+0.2 1.7+0.4 0.8+0.2 2.2+0.1 0.6+0.1 0.8+0.1

0.5+0.1

Point 4

Point 5

Point 6

12

13

14

38.3+1.3 0.63+0.25 0.75+0.19 3.8+0.1 0.27+0.1

66.2+0.7 0.30+0.06 10.8+0.1

1.54+0.3

4.1+0.2 1.6 ± 0.1

1.6+0.2

2.3+0.2

1.1+0.2

0.2+0.1 0.2+0.1 2.0+0.2

0.6+0.1 74.1 + 1.1

92.3+0.4

0.4+0.1 95.0+0.3

66.3+0.3

95.0+0.3

0.06+0.03 0.22+0.05 0.06+0.03 9.4+0.1 13.6+0.1 0.17+0.5 0.35+0.05 0.14+0.04

0.4+0.1 8.0+0.1 19.2+0.1 0.14+0.05 0.5+0.06 0.2+0.05

0.8+0.2 0.2+0.1

2.2+0.2

44.5+0.3 0.2+0.1 1.2+0.1

92.6+0.7 0.4+ 0.1 2.8+0.3

0.20+0.07

0.12+0.06

1.5+0.2

1.35+0.13 0.37+0.05

2.1+0.2

70.8+0.3

0.16+0.08 54.5+0.3

0.10+0.04 22.1+0.1

95.9+0.3

0.16+0.08

0.04+0.02

2.9+0.25 0.54+0.1

0.2+0.06 0.15+0.1 0.6+0.1

0.2+0.1 0.6+0.1

0.17+0.08 0.21+0.07

0.16+0.06

0.08+0.04

0.07+0.02

*EDX voltage 25 kV, # 1694. **Columns 2—6 are the fragments of boundary of glow discharge and screening zones. • • Columns 8—14 are the fragments of irradiated zone.

N2

CO

250

However, for reactions (7-9) with the participation of oj-particles, first the following possible reactions are to proceed: d + 4 ° 4 Pd - • ?§Ne + §gBr* + a + 5.21 MeV,

(10)

d + !g 5 Pd -» f0Ne* + |§Br* + a + 3.3 MeV,

(11)

d + f68Pd

(12)

-> |Be* + l?Nb* + a + 2.75 MeV,

IfNb* -> 51M:/3~2.3,1.9 : 7787.3, 722.7 -> f|Mo, Table 15. Isotopes ratio in possible nuclear reactions in Sample No. 1734 (SMS). Mass

cps

Possible reactions

26

40

d + 4 ° 4 P d - • 12 2 6 Mg + |gBr* + 15.8; §°Br* -> 17.66M:/5-2.00 : 76I6.6 ->§° Kr; or |°Br* -> 17.66MeV : /3+.85 : X76I6.6 --> 3 4 oe d + 4 g 8 Pd -> 2 | M g + |§As* + a + 12.2;

80

19 88 50 56

60000

80 50 30 18

|°As* - • 16S:/3-5.4,4.7 : 7665.9 — | ° S e d + i g 4 P d -> ^ S i * + |°As* + 2.63 MeV a + 4 |3 2 Pd -> 2 | M g + §°Kr + 8.60 MeV 2 6Si* - • 2.235S:/3 + 3.83 : 7829 - • fjjAl* -1• 6.345S:/3 + 3.21 --?§Mg 2 |A1* - • 7.3E5 A:/3 + 1.17 : 7I8O8.6 - • fj]Mg

1 2

3 4

p + 4<36Pd -> * 9 F + | | S r + 4.42 MeV

5

a + IfPd

6

-> | ° T i + ; | F e + 26.5 MeV

d + i°4Pd - ?°P*+^Zn*+a-r-9.64MeV, a + IfPd ->?§Ne+§tSr +3.16 MeV, a + 4°2Pd - -> i§Ne* + §§Sr + 2.92 MeV, a + 4°4Pd ->ioNe + §|Sr + 5.55MeV, a + 4°6Pd --+?3Ne*+§gSr +2.98 MeV, a + 4°8Pd ^ ? o N e + 3sSr +6.85 MeV It is necessary to note that TIMS in analyzed samples revealed masses of isotopes 18 and 22 to a small extent many times. Isotopes of molybdenum were always present significantly. As it was noticed earlier, molybdenum could also be a consequence of its over-sputtering from the surface of the sample holder. Mass of isotope

251

22 in a quantity of 60 cps and mass 80 in a quantity of 95 cps were also observed in this spectrum. d + ^ 2 P d - • 22Ne + | 2 R b

+

5 90 MeV

.

Masses 22 and 82 were also present in TIMS spectrums of this sample in quantities of 60 and 540 count per second (cps). It is necessary to note that the instable finding of Ag by method EDX 6 could be a result of formation 108 A „* 106A * 108 A * 110A * 47 A 6 , 47 A 6 , 47 A 6 , 47 A 6

in the following reactions with the further transmutation of these isotopes into stable. d + i° 4 Pd -> i°6Ag* + 10.7 MeV, 106Ag* ^ 24.0M: |9~1.96:7511.9 - • ^ 6 C d , d + ^ 6 P d - • i?8Ag* + 10.8 MeV, ™8Ag* -> 2 . 3 9 M : g : / 3 ~ 1.65:7633.0 -> ^ 8 C d d + \°8Pd -+ \]°Ag* + 11.1 MeV, #°Ag* -* 24.65 l :/3~2.981:7657.8 - • ^°Cd. The opportunity of going above described reactions with the formation of argentums isotopes in an excited state and their subsequent transition into stable state can help to understand that the results of finding many elements change with a change in the interval of the samples analysis time after the experiment termination. This fact is undoubtedly important, and it is necessary to take into account when isotopes quantity and their composition are to be correctly estimated, as the performance of the analysis at the time planned after the experiment termination is not always feasible. 5. Conclusion 1. The complex of examinations showed that changes of structure and element composition in the samples irradiated by glow discharge ions depended on: (a) density of ions flow, (b) dose of irradiating ions, (c) kind of irradiating ions, and (d) sort of current and other parameters of process. 2. Dependence on parameters is ambiguous as some factors simultaneously effect (influence) the change of composition. 3. More homogeneous structure and more homogeneous change of composition are observed for long experiments.

252

4. Maximum changes of element composition are observed in " hot (active) points " - micro craters, areas of micromelting and others new structural formations. 5. Various methods of low-energy action on different materials give a formation of plurality of basic elements (Si, Al, Mg, and Ca) found by various methods of the analysis of these materials. Such more rare elements as Mn, Sc, Co, Sr, Ne, and Ba were found in a smaller extent. 6. T h e peak changes of the 5 6 / 5 7 iron isotope composition (1000 times) were observed for pulsed current. 7. A comparison of elements and isotopes found by various analysis methods with possible types of fusion-fission reactions is carried out.

Acknowledgements Authors express the gratitude to corresponding member of the Academy of Sciences LI. Fedik ("Lutch") and Professor, Dr. B.U. Rodionov (MEPhI) for valuable notes by preparation of this article.

References 1. I. Savvatimova, Ya. Kucherov, and A. Karabut, Transaction of Fusion Technology 26, 4T, 389 (1994). 2. I. Savvatimova, A. Senchukov, and I. Chernov , ICCF6, Progress in new hydrogen energy. Japan (1996), p. 575. 3. I. Savvatimova, A. Karabut, Nuclear Reaction Products Registration. Surface, Moscow: RAN (1996), Vol. 1, p. 63. 4. I. Savvatimova B, Karabut A.B., Radioactivity of the Pd cathode after GD. Surface, Moscow: RAN (1996), Vol. 1, p. 76. 5. I. Savvatimova, Transmutation in cathode materials at GD. ICCF-7, Canada (1998), p. 342. 6. I. Savvatimova, Reproducibility of experiments in GD, ICCF8, Italian Phys. Society, Italy (2000), p. 277. 7. J. Dash, I. Savvatimova and H. Kozima, Effects of GD on Radioactivity Proc. ICENES 2002 (2002), p. 122 8. J. Dash, and I. Savvatimova, Effects of glow discharge with hydrogen isotope plasmas on radioactivity of uranium, Proc. ICCF10, Bejing, China, 2002. 9. I. Savvatimova and D. Gavritenkov, Results of Ti analysis after GD. Proc. ICCF11 (2004). 10. A. Karabut, Ya. Kucherov, and I. Savvatimova, Possible nuclear reactions mechanisms at glow discharge in dseuterium. Proc. ICCF3, Japan (1992), p. 165 11. V. Ivanov, Excitation and effect of microplasma discharges on metals and alloys in a microwave plasma torch, Applied Physics B2, 5(2001). 12. Rodionov, Proc. 12 Rus. CF Conf. 2004, Moscow (2005), p. 110. 13. Ya. Kucherov, A. Karabut, and I. Savvatimova, Phys. Let. A170, 265 (1992). 14. G. Vorontzova, and I. Savvatimova, Atomic Energy 69(5), 297 (1990).

ELEMENTAL ANALYSIS OF PALLADIUM ELECTRODES A F T E R P d / P d LIGHT WATER CRITICAL ELECTROLYSIS

YU TORIYABE Division of Quantum Science and Engineering, Graduate School of Engineering, Hokkaido University, North 13, West 8, Kita-ku, Sapporo 060-8628, Japan E-mail: [email protected]. ac.jp TADAHIKO MIZUNO Division of Energy and Environmental System, Graduate School of Engineering, Hokkaido University, North 13, West 8, Kita-ku, Sapporo 060-8628, Japan TADAYOSHI OHMORI Advanced

Technology,

Inc.,

Hokkaido Institute Sapporo 006-8585,

of Technology, Japan

Maeda,

Teine-ku,

YOSHIAKI AOKI Technology

and Electronics

College of Hokkaido, Nakanoshima, Sapporo 062-0922, Japan

Toyohira-ku,

Elemental analyses of palladium electrodes were conducted after a new type of light water electrolysis was performed at optimum conditions in a system designed to induce a nuclear reaction. This process is referred to as P d / P d light water critical electrolysis. The conjecture that a nuclear transmutation process is occurring in this experiment is easier to test in this system, because it is easy to determine whether the elements detected on the cathode surface are impurities or transmutation products. We assume that the elements detected only on the cathode surface, and nowhere else in the cell as contamination, namely iron, titanium, chromium and so on, must be transmutation products. Furthermore, countless Ohmori-type palladium craters were observed for the first time for this system, and these are evidence that nuclear reactions occurred at the electrode surface.

1. Introduction Since Ohmori et al. reported nuclear transmutation reactions with anomalous isotopic yields in his light water electrolysis system, 1_4 many researchers still have claimed various kinds of low energy nuclear reactions. At the same time they observed continuous excess heat as results and countless craters as an evidence of nuclear reactions. A chain of their results in light water system deserves close attention that strongly suggest the existence of condensed matter nuclear reactions. It is, however, still difficult to replicate that reaction in normal electrolysis condition. Through our previous experiments and the other reports, 5 ~ 8 we conjecture 253

254

Figure 1. Surface damage as an indirect evidence of nuclear reactions occurred at the electrode surface. These craters were observed on gold electrode after normal electrolysis, with current density of 0.5 A / c m 2 for 30days in 0.5 M Na2CC>3 solution. 9

that the electrolysis system and electrical parameters are very important factors to induce nuclear reactions. We have investigated an optimum electrolysis system and condition and describe details in this paper. Both transmutation products and surface damage are needed to prove that a nuclear reaction has occurred. Figure 1 shows an example of damages in a gold electrode reported by Ohmori et al9 Although many researchers have reported nuclear transmutation, as far as we know, there has been no other reports of the Ohmori-type craters. If the nuclear reactions occur on the electrode surface, the surface damages like Ohmori-type craters should be found after the experiment. 2. P l a s m a Electrolysis

2.1. Time

Variations

It is widely recognized that plasma electrolysis can produce a large amount of excess heat, and nuclear transmutation products. When the temperature of an electrode exceeds the boiling temperature of electrolyte due to intense polarization, a thin vapor layer is generated at the electrode/electrolyte interface in which high electric field ionize vapor molecules to generate the plasma state. Formation of this vapor film is the first key factor to achieve the plasma electrolysis condition. Time variations of cell voltage and current during the plasma electrolysis are shown in Fig. 2. In this case the axis of ordinates indicates not only current but also current density because the electrode surface of cathode is ca. 1cm 2 . The period of electrolysis is divided into six regions for the sake of convenience, namely conventional region, critical region, breakdown point, transitional region, partial plasma region, and full plasma region. The electrical current increases with applied voltage up to the breakdown point at which time the sheath of vapor film is generated. Then the current drops down through the transitional region because the electrode and the electrolyte cannot touch each other directly owing to the vapor layer.

255 320

swH

2 1

280

<3

4

•••-•-M

Plasma region

JSL

fer

2.5

240 ,1V

>^

V


JV

80

(w^Um, 0.5

"M I I : 0

2000

4000

6000

8000

10000

Time (s)

Figure 2. Time variations of cell voltage and current during plasma electrolysis with 1.5 mm diameter tungsten cathode in 0.2mol/dm 3 K2CO3 solution. (1) Normal region, (2) critical region, (3) breakdown point, (4) transitional region, (5) partial plasma region, and (6) full plasma region.

If cell voltage is sufficiently high, some atoms or molecules in that gas phase are ionized. Therefore, current does not drop to zero and the electrode temperature remains high due to the good electrical conductivity and reduced thermal loss of the gas phase. Starting from this region, light emission occurs. The color of light depends on the electrolyte solution. Light emission area expands with increasing the cell voltage. Finally, in region-6, the glow covers the entire surface of the electrode and the intensity of light becomes strong. We defined these two regions, regions 5 and 6, as plasma region. 2.2. VI

Relation

A voltage-current relation of plasma electrolysis is shown in Fig. 3, which is converted from Fig. 2. When the current density increases above approximately 2.5 A/cm 2 , the type of electrolysis changes to the plasma where the current is

0

Figure 3.

40

80

120 160 200 Cell voltage {V}

240

280

320

Voltage-current relation during plasma electrolysis converted from Fig. 1.

256

almost constant. This critical value also supports the experimental result reported by Ohmori et al.w It is necessary to select an experimental condition, current and voltage, from this VI curve. 2.3.

Shortcomings

Although the plasma electrolysis can induce a large amount of excess heat with hydrogen and anomalous nuclear transmutation, 11 ' 12 this type of electrolysis has some and fatal shortcomings. At the boundary between regions 5 and 6, that is, at the time when whole area of the electrode surface is covered with the glow, the temperature of the surface rises to 1400°C. Furthermore the local temperature exceeds the melting point of the electrode at where the sparks like arc discharges occur due to current flow paths between the electrode and the electrolyte. Therefore, the electrode cannot survive more than 30 min without being melted or broken. And the electrolyte solution is also pyrolyzed by the high-temperature plasma. The most serious problem is that the rare nuclear transmutation products on the electrode surface are lost from this damage. Therefore another, milder type of electrolysis, which does not severely damage or disintegrate the electrode, is called for to prove that nuclear reactions occur. 3. Critical Electrolysis 3.1. Optimum

Region

We assume the positive correlation between the excess heat and the current density exists in normal region, while the excess heat increases with the input voltage in plasma region. This assumption is illustrated in Fig. 4 with the VI relation described in Fig. 3. In fact, some researchers have reported these correlations. 13~15 Since the plasma region is inappropriate, Ohmori et al. specified that region-2 is most favorable one to obtain the excess heat and the transmutation in electrolysis system, and they referred to this type of electrolysis as Critical Electrolysis. 7 ' 8 Although the exact condition required depend on the experimental system, a target „

"

^

Excess heat and

2.5

<

2

I" 1 0.5

0

40

80

120

160

200

240

280

320

Cell voltage (V)

Figure 4.

An optimum region to induce nuclear reaction without disintegrating the electrode.

257

current density is approximately 2.5 A/cm 2 . Through this type of electrolysis, a long duration time experiment is possible because the electrode is not damaged. Thus transmutation products are well preserved and continuous excess heat can obtained. 3.2.

Results

We had conducted critical electrolyses with nickel cathodes in 1M Na2CC>3 solutions. 5 Figure 5 shows EDX spectrums of nickel electrodes after the experiment through which the current density was kept ca. 2.6 A/cm 2 for 15 days. The mean voltage applied was 14 V and solution temperature raised up to 80°C. Detected strong platinum peaks are probably originated from a counter electrode though the isotopic ratio for this platinum has not been confirmed yet. In general, the platinum anode is less dissolved and electrodeposited in alkaline solution, especially K2CO3 or Na2CC>3. However the experimental results suggest that this unusual reaction is accelerated in certain conditions, and this platinum complicates transmutation processes such as photofission.16 Then that electrodeposited platinum makes an evaluation of process difficult. Therefore in the experimental system the anode material should be the same as the cathode. 1000000

100000

I

10000

o O 1000

Energy (keV)

Figure 5. EDX spectrums of nickel electrodes before and after the critical electrolysis with current density of 2.6 A / c m 2 for 15 days in 1 M Na2C03 solution.

4. P d / P d Critical Electrolysis 4.1. Experimental

Set-up

P d / P d Critical Electrolysis is defined as the optimum condition to evaluate the transmutation process precisely. In this system, the effect of materials electrodeposited from the anode is avoided by making the anode from the same element as the cathode. This limits the elements detected on the cathode to being either impurities from elsewhere in the cell, or from transmutation. Furthermore, if these elements are transmutation products, evaluating them is simpler.

258

A schematic view of an experimental set-up is illustrated in Fig. 6. The system should be very simple, because it has to be cleaned very carefully before the experiment, to avoid contamination.

Hose

|

^iftCOtl

Figure 6.

fuB*>^

An experimental set-up for the P d / P d critical electrolysis experiments.

A Teflon (PFA) cell (Flon Industry Co. Ltd., Tokyo, Japan) whose capacitance, diameter and height are 300 cm 3 , 80 mm and 70 mm, respectively is capped with a silicon rubber. Although vapor cannot leak from this system, hydrogen can easily leak from a hole with another silicon rubber to add the Milli-Q water to restore the volume of the electrolyte, which decreases due to the decomposition. In this experiment the anode and cathode are made from identical palladium wires (Tanaka Kikinzoku Kogyo, Tokyo, Japan) taken from the same stock. Both are 99.95% pure Pd, 1.0mm diameter, 15.7rnm long, with ca. 0.5cm 2 surface area. They were polished up by emery papers (No. 1500 and No. 2000), and washed with acetone. After being covered with Teflon (PTFE) tubes, they were located at the both side of the cell symmetrically. Before the experiment, the cell and electrodes were cleaned carefully with nitric acid or sometimes mixed acid (1:1 H2SO4+HNO3), and rinsed with Milli-Q water. The electrolyte solution of 1M and 200 cm 3 was prepared by K2CO3 (Kanto Chemical Co. Inc., Tokyo, Japan) whose purity is over 99.95% and Milli-Q water whose specific resistance is over 18.0Mf2cm. Isotopic abundant of hydrogen and deutrium atoms of this Milli-Q water is natural since ordinary water was used. The natural concentration of D 2 0 is so low the influence from it is negligible. The cell was placed in a constant temperature chamber (MIR-151, Sanyo Electric Co. Ltd., Osaka, Japan). The solution temperature was roughly measured by two thermo couples, which located at the center and edge of the cell. Air temperature v/as also monitored and kept 22.0-24.0°C. The current density exceeded 2.5 A/cm 2 controlled by a constant current/voltage power supply (GP0250-3R, Takasago Ltd., Hyogo, Japan). The experiments were continued for 7 or 10 days, while various data was collected on a data logger (842150, Hioki E. E. Co., Nagano, Japan). During the electrolysis, Milli-Q water was added every 12 h to restore the volume of electrolyte lost to decomposition.

259

4.2. Elemental

Analysis

After the experiments both electrodes were observed by SEM (JSM-6500F, JEOL Ltd., Tokyo, Japan) and analyzed by EDX (JED-2300, JEOL Ltd.). Figure 7 shows those spectrums from the whole area of each electrode. In this case, current density had been 3.2 A/cm 2 for 7 days. The thick line means the cathode palladium spectrum, and the thin line is the anode spectrum. The count of the anode spectrum is multiplied 1.18 to make it overlap with the cathode spectrum. Through P d / P d electrolysis a comparison between the cathode and the anode is more suitable than that between before and after. ' Pdi

Cathode 1 Anode |

»Pd

1

--P-d-i

'"Cu""

Fe

W/Mg

Fe

^

0

Energy (keV)

Cu

^

Energy (keV)

Figure 7. EDX spectrums of palladium electrodes, cathode and anode, after the P d / P d critical electrolysis with current density of 3.2 A / c m 2 for 7days in 1 M K2CO3 solution. Counts of anode spectrum are multiplied 1.18 to be overlapped with the cathode spectrum.

The elements shown in bold letters iron, titanium, chromium, manganese, and nickel were detected from the cathode palladium only, on the other hands, the elements shown in italic letters, copper, zinc, and magnesium were detected from both electrodes in this case. Therefore, we consider the elements shown in bold letters must be transmutation products. Especially, the iron peaks were detected from all cathode samples after P d / P d critical electrolysis. The elements shown in italics may have originated from two possible sources: transmutations or impurities. If these were transmutation products, at least two processes may explain their existence. The first nuclear reaction presumably occurred at the cathode and only produced the bold letter elements, while the second reaction occurred at both electrodes, and produced the italic letter elements. Since we have not analyzed the samples by the other methods, we cannot determine the origin of these elements yet. If we confirm the isotopic distribution is anomalous, we will then be prepared to discuss the origin and transmutation processes of the detected elements, whether they are electrodeposited impurities or transmutations. 4.3.

Micro-Structure

Figures 8 and 9 are the SEM photographs of the anode palladium surfaces and the cathode surfaces after the P d / P d critical electrolysis, respectively. The anode palladium has some cracks due to the oxidation.

260

Figure 8. SEM photographs of the anode palladium surfaces after P d / P d critical electrolysis with current density of 3.6A/cm 2 , for 10days in I M K2CO3 solution. Magnifying power and scale standard line are shown at the bottom of each photograph.

Figure 9. SEM photographs of Olnnori-tYpe palladium crater^ un the cathode sui(Vu«> after P d / P d critical electrolysis with current density of 3.6 A / c m 2 , for 10days in I M K2CO3 solution. Magnifying power and scale standard line are shown at the bottom of each photograph. The craters whose maximum size is over 10 fim. are located along the surface cracks.

261

On the cathode surfaces the countless Ohmori-type palladium craters were observed as an indirect evidence of nuclear reactions. These craters, which are located along the surface cracks or grain boundaries, were observed on the cathode only up until now. This result indicates that the nuclear reactions occur more easily around the surface and the cracks. The maximum width and height of craters are over 10 /mi. These crater sizes have a positive correlation with the current density. This result supports our prediction that the amount of excess heat and transmutation have a positive correlation with increase of current density. Therefore, the critical region is optimum to induce the nuclear reactions as described above. 4.4.

Discussion

To our knowledge, this is the first report of the Ohmori-type craters observed on the palladium electrodes. The characteristics of these palladium craters are similar to the gold craters first reported by Ohmori et al.3 Although the report was made 10 years ago, the formation mechanism is still unknown. Kamada et al. reported anomalous heat evolution and surface melting of deuteron implanted aluminum foil upon electron bombardment. 17 They estimated that the amount of anomalous heat exceeds the total amount of any kind of chemical reactions and, therefore, concluded a novel nuclear reaction had been occurred in the deuterated aluminum. If palladium electrode were melted due to this type of nuclear reaction, the palladium gas should be erupted. Then it should have cooled down in the solution to be recrystallized like the crater. Numata et al. found vortex patterns on well annealed thick palladium electrodes after a long-term heavy water electrolysis,18 and simulated a magnetic interaction of hypothetical particles to elucidate an evolution mechanism of vortexes. 19 They showed the vortex can be formed at the electrode/electrolyte interface by FEM method. If charged palladium particles dissolved from the anode were caught in a vortex, which is generated at the electrode/electrolyte interface, they might be accumulated to the cylindrical shape like the vortex to form the craters. Mizuno et al. described a large explosion that occurred during a normal light water electrolysis. 20,21 They made a rough estimate of the energy balance and concluded that it could not be a simple explosion, but rather it must have been caused by a large burst of anomalous heat. If micro explosions occurred on the electrode surface from this same type of heat, craters could be generated. It is still difficult to explain the mechanism by these theories. Although they may be impurities electrodeposited uniformly, we claim that the crater is an indirect evidence of nuclear reaction occurred at the electrode surface. 5. Conclusion P d / P d light water critical electrolyses were performed as the optimum condition and system to induce nuclear reactions. In this study the shape of both electrodes

262

was just same and the current density was over 2.5 A / c m 2 , for 7 or 10days, in 1 M K2CO3 solution whose t e m p e r a t u r e was u p to 70-90°C. After the experiment, the obvious t r a n s m u t a t i o n products namely iron, titanium, chromium, manganese, and nickel were detected by EDX. In particular, the iron peaks are very strong and detected from all cathode samples. The anomalous isotopic yield of detected iron should be expected since the anomaly has already claimed by many researchers. 3 ' 4 ' 2 2 T h e elements detected from the b o t h electrodes, namely, copper, zinc, and magnesium, however, cannot indicate their origin at this time. If they are t r a n s m u t a t i o n products, at least two mechanisms exist. T h e analysis of isotopic yields for all elements detected by SIMS must be indispensable to prove nuclear reactions. Quantitative analysis of the detected elements, distribution especially around craters, and isotopic yields are under considerations. Moreover, nuclear radiation detection could give important information to evaluate the process. Precise heat measurement is also required. Accurate estimation and reduction of impurities is also vital. Although the isotopic yields have not confirmed yet in this study, Ohmori et al. have already reported anomalous isotopic distribution of palladium with excess heat in their P d / P t critical electrolysis s y s t e m . 7 , 8 Furthermore the indirect evidence of nuclear reactions, namely Ohmori-type palladium craters were observed for the first time. Since the t r a n s m u t a t i o n products and the surface damages have been found, P d / P d critical electrolysis is optimum to induce condensed m a t t e r nuclear reactions. References 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16. 17.

T. Ohmori and M. Enyo, Proc. ICCF4 1, N2.3 (1993). T. Ohmori and M. Enyo, J. New Energy 1(1), 15 (1996). T. Ohmori, T. Mizuno, and M. Enyo, J. New Energy 1(15), 90 (1996). T. Ohmori, M. Enyo, T. Mizuno, Y. Nodasaka, and H. Minagawa, Fusion Technol. 31, 210 (1997). Y. Toriyabe, T. Mizuno, T. Ohmori, and Y. Aoki, Proc. JCF6 11 (2005). T. Mizuno, T. Ohmori, and T. Akimoto, Proc. ICCF10 (2003). T. Ohmori, S. Narita, H. Yamada, T. Mizuno, and Y. Aoki, Proc. JCF4 22 (2003). T. Ohmori, T. Mizuno, H. Yamada, and S. Narita, Proc. JCF5 36 (2004). A. Takahashi, H. Numata, H. Yamada, Y. Iwamura, T. Ohmori, T. Mizuno, and T. Akimoto, Study Nucl. React. Solid 159 (1999). T. Ohmori, Curr. Top. Electrochemistry 7, 102 (2000). T. Mizuno, T. Ohmori, T. Akimoto, and A. Takahashi, Jpn. J. Appl. Phys. 39, 6055 (2000). T. Mizuno, T. Akimoto, K. Azumi, T. Ohmori, Y. Aoki, and A. Takahashi, Jpn. J. Appl. Phys. 44(1A), 396 (2005). T. Ohmori and T. Mizuno, Curr. Top. Electrochemistry 5, 37 (1997). M.C.H. McKubre, S. Crouch-Baker, A.M. Riley, S.I. Smedley, and F.L. Tanzella, Proc. ICCF3 5 (1993). K. Kunimatsu, N. Hasegawa, A. Kubota, N. Imai, M. Ishikawa, H. Akita, and Y. Tsuchida, Proc. ICCF3 31 (1993). A. Takahashi, M. Ohta, and T. Mizuno, Jpn. J. Appl. Phys. 40, 7031 (2001). K. Kamada, H. Kinoshita, and H. Takahashi, Jpn. J. Appl. Phys. 35, 738 (1996).

263

18. H. Numata, R, Takagi, I. Ohno, K. Kawamura, and S. Haruyama, Proc. ACCF2 71 (1991). 19. H. Numata and M. Ban, Proc. ICCF12 (2005). 20. T. Mizuno, Y. Toriyabe, A. Takahashi, and A. Takada, Proc. JCF6 19 (2005). 21. T. Mizuno and Y. Toriyabe, Proc. ICCF12 (2005). 22. G. H. Miley and J. A. Patterson, J. New Energy 1(3), 5 (1996).

P R O G R E S S O N T H E S T U D Y OF ISOTOPIC C O M P O S I T I O N IN METALLIC THIN FILMS U N D E R G O N E TO ELECTROCHEMICAL L O A D I N G OF H Y D R O G E N

M. A P I C E L L A A N D V. V I O L A N T E ENEA

Frascati Research

Center, V. le E. Fermi 45, 00044 Frascati E-mail: violante®frascati. enea.it

(Roma),

Italy

F . S A R T O , A. R O S A D A A N D E. S A N T O R O ENEA

Casaccia

Research

Center,

V. Anguillarese (Roma), Italy

301, 00060 S.Maria

di

Galeria

E. C A S T A G N A A N D C. SIBILIA La Sapienza

University,

Via Scarpa,

14, 00100 (Roma),

Italy

M. M C K U B R E A N D F . T A N Z E L L A SRI International,

333 Ravenswood

Ave, Menlo Park,

CA 94025,

USA

G. H U B L E R Naval Research

Laboratory,

4555 Overlook Ave.,

S.W.

Washington,

DC 20375,

A research activity has started some years ago in the framework of collaboration between the ENEA (Italy) and the SRI (USA), aimed to the identification of traces of nuclear reactions in condensed matter. This work has also involved cross-linked analysis in order to identify effects due to contaminants that could affect the isotopic shift estimate. Nickel thin films have been sputtered on a polymeric substrate and loaded with hydrogen by electrolysis. Reference and active thin films have been prepared contemporaneously during the same sputtering process to have on both the same deposition and the same impurities composition. Secondary Ion Mass Spectroscopy (SIMS) has been used to analyze the isotopic composition of the electrolyzed and blank substrates. Preliminary results (Violante et al, Proc. 10th Int. Conf. Cold Fusion (ICCF-10), Cambridge, 2003) indicated that a reasonable reproducible apparent shift of the isotopic composition of the Cu element occurred in some of the electrolyzed films, with an increasing of mass 65, while the natural value was always observed for all the blank samples. Cu was particularly suitable for being used as a marker elements because of its only two mass isotopes (63/65) that do not overlap with isotopes of other elements having the same masses. In this work, new experiments have been reproduced to increase the statitistics and further analysis has been performed in order to exclude that the revealed shift was traceable to an artifact.These included SIMS scanning of the sample surface, depth profile analysis by SIMS, mass spectrometric analysis of the electrolyte, SUPER-SIMS [2] analysis of one couple of reference and active films. In particular, the possible contribution from mass interferences on the 65-mass extrasignal has been considered, coming from contaminants or double ionized species. On the basis of the new results, a more complex scenario has been evidenced,

264

USA

265 suggesting that the former attribution of the C u 6 3 / C u 6 5 isotopic shift could be not correct. The indication of new experiments and tests that potentially should provide a complete understanding of the present results has been given. The work wants to stress that the identification of elemental transmutations in metal hydrides is an extremely complex topic, which necessitate of severe scientific accuracy, cross-matched analysis, multidisciplinary expertise, and the access to top performance experimental facilities. All these requirements can be fulfilled only in the framework of top-level international scientific collaboration.

1. Introduction The detection of nuclear ashes inside metallic hydrides is one of the most direct evidences of the happening of nuclear reaction in the condensed matter. But this topic is also a very complex and delicate issue, first of all because of the low level of the signals to be detected, which can be easily overlapped by instrumental noise or background interferences. The measurement of the isotopic composition of metallic hydrides is an efficient method to reveal nuclear products eventually formed during the hydrogen loading. Actually, the presence of "new" (i.e. "not detected before") elements in the metal specimens cannot be assessed as products of a nuclear reactions, because the possibility of contamination from the environment or the diffusion of impurities inside the sample to the detection areas are very difficult to be excluded completely. A research activity has started some years ago in the framework of collaboration between the ENEA (Italy) and the SRI (USA), aimed to the identification of traces of nuclear reactions in condensed matter. Preliminary results 1 by Neutron Activation Analysis (NAA) have given indication of Ag isotopic shift occurring in Pd thin films after electrolysis. A first screening by Secondary Ion Mass Spectrometry (SIMS) of the isotopic composition of Nickel thin films undergone to similar experiments has also pointed out an isotopic ratio different from the natural one on the 63/65 masses imputable to copper. 2 In this work, further reproduction of the previous experiments and a more accurate analysis of the experimental data have been performed. Cross-linked analysis has also been involved, in order to identify artifacts that could affect the isotopic shift estimate.

2. Experimental The typical experiment, already described in Ref. 2, consisted in three steps: • Deposition of two identical Reference and Active nickel films during the same deposition run; • Hydrogen loading of the Active film by electrolysis; • SIMS analysis of both Reference and an Active sample isotopic composition, to search deviations from the natural abundances.

266

Steps (1) and (2) have been carried out in a class 1000 clean room laboratory, by using clean room grade gloves and papers in order to reduce source of contaminants. To the same aim, a reduced number of high-purity materials have been used both for sample production and electrolysis cell assembling. 2.1. Metallic

Film

Deposition

The films (with 45 nm thickness) have been deposited by ion beam sputtering of a Ni target (MRC, 99.98% purity) on polyethylene (kartell) 12 mm diameter - 1 mm thick disks. Before deposition, the substrates have been chemically cleaned as reported in Ref. 2, and ion beam etched to improve film/substrate adhesion and to assure good film surface status after electrolysis.Up to six identical Reference and an Active nickel films have been deposited during the same run, loaded on a rotating sample holder. 2.2. Hydrogen

Loading

The hydrogen loading of the Active film has been carried out by electrolysis, in Light water (18 MW) LiS04 solution (1M). The cell was realized in polyethylene (Kartell), with high purity (99.98%) Pt electrodes (see photo in Ref. 2). Typical values of the current and voltage used during the experiments ranged between 5190 mA and 2-7 V, respectively. Loading times went from a minimum of 3 h to a maximum of 40 h. 2.3. SIMS

Analysis

Secondary Ion Mass Spectrometry measurements have been carried out with a Leybold SSM-Mass Spectrometer Module, operating at the ENEA research centre in Frascati (Rome, Italy). The Mass Spectrometer is equipped with a source Leybold IQE 12/38 ion source and a Balzers Quadrupole Mass Analyser working in the mass range 0-511 a.m.u. The primary beam was fed by Ar + ions at 5keV. The beam spot had a diameter of about 2 mm, small enough to allow scanning of the sample surface. Typical sensitivity and resolution were 0.5 a.m.u. (m/<5m « 100) and 1012 at/cm 2 , respectively. Reference and electrolyzed films have been loaded together into the analysis chamber, positioned at 180° on a cylindrical support and analyzed in series under the same SIMS conditions. 3. Results Preliminary results reported in Ref. 2 showed an apparent isotopic shift on the 63 Cu/ 6 5 Cu masses in nickel thin films undergone to electrolysis (active films), whereas an isotopic composition matching the natural abundance was always detected in the not-electrolysed (reference) films.

267 Table 1.

Synoptic of the new experiments described in this work Apparent i sotopic shift

Sample

Film after electrolysis

Electrolysed

Reference

Ni Ni Ni Ni Ni

Ok Ok Ok Ok Ok

Yes Yes Yes No Yes

No No No No No

Ibis 3bis P2 P3 4

The tuning of the SIMS instrumentation was checked during each of the analysis runs, by moving the sputtering argon beam on the stainless steal sample-holder where the Cu isotopic composition was always found to be the natural one. We have repeated the same experiment in order to increase the statistics and evaluate its reproducibility. A synoptic of the new experiments has been reported in Table 1, giving evidence of the apparent isotopic shift in 4/5 cases. The SIMS analysis has been carried out on different points of the sample surface, showing a more relevant effect in the middle of the sample (see Fig. 1). Furthermore, a dynamic SIMS analysis has been done in order to check if the shifted isotopic ratio was maintained below the surface. The depth profile of the 63, 65, 58, and 12 masses has been recorded, showing that the 63/65 shift survives beyond the surface down to the film/substrate interface, and it is not coupled with the C 12 signal of carbon but with the Ni 58 signal, originated by from the main constituent of the film (see discussion below). In addition, a cross-linked analysis has been done by using the SUPER-SIMS facility located at the ETH, in Zurich (Switzerland). 3 The instrument used Cs + primary ions and the analysis revealed negative secondary ions. A couple of Reference and Active samples have been analyzed to verify the above results. Due to unwanted charging of some parts of the extraction section, causing signal instability, the Cu 63 /Cu 65 isotopic ratio measurement needed calibration by a pure standard. Then, a sequential procedure has been followed to carry out the measurements, consisting in the analysis of a pure Cu standard, the Reference sample, the pure Cu standard again and the Active sample. The values measured for each sample, after calibration, showed some discrepancies with the measurements performed in Rome, giving Cu 6 3 /Cu 6 5 = 2.40 ±0.31 for the Active sample and Cu 6 3 /Cu 6 5 = 1.79 ±0.02 for the Reference sample. In the following discussion, both results are carefully analyzed, in order to get informing conclusions. 4. Discussion An alteration of the isotopic ratio of the copper is relatively simple to detect because copper has only two stable isotopes, which do not overlap with isotopes of other elements having the same masses. However, mass interferences on the considered

268

1.00e+003 SINS-SNNS

cps

Mass scan Datapoints/[amu] 54 Scan speed [sec/amu] 6.000 Resolution 7.0 Smoothing ON Vertical scale LIN J=3

65

1

r 63

V 1

1

',

i

If

1.00e+000 52 5 0 0

>f

\

i1 Ni/Pe

V

5.00e+002

SINS-SNNS

cps

!

i

f

i If 1

61.500

Mass scan Datapoints/[amu] 64 Scan speed [sec/amu] 6.000 Resolution 7.0 Smoothing ON Vertical scale LIN Current 10 Speed 6

A

! i

1-OOe+OOO

s.

*

Pos 6=340 Z=57.5 66.500 [amu]

i

I

63

*

in

•

A As

\

'/ «

Ni/Pe

Pos. 57.5

9=335

65.500 [amu]

m

«—-^

Figure 1. SIMS spectrum of the Active sample in the midway of the specimen (left) and close to the edge of the specimen (right).

65 and 63m/e signals from compounds or double ionized species could affect the results, when using a conventional SIMS facility with limited resolution. Therefore, a careful analysis of all possible contribution to the 65-m/e signal in the SIMS spectrum has to be done, concerning the above described results. Ni 64 H (65 mass) detection has been considered unlikely, because the isotopic ratio Ni 62 H (63 mass)/Ni 64 H (65 mass) of Ni more abundant isotopes did not match the natural value (3.9), being the observed isotopic shift just into the opposite direction. The contribution to the 65 m/e signal from double ionized ions had also to be excluded because of the absence of signals at 130 m/e, relative to the corresponding single ionized elements (Te 130 or Ba 130 ?). A more complicate issue consisted in excluding possible interferences from organic contaminants, which could produce positive ion fragments having 65 molecular masses. Actually, 65 mass C 5 H^ ion is very reactive, but it could be produced

269 Table 2. Peak intensity ratio of the SIMS signals during the dynamic analysis of the Active sample: column 2 shows values at the film surface, column 3 at the interface between the film and the substrate Mass peak ratio

On the surface

Close to the substrate

Ni58/C12 Ni58/mass65

35 ± 2 65 ± 6

8.1 ± 0 . 5 49 ± 16

during the SIMS analysis by fragmentation of higher mass organic molecules (hydrocarbons). Typical spectra of hydrocarbon contaminants show groups of odd mass peaks with 12a.m.u. periodicity (due to 1 C atom increment in the chain fragment). 4 Fragmentation patterns of hydrocarbons involving 65-mass positive ion are reported in literature, 4 ~ 6 but they were not clearly readable in our SIMS spectrum [see Fig. 2: masses 15, 43, 69 are not detected masses 51, 53, 55, 57 are masked by signals due to isotopes of clearly identified elements, present also in the reference sample (V 51 , Cr 53 53, Mn 55 , Fe 57 )].

10

20

30

40

50

60

70

80

90

m/e (a.m.u.) Figure 2.

SIMS spectrum of the Active film in the wide mass range.

Furthermore, the dynamic SIMS analysis showed that an increasing of the C 12 signal due to the substrate was coupled with a decreasing signal of other species but without any change in the Cu isotopic ratio, so that one may exclude an effect of the polymeric substrate on the increasing signal of mass 65. In Table 2 the peak intensity values of the SIMS signals at the masses 12 (carbon), 58 (nickel), and 65 have been reported as they have been measured at the film surface and close to the film/substrate interface.

270

The possibility of organic contamination of the film surface from the electrolytic solution has been also considered. Gas chromatography analysis of the electrolyte has been performed, showing that organic contaminants are less than 1 ppb. On the basis of the above-mentioned observations, one should exclude a contamination due to organic substances at mass 65. Finally, the possible interference from inorganic compound contaminant matching 65 mass has been considered. By seeing at the more abundant elements revealed in the whole range SIMS spectrum, detection of Ni 58 Li 7 (total mass = 65) compound could be expected. In fact, despite of NiLi is not a stable compound; Li is clearly detected on the active film surface, coming from the electrolytic solution. Supporting this assignation is the detection in our SIMS spectrum of the 65, 67, 82, and 84 mass peaks, which can be associated to the isotopes of the NiLi and NiLiOH compounds (mass 65 =4> Ni 58 Li 7 , mass 67 =4> Ni 60 Li 7 , mass 82 => Ni 58 Li 7 OH, mass 84 =>• Ni 60 Li 7 OH). In Table 3 are reported the intensity ratios between the SIMS peaks associated with the above compounds. The obtained values match the natural isotopic ratios in the case of the Ni 58 and Ni 60 isotopes, but nothing can be said in the case of Li 7 , Li6 isotopes, due to the poor accuracy of the data, affected by the Ni 64 contribution to the 64 peak. In conclusion, the contribution to the 65 mass peak from Ni 58 Li compound seems to be the only reasonable explanations of the reported results, out of the copper isotopic shift hypothesis. This supposition could also be consistent with the SUPER-SIMS results, which indicated a value for the isotopic composition of copper similar to the natural one for both the active and reference films analyzed. Some uncertainty still affect our results, concerning the fact that Li contamination from the electrolyte is expected in all electrolyzed samples while in some of them the 65 extra signal has not been revealed. As concerning the SUPER-SIMS measurements, the information is limited to a restricted area of the film surface, because only one point of the surface of each sample has been analyzed, which could be not representative of the whole sample surface, since a gradient effect in the isotopic composition has been demonstrated by the conventional SIMS surface scanning analysis. Further experiments and tests could be useful in the future, to completely understand the present data. In particular, surface scanning by ultra-high resolution SIMS apparatus (m/<5m > 3000, enough to resolve mass interferences), Table 3. Intensity ratios between the SIMS peaks associated with the NiLi and NiLiOH compounds Isotopes ratio

SIMS peaks ratio

Natural isotopic ratio

Ni58Li7/Ni60Li7 Ni 5 8 Li 7 OH/Ni 6 0 Li 7 OH Ni58/Ni60

2.0 ± 0.5 2.5 ± 0.5 2.71 ± 0 . 0 1

2.60 2.60 2.60

271

cross-matched analysis by other methods (e.g. Nuclear Activation Analysis), similar experiments with changed electrolyte (e.g. N a O H instead of LiS04).

5.

Conclusions

Based on preliminary results, showing evidences of isotopic shift on the Cu masses (65 too high) in Ni hydrogenated films, a new set of experiments has been reproduced and further analysis have been performed in order to exclude t h a t the revealed shift was traceable to an artifact. These included SIMS scanning of the sample surface, depth profile analysis by SIMS, mass spectrometric analysis of the electrolyte, SUPER-SIMS analysis of one couple of reference and active films. On the basis of the new results, a more complex scenario has been evidenced, suggesting t h a t the former attribution of the C u 6 3 / C u 6 5 isotopic shift could be not correct. T h e work wants to stress t h a t the identification of elemental transmutations in metal hydrides is an extremely complex topic, which necessitate of severe scientific accuracy, cross-matched analysis, multidisciplinary expertise and the access to top performance experimental facilities. All these requirements can be fulfilled only in the framework of top-level scientific collaboration worldwide.

Acknowledgments T h e authors t h a n k Dr. K. Grabowski and Dr. M. Melich of Naval Research Laboratory (Washington, DC, USA) for the important help received on this matter. T h e contribution of Dott. Luigi Nardi of E N E A research center Casaccia (Rome, Italy) in performing the gas cromatography analysis is sincerely acknowledged.

References 1. V. Violante, M. L. Apicella, L. Capobianco, F. Sarto, A. Rosada, E. Santoro, M. McKubre, F. Tanzella, and C. Sibilia - Search for nuclear ashes in electrochemical experiments. Proc. of 10th International Conference on Cold Fusion (ICCF-10), Cambridge, MA, August 24-29 (2003), World Scientific Inc., Singapore. 2. SUPER-SIMS analysis has been performed by the facility located at ETH, by Dr. M. Doebely. 3. V.Violante, P.TYipodi, D. Di Gioacchino, R. Borelli, L.Bettinali, E.Santoro, A. Rosada, F.Sarto, A.Pizzuto, M.McKubre, F.Tanzella, X-ray emission during electrolysis of light water on palladium and nickel thin films. Proc. of 9th International Conference on Cold Fusion, (ICCF9), Beijing, May 19-24 (2002). 4. SIMS technical report by RIBER Instrumentation Ultra-vide, France. 5. Integrated Spectral Data Base System for Organic Compounds by National Institute of Advanced Industrial Science & Technology, SDBSWeb: http://www.aist.go.jp/ RIODB/SDBS/. 6. Organic Compound Database by Harold M. Bell at Virginia Tech., http://www.colby. edu/ chemistry/cmp/cmp.html.

IN SITU ACCELERATOR ANALYSES OF PALLADIUM COMPLEX UNDER DEUTERIUM PERMEATION

A. K I T A M U R A , R. NISHIO, H. IWAI, R. SATOH, A. TANIIKE A N D Y. F U R U Y A M A Department of Environmental Energy Science, Graduate School of Science and Technology, Kobe University, 5-1-1 Fukaeminami-machi, Higashinada-ku, Kobe 6580022, Japan E-mail: kitamura@maritime. kobe-u. ac.jp

Preliminary results of experiments on D2 gas permeation using a system (vacuum/CaO/Sr/PdD a ; /D2) have shown some evidence of nuclear transmutation from Sr to Mo. The system is a little simpler than that used by Imamura et al., and has a reversed gas flow direction. The diagnostic method used to identify the elements was conventional X-ray photoelectron spectroscopy, giving the areal densities of 4.2 X 10 1 4 c m " 2 (Sr) and 3.3 X 10 1 4 c m " 2 (Mo). Extended analytical methods are now being prepared, including in situ and simultaneous particle induced X-ray emission, Rutherford backscattering spectroscopy, nuclear reaction analysis, and elastic recoil detection analyse for areal densities of transmutation elements and deuterium distribution.

1. Introduction It has been claimed 1 ' 2 that forced permeation of deuterium through P d / ( C a O + P d ) / P d samples doped with some element X induced nuclear transmutations from X to X', where (X, X') being ( 133 Cs, 1 4 1 Pr), (88Sr, 96 Mo), ( 138 Ba, 150 Sm), and ( 137 Ba, 149 Sm). The main diagnostic methods in these studies were X-ray photoelectron spectroscopy (XPS), time-of-flight secondary-ion mass spectroscopy (TOF-SIMS), and X-ray fluorescence (XRF). To confirm and investigate the phenomena, it is essential that the same results be obtained in different laboratories with different analytical methods. We have constructed an experimental system, with which accelerator analyses of the samples including particle induced X-ray emission (PIXE), elastic recoil detection analysis (ERDA), nuclear reaction analysis (NRA), and Rutherford backscattering spectroscopy (RBS) can be made in situ and simultaneously with gas permeation through the samples. In the present work, we use a sample similar to, but somewhat different from those used in Refs. 1 and 2: vacuum/CaO/Sr/PdD a ; /D2. Here we report preliminary experimental results on the transmutation diagnosed by conventional XPS method. Results from the in situ analyses will be published later, elsewhere. 272

273

I 0

I 2

I

I

I 4

I 6

l

I 8

l 10

Time [s] Figure 1. (a) Schematic of deuterium permeation in situ accelerator analyses system, (b) the CaO/Sr/PdDj; sample structure, and (c) electrochemical method used for Sr deposition onto the Pd sample.

2. Permeation in situ Analysis System and Sample Preparation The experimental setup is shown in Fig. 1. The multi-layered sample is placed at the center of the vacuum chamber. The sample surface can be diagnosed in situ with probe beam ions to emit characteristic X-rays, which are analyzed either with a CdTe detector or a Si-PIN-type X-ray detector positioned at 150° relative to the probe beam direction. Additional solid-state charged-particle detectors are provided for RBS, ERDA, and/or NRA characterization of the sample. The multi-layered Pd samples were prepared as follows. The Pd sheets of 33 x 33 x 0.1mm 3 were annealed for 3h at 570 K after 1-second immersion in aqua

274

regia/D20. Sr atoms were then deposited on one side of the Pd surface using a method similar to electroplating: as shown in Fig. 1(c), the Pd sheet was carefully placed on the surface of the 10 mM Sr(N03)2/D20 solution, so that only one side of the sheet was in contact with the solution. A bias voltage of 1V was applied between the Pd cathode and a Pt anode wire immersed in the solution. The ion flow onto the Pd cathode was appreciable only at the beginning of the electroplating process, as can be seen in the graph, implying a saturation of the surface with contamination layer containing Sr. Neither further increase in the processing time nor multiple immersions and biasing resulted in any increase in the areal density of Sr deposited. Next, a CaO layer was deposited on the Sr/Pd surface by RF sputtering for 5-20 min. The thickness of the CaO layer was deduced from variation of the XPS spectral intensities. As shown in Fig. 2(a), the peak intensities of Pd-3d and Ca-2p photoelectrons vary with surface etching time. The CaO layer thickness x is calculated from the intensity ratio of these peaks, Ica^p/ypd-sd: using the following equation: exp

, AcaO-Pd J \

1 — exp

*" V

_ AcaO-Ca J J

" P d <7Pd Apd-Pd frba-2p " C a OCa AcaO-Ca ^Pd-3d '

(1)

where n C a , "Pd, cca, opd, ACao-Ca, A Pd _ Pd , and ACao-Pd are the atomic density of Ca and Pd, the differential photoelectron emission cross-section for Ca-2p and Pd-3d, and the mean free path 3 of Ca-2p photoelectrons in the CaO layer, that of Pd-3d photoelectrons in the bulk Pd and that of Pd-3d photoelectrons in the CaO layer, respectively. For samples thicker than several nano meters, an extrapolation of the thickness to the null etching time is necessary to deduce the initial thickness of the CaO layer as shown in Fig. 2(b). Pd-3d

Ca-2p

• A. • •

320

340

360

Binding energy [eV]

380

100

150

Sample#1 Sample#2 Sample#3 Sample#4

200

Etching time[s]

Figure 2. (a) XPS analysis of C a O / P d samples and (b) determination of the CaO layer thickness from the XPS peak intensities.

3. Deuterium Permeation A disc-shaped sample thus prepared with a diameter of 26 mm was placed in the vacuum chamber as shown in Fig. 1. Its rear surface was exposed to D2 gas at a

275

pressure of 0.1 MPa, while the front surface was faced to vacuum with an effective area of 2.5 cm 2 . Variation of the D2 gas pressure after its introduction into the reservoir was monitored to give the number of deuterium atoms absorbed in and/or transmitted through the sample as shown in Fig. 3(a). If the CaO layer acted as a barrier for deuterium permeation to allow negligible transmission into the vacuum, the sample would have become saturated with deuterium, i.e., PdD0.86, at about 100h. This process of deuterium charging is described by a 1-dimensional solution of the diffusion equation for the sample with a thickness and area of a and S, respectively. One side of the sample is opaque for deuterium, while the other faces hydrogen gas to give a boundary condition for the deuterium density; n(a) = noThe number of deuterium atoms absorbed in the sample, Na(t), is given as a function of time by OO

E

Na(t) = aSn0 1

;2s + i ) ^ 2a

exp

(2s-

Dt

(2)

s=0

A characteristic time £i/ 2 for the number of deuterium atoms absorbed to reach a half of the saturation value, i.e., Na(ti/2)/aS = Na(oo)/2aS = 2.9 x 1022 c m - 3 , is therefore given by 0.1967a2 6 x lO's. (3) h/2 — D The observed value is more than three orders of magnitude larger than this value. This fact implies that there is another barrier on the rear surface facing the D2 gas, possibly due to contamination. Figure 3(a) shows that the deuterium flux through the sample should have been about 2.5xl0 1 5 cm 2 /s. After 10 days of permeation with deuterium, desorption of the D 2 gas from the sample was so severe that an outgassing procedure was necessary for the sample

PdD 0.86 ~„ 5

1

1

1

•

1

•

•

|r

1

1

(a) 1

1

1

1

• • •

1

1

1

1

1

1

J-

4

-

3

"

2

- fty

/

\ !

\

^

/

• •

1 50

100 150 Time [h]

200

250

50

100

150 200 Time [h]

Figure 3. (a) Number of D atoms absorbed and/or transmitted during permeation and (b) number of D atoms desorbed from the sample after finishing the permeation procedure.

276

to be introduced into the XPS vacuum system. The sample was then introduced into a vacuum chamber to measure the D2 partial pressure with a quadruple mass spectrometer. Variation of the integrated number of deuterium atoms released during the outgassing in vacuum calculated from the partial pressure is shown as the solid line in Fig. 3(b). The outgas measurement was started 120 h after finishing the permeation. Correction for the release into atmosphere before the measurement have been made by extrapolating the measured variation to time t = 0. The sudden increase at about 150 h is due to a deliberate elevation of the temperature. The total amount of deuterium atoms desorbed from the sample, 8.7 x 10 20 , corresponds to the composition of PdDrj.24- This does not always mean that the whole sample did not saturate with deuterium, when we take account of possible error in the partial pressure measurement. However, the fact that the time necessary for the release of deuterium was also of the order of 100 h again implies that the deuterium flow was recombination limited on both surfaces of the sample during the deuterium permeation.

4

140

160 180 200 220 Binding energy (eV)

(b) _

CaO layer

i • • "•

I < •

k

, Pd layer

w

• 1 " . • . • 1 • f • .

Distance from the CaO/Pd interface [nm]

Figure 4. (a) XPS spectra for the sample before (thin line) and after (thick line) the permeation process and (b) depth profiles of the Sr (solid circle) and Mo (open circle) densities calculated from the XPS peak intensities for the sample before (thin) and after (thick) the permeation process.

4. X P S Analysis after Deuterium Permeation Examples of the XPS analyses of the samples before and after deuterium permeation are compared in Fig. 4(a). The samples were subjected to multiple processes of surface etching followed by analysis, giving the total etching time of 260 s, which corresponds to the probing depth of about 8 nm. We notice that the peak intensity of Mo-3d 5 / 2 photoelectrons has increased drastically after the permeation in exchange for decrease in that of the Sr-3d 5 / 2 . The densities of elements found in the XPS spectra are calculated from the photoelectron yields by the conventional method using the cross-sections with correction taken into account for probability of emission without scattering. 3 These are

277

plotted in Fig. 4(b) as a function of distance from the C a O / P d interface calculated from the relation between the distance and the etching time shown in Fig. 2(b). It is rather clearly indicated t h a t the existence of Mo in exchange for Sr is recognized only near the C a O / P d interface after deuterium permeation. This implies occurrence of nuclear t r a n s m u t a t i o n of Sr to Mo, i.e., Sr atoms with areal density of 4.2 x 1 0 1 4 c m ~ 2 appear to be transformed to Mo atoms of 3.3 x 1 0 1 4 c m - 2 by deuterium permeation. T h e F W H M ' s of the spatial distributions, 2.0-1.0 nm, are consistent with the mean free p a t h s of Sr-3d5/2 and Mo-3ds/ 2 electrons of 3.8 and 3.5 nm, respectively, in C a O , if we take into account t h e statistical error, which is about ± 2 0 % . T h e extended analytical methods are now being prepared, including the in situ accelerator analyses, will be very effective for further study. T h e minimum areal densities of P r and Cs detectable in the upcoming P I X E analysis are estimated to be 4 x 10 1 4 and 2 x 10 1 4 c m " 2 for 100-pyuC/5-MeV a-particle probing. These limiting values of the areal densities have been confirmed by preliminary analyses of an A u / P d sample and a C a O / P d sample.

5.

Summary

Implication of nuclear t r a n s m u t a t i o n of Sr to Mo has been obtained using a system ( v a c u u m / C a O / S r / P d D z / T ^ ) , which is simpler t h a n t h a t of Iwamura et al, with the flow direction reversed. Reproduction of the results is necessary to confirm the transmutation.

References 1. Y. Iwamura, M. Sakano and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4650 (2002). 2. Y. Iwamura, T. Itoh, M. Sakano, S. Kuribayashi, Y. Terada, T. Ishikawa and J. Kasagi, Proc. ICCF11, Marseilles, France (2004). 3. e.g., The Surface Science Society of Japan (ed.); X-ray Photoelectron Spectroscopy (Maruzen, Tokyo, 1998).

HIGH-RESOLUTION M A S S S P E C T R U M FOR D E U T E R I U M ( H Y D R O G E N ) GAS P E R M E A T I N G PALLADIUM FILM

Q I N G M. W E I , X I N G Z. LI A N D BIN LIU Department

of Physics,

Tsinghua University, Beijing lxz-dmp@tsinghua. edu. en

100084,

China

N. M U E L L E R , P. S C H O C H A N D H. O E H R E Inficon

Limited,

LI-9496

Balzers,

Principality

of Liechtenstein,

Yokohoma,

Japan

High-resolution mass spectrometer was used to analyze the gas from a deuterium flux maker. Mass 3 components were analyzed carefully to inspect any anomaly from the deuterium gas permeating a palladium film. Mass 3 component is confirmed again, but more work is needed to separate the signal of the helium-3 (if any) from the heavy background of D - T molecules.

1. Introduction More than 100 years have been past since the discovery of the strong absorption rate of hydrogen in palladium; however, only a little has been revealed about the process of absorption. An experiment based on Hall effect1 showed that hydrogen molecules are dissociated and ionized when they are absorbed in palladium. Usually, it was thought that those hydrogen atoms would be recombined again as molecules when they permeated through the palladium thin film. Thanks to INFICON, experiment has been conducted using the high-resolution mass spectrometer in their R&D laboratory. It has been found that only part of the deuterons were recombined into the deuterium molecules after permeation through the Pd film, most of the deuterons were combined with the residual hydrogen atoms into D-H molecules, and other deuterons remain in the atomic status in the vacuum environment. The mass 3 components were carefully analyzed in order to see if there was any trace of helium-3 or tritium. 2. Apparatus There were two sets of experiments, which were conducted in the INFICON R&D Laboratory. In one set, the palladium tube was heated by the electrical heater at one end of palladium tube. The second set utilized the electrical heater surrounding the palladium film. This paper presents this second set of experiment. A palladium film (020 x 0.1mm) was sealed in a Swagelok connection as Fig. 1. An electrical heater was wrapped around the stainless steel nut to heat the Pd film through the nut. 278

279

Swagelok connection Thermal couple

MkMm

Heating coil

1

D2

Figure 1. A thin palladium film is sealed between two tubes using a Swaglok connection structure. There are two small holes on the nut. Thermal couples are inserted into holes in order to measure the temperature at the edge of the Pd film. The heating coil winding is wrapped around the stainless steel nut to heat the Pd film.

Thermal couples were inserted through the small holes on the nut, and monitored the temperature at the edge of the Pd film. Deuterium gas was fed from both sides of the Pd film, and might be evacuated from both sides using the turbo-molecular pumps (Fig. 2). When the pressure was down to less than 10~ 5 mbar, the system was connected to a high-resolution quadruple mass spectrometer in order to analyze the components of the remaining gas. This QMS422 was designed for running in the second stability zone, which was particularly designed for the operation at low-mass region. It was able to find the D2 molecules in the heavy background of helium-4. Even if the ratio of He:D2 is about 99:1, this QMS422 was still able to clearly distinguish them. 2 For the helium 3, the FWHM resolution of 0.0035 amu and a 10%-peak-height resolution of 0.0065 amu were obtained. 2 Hence, if we were able to produce any trace of helium-3 in the deuterium flux maker, possibly we might be able to find them in the QMS analysis. 3. Experiment One atmosphere deuterium gas was fed into a thin palladium film at 330°C. After 1 h, when the deuterium gas was pumped out, a temperature rising was recorded which is reported in another presentation. 3 In parallel, the outgoing gas was sent to a high-resolution quadruple mass spectrometer. Figure 3 shows the results of the QMS analysis. The first row of Fig. 3 shows the ion currents collected for mass numbers 1, 2, 3, 4, 5, and 6 in each window. The mass number for each peak is shown by the abscissa (multiplied by a factor of 100). The original deuterium was of

280

Figure 2. Schematics of the connection between deuterium flux maker (Pd) and the QMS422. The left-hand side shows the manifold, pumps, and valves, which might feed various gases during the experiment, and measure the volume of the system.

high purity. The mass 2 and mass 3 components in the original deuterium gas were relatively low. There was no signal for mass 5, but a little peak for mass 6. It can be explained as the Longevine effect (i.e. the ion may polarize and dissociate the neutral molecule; then, combine with one of the resultant atoms 4 ). The high concentration of deuterium molecules in the ionization chamber enhanced the reaction channel: D^ + D2 —> D j + D; which is proportional to the square of the concentration of deuterium molecules. Thus mass 6 corresponds to the molecular ion D3". Because the concentration of hydrogen molecules is much lower than that of deuterium molecules; hence, its Longevine effect for reaction channel, Do*" + H2 —> D 2 H + + H, is still negligible. That is, the ion current for mass 5 (D2H + ) is much lower than that of mass 6. The situation changed dramatically, when the gas sample was pumped from the palladium film. The second row of Fig. 3 shows the result of QMS analysis. The mass 4 component is much lower than that of mass 2. It means that most of the deuterons remained in the atomic state (mass 2, D) instead of recombination into molecules (mass 4, D2). The mass 3 peak was almost as high as mass 2. It might be explained as the Longevine effect of reaction channel: D + + H2 —> DH + + H. 5 ' 6 This effect is enhanced because of the high density of D-atoms and some hydro-

281 ffjHypftayr....;

0ri innal Deuterium Gas

(..item JA,

.*)&£&.

, „ „ Ion C m * [A]

lor. Current |Aj

B

'it,y k ,<*'*!*j C» sl>
"'#M

HAJWF I

Ui

"-liiiiil v

">'uu4

" uLMNu

VJJk

DilfL

** ,,-y, 'j t **?,^! i ,^ ,*T.. H JBH'*'»'

^impTe C a ^ f r o i ^ ^ F n

Cfcwte- 5et*l Setup ( . u t r c M [A|

'II ,...„

I ,

0.SO000

|l

1i

22000

o.o?ooo o afisno

20000

006OOO

10000 14000

0*1000-

; 1 1 : ;

0 25000^

o IMSOII

D ZUDOO

& D35O0

00000

w * ;~ if 33 ti> *© ^ P4

Epptsy

3»*K*

ap o

O D 05011 -

* ,y,f^^y,,^li^i,iNa'p''^o*w*'"

, 1 3030

njpfj*

Ji&Sl

S tanwr^f^ffiSSTS

5SWP r-«r>#S»> Ssxtelt* ( r f e r«nt[f- l l f t i

>

Q u n o o D %— 30D 6

J o n C u r r e n t IF

r u m - f i t IF 09A1

I o n C u r n - n l [A,

4U0O 3000 ZOOO-

95 0

IDS II

200 B

203 0

308 S

303 0

Figure 3. Plots of QMS analysis. First row—original deuterium gas; second row—gas sample permeating through P d film; third row—mass 3 peak in linear scale for gas sample permeating through Pd film; fourth row—standard helium 3 gas.

282

gen molecules (H 2 ), which was released from the stainless steel parts of Swagelok connection due to the heating (330°C). However, one might still wonder if there was any helium-3 or tritium involved in peak of the mass 3. In the third row and the fourth row of Fig. 3, standard helium-3 sample was used to calibrate the peak position of mass 3. The logarithmic scale in ordinate was switched to linear scale in order to clearly show the peak position. The third row shows the mass 3 peak from the gas sample permeating from the palladium film, and the fourth row shows the helium-3 peak from the standard helium 3 sample [m(3He) = 3.016], which is on the left-hand side of the mass 3 peak in the third row. It is clear that the major part of mass 3 peak in the third row is from the DH + [m(DH) = 3.021] due to the Longevine effect. The mass 1 peak supports this assumption of residual hydrogen gas during the heating. Nevertheless, we might suspect if any helium-3 was covered by the strong HD peak. In Fig. 4, a careful analysis was done for the strong peak in mass 3. The width of the slot in front of the Faraday collector in QMS was narrowing down gradually in order to improve the resolution further at the cost of reducing sensitivity.

E-13-i

300

I, i , i • i ,

301

302

,

303

304

i

305

Figure 4. Mass 3 peak was re-analyzed in terms of narrowing slot in Faraday collector. A turning point appeared near the 3.016 might imply a trace of helium-3 covered by strong HD peak.

283 Acknowledgments This work is supported by the Natural Science Foundation of China (no. 10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds).

References 1. A.H. Verbruggen et al, Phys. Rev. Lett. 52, 1625 (1984). 2. P.H. Dawson, J. Vac. Sci. Technol. 11(6), 1151 (1974). 3. B. Liu, X.Z. Li et al, in: A. Takahashi, Y. Iwamura, and K. Ota (eds), Proc. ICCF-12, Yokohama, Japan (Nov. 27-Dec. 2, 2005). 4. P. Langevin, Ann. Chem. Phys. 5, 245 (1905). 5. X.Z. Li, G. L. Schmidt and J. Tian, The Proceedings of the 5th Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, Asti, Italy (19-21 March 2004). 6. Q.M. Wei, X.Z. Li et al, in: J.-P. Biberian (ed.), Proc. Iccf-11, Marseilles, France (31 Oct.-5 Nov. 2006, 2004), p. 351.

ICP MS ANALYSIS OF ELECTRODES A N D ELECTROLYTES A F T E R H N 0 3 / H 2 0 ELECTROLYSIS

S. T A N I G U C H I , S. S H I M A D U , H. Y A M A D A A N D S. N A R I T A Department

of Electrical

and Electronic Engineering, Iwate Morioka 020-8551, Japan E-mail: [email protected]

University,

Ueda If-3-5,

T . O D A S H I M A A N D N. T E S H I M A Department

of Chemical

Engineering, Ichinoseki National Takanashi, Ichinoseki 021-8511,

College of Technology, Japan

Hagiso,

T. O H M O R I Advanced

Technology

Inc., Hokkaido Institute Sapporo 006-8585,

Technology, Japan

Maeda

7-15,

Teineku,

We carried out light water electrolysis with Pd cathode and Pt anode. The composition of both electrodes and the electrolytes were analyzed by Inductively Coupled Plasma-Mass Spectrometry to search for the evidence of the nuclear transmutation. In the light water electrolysis experiment, various elements have been observed on the metallic electrodes and in the solution after the electrolysis. In particular, amount of P b increased remarkably after the electrolysis, and this result gave good reproducibility. There was no difference between the isotopic ratio of P b detected and natural one

1. Introduction In light water electrolysis experiments, elements production has been reported. 1 In most of them, only the surface compositions of the electrodes were analyzed. In addition to analysis of the electrodes, it is desirable to investigate electrolytes since elements on/in the electrodes can be dissolved in it. In this study, both solutions of electrodes and electrolyte were analyzed by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS)(SII : SPQ9000). The sample solution introduced into the ICP MS should be acid in general. Then, we utilized HNO3/H2O as electrolytic solution instead of Na2S04/H 2 0 or K2SO4/H2O, that we previously used in our experiment so that the electrolytes can be directly introduced into the device. 2. Experimental We employed a PTEF test cell in this study. The cell is shown in Fig. 1. The cell was 73 mm in diameter, 175 mm of height, and cylindrical shape with volume capacity of 500 ml. The Pd foil (99.95% pure) for cathode was 0.1 x 5x10 mm 3 in 284

285

size and the Pt foil (99.98% pure) for anode was 0.1 x 5 x 10 mm 3 in size. The gap was about 3 cm. A Pd lead wire (4>1 mm) and a Pt lead wire (<j>l mm) were used for connecting cathode and anode to a power supply, respectively. They were coated with Teflon heat-shrinkable tubes. Before the electrolysis, the electrodes were washed with acetone and aqua-regia to remove the impurity. The electrolytes used were ultrapure nitric acid (Ultrapure reagent, Kanto kagaku, Tokyo, Japan). The volume of electrolyte solution was 500 ml. J DC 2 or 1 A

Pt (i|>1 mm) Pd (<|>1 mm)

, Cathode

Pd

^

Anode

3 cm

(0.1 x5x10mm)

< Pt to 1 x5x10mm)

(a)

(b) Figure 1.

P T F E cell.

In the electrolysis, 0.1 M HNO3/H2O was used and DC 1 or 2 A was applied for 14 days. 2 The cell was replenished with ultra pure water of 100-200 ml every day. The electrodes (we call it "After sample") were cut off from the lead wires, after the electrolysis. We prepared reference sample, which was just soaked into the electrolyte for 14days (we call it "Before sample") without supplying the current. We used this cell as an open-cell. The pressure inside cell was kept to be slightly higher than atmospheric pressure during the electrolysis.3 The cell was set in an outer container. Moreover, whole the container was set in a box to avoid contamination. The temperature inside of box was kept constant at 15°C. The elemental analysis of the electrodes and electrolyte was examined by ICP-MS. It can detect the most of elements with high sensitivity (~ppb) and measure the density in the sample for specified elements. It can also evaluate the isotopic abundance. 3. Results and Discussion 3.1. Change in Weight and Thickness

of

Electrodes

In pre-processing of ICP-MS analysis, the Pd and Pt electrodes were immersed in 1 ml of ultra pure nitric acid for 10 s to dissolve most of all the elements on the surface of samples in the nitric acid. Then pure water was added to the nitric acid solution to be totally 50 ml of more thin acid solution for the processing ICP-MS. In the processing, a semi-quantitative and quantitative analysis was done by ICP-MS in this research.

286 Table 1.

Change in weight and thickness of electrode

Current (A)

Pt (before)

P t (after)

Pd (before)

Pd (after)

2 Amount dissolved (mg) 0.04 Depth (nm) 19.0

0.01 4.7

0.56 5.0 X 10 2

0.49 4.0 X 10 2

1 Amount dissolved (mg) Depth (nm)

0.02 9.4

0.20 2.0 x 10 2

0.02 16.4

0.02 9.4

To estimate the depth of samples dissolved in the nitric acid, we compared the weight of samples before the pre-processing with that after the pre-processing. The depth was calculated using the density of the electrodes, 21.37g/cm 3 for Pt and 12.16g/cm 3 for Pd. Table 1 shows the amount dissolved and the depth of Pt and Pd electrodes in HNO3. After treatment by the nitric acid, the dissolved amount for both "Before samples" of Pt and Pd is large than that for "After samples" under the test condition of current 2 A. In case of current 2 A for Pd sample, the dissolved amount 0.56 mg of "Before sample" and that 0.49 mg of "After sample" correspond to dissolved depth 5.0 x 102 and 4.0 x 102 nm, respectively. This indicates that amount of impurity from "After sample" of Pd should be less than that of "Before sample" of Pd. Under the same test condition of 2 A for Pt, similar result can be deduced from comparing weight of "Before sample" with that of "After sample". 3.2. Elements Newly Detected Electrolysis

and Increased

after

HNOz/H^O

All the elements with mass number from 6(Li) to 238(U) can be detected in a run of the ICP-MS with high sensitivity (ppb). In our analysis, the signal stands out when the corresponding element exists with the density above 0.1 ppb. Element Pb was newly detected by the ICP-MS only after electrolysis as shown in Table 2. In particular, marked count of Pb was observed in electrolyte after electrolysis for 1 A. To the contrary, no count was observed on both electrodes and in electrolyte for the "Before samples", as seen in this table. Furthermore, we analyzed the amount of Pb in bulk Pd piece of 29.50 mg and Pt piece of 52.41 mg after each whole piece volume was dissolved in the aqua-regia, and have found no count of Pb in these pieces by Table 2.

Density of P b in the thin nitric acid solutions and electrolytes

Current (A)

Pt (before) (ppb)

Pt (after) (ppb)

Pd (before) (ppb)

Pd (after) (ppb)

Electrolyte (before) (ppb)

Electrolyte (after) (ppb)

Pb 2 1

— —

— 2.7842

— —

9.1406 6.7815

— —

6.401 14.1592

287 8.0

• 2A

6.0

5 4.0 2.0

0.0 Pt (Anode)

Figure 2.

Electrolyte

Amount of P b on the electrodes and in electrolyte.

ICP-MS. It should be noticed that the change in weight of "Before sample" was larger than that of "After sample" for both Pt and Pd electrode, as mentioned above. From these results, it is unlikely that those Pb was impurity originating from bulk Pd and Pt electrodes. Since the volume of electrolyte is 10 times larger than that of the thin acid solution, the amount of Pb in the electrolyte is larger than these on electrodes. On the other hand, the density of Pb in air environment is generally thought to be 0.6 ng/m 3 . 4 Taking account of this low value, the Pb detected in this experiment is not considered to be impurities from the air environment. The deduced amount of Pb from the density values in Table 2, on both electrodes and in the electrolyte, is given in Fig. 2.

3.3. Isotopic

Distribution

of Pb

Table 3 shows counts of Pb on electrodes and in electrolyte after the electrolysis, using ICP-MS. The isotopic distribution deduced from the values in the table is presented in Fig. 3. The isotopic distribution of Pb obtained is close to the natural isotopic one.

Table 3. Count of P b in the thin nitric acid solutions and electrolytes

204

Pb Pb 207 Pb 208 Pb

206

(cps) (cps) (cps) (cps)

Pt (after)

Pd (after)

Electrolyte (after)

526.2 9069.5 8022.0 19429.4

1250.6 23567.1 20306.7 50040.5

3282.3 59884.1 50478.0 128258.3

288

Pt (Anode)

Figure 3.

4.

Pd (Cathode)

Electrolyte

Isotope distribution of P b in the thin nitric acid solutions and electrolytes.

Conclusion

We have analyzed the P d and P t electrodes and H N O 3 / H 2 O electrolyte after the light water electrolysis. (1) No element P b was observed on b o t h electrodes and in electrolyte before the electrolysis. (2) Considerable amount of P b was detected on b o t h electrodes and in electrolyte only after the light water electrolysis. (3) T h e isotopic distribution of P b is close to the n a t u r a l isotopic one. (4) Element P b detected is possible candidate of product resulting from low energy nuclear reaction.

References 1. J. Dash, R. Kopecek, and S. Miguet, The 32nd intersociety energy conversion engineering conference, vol. 2, pp. 1350-1355 (1997). 2. H. Yamada, S. Narita, Y. Fujii, T. Sato, S. Sasaki, and T. Omori, Proc. 9th International Conference on Cold Fusion, pp. 420-423 (2003). 3. T. Sato, S. Sasaki, T. Kubozono, S. Narita, H. Yamada, and T. Ohmori, Proc. J^th Meeting of Japan CF Research Society (October 17-18, 2002), pp. 9-12. 4. The periodic table of the elements, http://home.hiroshima-u.ac.jp/er/ Rmin_GL.html#anchor646130

THE ITALY-JAPAN PROJECT FUNDAMENTAL RESEARCH ON COLD T R A N S M U T A T I O N P R O C E S S FOR T R E A T M E N T OF NUCLEAR WASTES

AKITO TAKAHASHI Osaka University,

2-2 Yamadaoka Suita, Osaka 565-0871, E-mail: [email protected]

Japan

FRANCESCO CELANI INFN,

Via Enrico

Fermi,

40-00044

Frascati

(Rome),

Italy

YASUHIRO IWAMURA Mitsubishi

Heavy Industries

Ltd.,

16-5, Konan Japan

2-chome,

Minato-ku

Tokyo

108-8215,

The IJ Project proposes, as the first phase of research, that confirmation of the cold transmutation using radioactive isotopes such as 1 3 7 C s , 9 0 Sr, and 1 3 6 Cs to non-radioactive elements will be implemented based on the Mitsubishi Heavy Industries, Ltd. (MHI) method. A theoretical background has been given by the TSC-induced nuclear reactions (Proc. ICCF 10). Charge-neutral pseudo-particle of 4d/TSC can become as small as 10 fm radius in its minimum state of squeezing motion, and will make 4D-capture reaction with host metal (or added metal) nuclei in the surface region of permeation {Proc. ICCF 9, 10) samples. Major reaction will be: M(A, Z) + 4 d / T S C - • M(A + 8, Z + 4) + Q. Theoretical modeling of the process is briefly explained and resulting reaction products, their decays and final stable isotopes are predicted for 1 3 7 Cs, 9 0 Sr, and 135 Cs transmutation.

1. Introduction Recent studies on condensed matter nuclear effects in/on near surface regions of metal deuterides and hydrides have provided some confident experimental results about occurrence of cold transmutations in condensed matter containing deuterium and hydrogen. 1_3 Especially the latest works by Iwamura et al.4'5 are novel enough to be considered important new findings in condensed matter nuclear effects. Iwamura et al. have repeatedly shown that there occurs selective transmutation from 133 Cs to 1 4 1 Pr (or 88 Sr to 96 Mo) in the experimental system of D-gas permeation through Pd-complex samples. Pd-complex samples are made with multilayered P d / C a O / P d plates in nm size processing. The IJ-Project aims at confirming the selective transmutation process by using special samples containing radioactive Cs and Sr. This is a pure basic science project. 289

290

2. Selective Transmutation This new type of transmutation is the process of adding 4D or 8 Be to the host element M(A, Z) and to transmute to M'(A+8, Z+A). Therefore, some kind of coherent multi-body process in condensed matter should exist as the underlying physics mechanism. One theoretical interpretation has been proposed by Takahashi. 6 A theoretical background has been given by the TSC-induced nuclear reactions. 3 Charge-neutral pseudo-particle of 4d/TSC can become as small as 10 fm radius in its minimum state of squeezing motion and will make 4D-capture reaction with host metal (or added metal) nuclei in the surface region of permeation 1,2 samples. The major reaction will be: M(A, Z) + 4d/TSC - • M{A + 8, Z + 4) + Q.

(1)

7

Iwamura et al. has also reported that 6D added transmutation. Takahashi 6 has proposed a model for 6D/OSC process to interpret it. If we do experimental tests using radioactive samples of, e.g., 137 Cs, 135 Cs, and 90 Sr to confirm a significant decrease of their radioactivity, the transmutation effect will be clearly confirmed in the view of nuclear science. Then we may consider the possibility of applying the process to the remediation for long-lived radioactive wastes from nuclear plants, although that would require a drastic scale up of transmutation rates compared with the original claim by Iwamura et al. 3. Model of TSC-induced Transmutation According to the Takahashi model of TSC-induced reaction, 4D/TSC at its minimum-size state of squeezing motion may behave as a very small (about 10 fm in diameter) pseudo-particle of neutralized electric charge. A model of formation mechanism on surface of Iwamura sample is shown in Fig. 1. Surface elements analysis by TOF-SIMS by Iwamura 5 and Takahashi 7 revealed that supposed transmutation took place within 10 nm depth zone from surface of Pd-complex sample plate. Figure 1 models some sites like corner holes to provide site for TSC formation. Then TSC squeezing motion produce TSC-minimum-size state of about 10 fm diameter to approach and make strong force exchange with host metal nucleus as shown in Fig. 2. The capture reaction rate for the process of Fig. 2 can be approximately estimated by STTBA. 6 ' 7 For the 133 Cs + 4d/TSC to 1 4 1 P r + Q process, 4.6 x 10 14 Pr-atoms/week/cm 2 is estimated 6 and this value is close to Iwamura results. 4 4. Prediction for Radioactive Samples The reaction scenarios by TSC-induced transmutation predict the following reactions and products for 137 Cs, 135 Cs, and 90 Sr being considered for the IJ-Project. 133

Cs + 4d/TSC -^ 1 4 1 Pr(Ex = 50.49 MeV) -> FPs 141

Pr(stable) + gammas,

or (2)

291

Image of surface Dimer •

/

/o

W

W

w

o _o^o

o• o •

• °„ •o o O

A

° o°

W

•

« U

o! W • -

Adatom

>

*^

o*>«-

Corner-hole with dangling-bonds

°2W TSC is born here?

o

. Pd

CaO

Figure 1.

137

^BF Cs

O Deuteron

Model of surface of Iwamura type sample.

Cs- 4d/TSC -^ 1 4 5 Pr(Ex = 45.63MeV) - • Fission - Products (in 10fs) 145

Pr(5.98 h)

145

or

Nd(stable) + gammas (in few fs).

(3)

During the beta-decay of 1 4 5 Pr with 5.98 h half-life, there should be a small fraction (1%) of gamma-rays at £ 7 = 675.8 and 748.28 keV, which we can detect with HpGe detector to identify the occurrence of reaction (3). 135

Cs + 4d/TSC ^ 1 4 3 Pr(Ex = 48.03 MeV) - • Fission-Products (in f 0 fs) 143

90

or

Pr(f 3.57days) 143 Nd + gamma (in few fs),

(4)

Sr + 4d/TSC ^ 9 S Mo(Ex = 54.71 MeV) -> Fission-Products (in 10 fs) or 98

Mo(stable) + gammas (in few fs).

(5)

For all cases, fission channels may be opened due to very high-excited energies of intermediate compound nuclei. However, we predict gamma transitions will be more dominant than fission, due to shorter transition times (few fs) than about 10 fs life for fission break up by collective deformation of excited nuclei (dumbbell oscillation). Gamma-transition from highly excited states may emit very high-energy gamma quanta in about 50 MeV range. To detect and identify these very high-energy gamma-rays is difficult and money consuming effort is needed, because the process for detection is mostly by Compton scattering and we do not have definite method

292

M-nucleus

Figure 2. Strong interaction (PEF) between TSC-minimum-size and host-metal M-nucleus. The admixture of 4d/TSC forms 8 Be* compound state for short time.

for unfolding broadened pulse height spectra of observation with usual detectors (Nal, Ge, etc.). 5. C o n c l u s i o n s (1) T S C as small neutral pseudo-particle induces nuclear reaction with host metal-nucleus. (2) Cold t r a n s m u t a t i o n by high-energy 4 H e and 8 B e particles by self-fusion of 4 d / T S C is also predicted. (3) Cold t r a n s m u t a t i o n by T S C + Host-nucleus by (1) will be almost nonradioactive. (4) Confirmation by the IJ Project is expected. (5) If confirmed, a scale-up study is expected. References 1. Proc. ICCF9, Tsinhua University Press (see also; http://www.lenr-canr-org/). 2. Proc. ICCF10, Boston (2003) to be published (see also the above site). 3. Proc. ICCF11, Marseilles (2004) to be published (see also the above site and http://www.iscmns.org/). 4. Y. Iwamura et al, Jpn. J. Appl. Phys. 4 1 , 4642 (2002). 5. Y. Iwamura et al., Proc. ICCF10, Boston (2003). 6. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Proc. Siena Workshop, http://www.iscmns.org/ (2005). 7. A. Takahashi, Recent Res. Dev. Phys. 6, 1-28 (2005).

R E P R O D U C I B L E N U C L E A R EMISSIONS FROM Pd/PdOiDa: H E T E R O S T R U C T U R E D U R I N G CONTROLLED E X O T H E R M I C DEUTERIUM DESORPTION

A . G . L I P S O N A N D G.H. M I L E Y University

of Illinois at Urbana- Champaign, Department of Nuclear, Radiological Engineering, Urbana, IL 61801, USA E-mail: [email protected]

Plasma

and

A.S. R O U S S E T S K I P.N. Lebedev Physics

Institute,

Russian

Academy

of Sciences,

Moscow

119285,

Russia

199991,

Russia

A . G . L I P S O N , B . F . L Y A K H O V A N D E.I. S A U N I N Institute

of Physical

Chemistry,

Russian

Academy

of Sciences,

Moscow

Weak nuclear emissions accompanied deuterium loading/deloading into Ti and Pd matrix have been studied for more than a dozen years. PdDa; sample subjected to electrochemical/gas loading or deuterium desorption/deloading generate weak random fluxes of DD-reaction products (neutrons and protons) and energetic alpha particles. However, reproducibility of these emissions was low depending on material quality and experimental conditions. Here we present new reproducible results on DD-reaction products, energetic alpha particles and soft X-ray emissions detected in controlled conditions of exothermic deuterium desorption from the surface of Pd/PdO:Da; heterostructure.

1. Introduction Weak nuclear emissions accompanied deuterium loading/deloading into Ti and Pd matrix have been studied for more than a dozen years. 1 ' 2 It was found that in some cases neutrons and charged particles (protons and tritons) are observed in Pd cathodes during electrolysis, glow discharge bombardment and deuterium desorption from these samples. The rate of those emissions considering as a signature of low-energy DD-reaction is very low and still unpredictable. This indicates low reproducibility of low-energy DD-reaction in deuterium-loaded metals and makes doubtful existence of entire low-energy nuclear processes in non-equilibrium solids. Moreover, the existence of nuclear processes of any type in D-loaded Pd requires observation of X-rays accompanying charged particles braking in solids. So far, there were no unambiguous reports concerning X-ray generation from PdDa; during and after electrochemical loading with deuterium. Meanwhile, earlier we just have reported observation of 2.45 MeV neutrons and high-energy alpha particles during exothermic deuterium desorption from specially 293

294

prepared Pd/PdOiDz heterostructure. 3 ' 4 It was also shown that Pd/PdO samples demonstrate highest screening potential and highest deuterium diffusivity (compared to other metals including pure Pd) in experiments on 2.5-10 keV deuteron bombardment with accelerator. 5 ' 6 These facts allow to assume that Pd/PdO:Da; heterostructure samples could serve as a good candidate to achieve reproducible LENR effects in exothermic deuterium desorption process, including both nuclear and X-ray emissions. Thus, to verify our assumption concerning unique nuclear properties of Pd/PdO:Da; system during D-desorption the objectives of this research were directed to: • Obtain reproducible nuclear emissions in controlled conditions of exothermic D-desorption from PdO/Pd/PdOiDrr heterostructure. • DD-reaction yield (3.0 MeV protons). • Energetic alphas. • Soft X-rays. • Control of sample temperature and D-desorption rate on-line. • To figure out how these emissions could be linked via D-desorption. In the present paper, we show new reproducible results on DD-reaction products, energetic alpha particles and soft X-ray emissions detected in controlled conditions of exothermic deuterium desorption from the surface of Pd/PdChDa, heterostructure. 2. E x p e r i m e n t a l The samples of Pd/PdO were synthesized by thermal growing of thin oxide layer (PdO y ) of 20 nm thick on top of 110 ^m thick annealed cold worked Pd foils (area 2.3 x 1.1cm2) using an oxygen-propane torch. The electrochemical loading of Pd/PdO cathodes by x = D/Pd = 0.7 has been carried out with low current density (j ~ 20mA/cm ) electrolysis in lM-LiOD/D20 solution using a special cell with divided cathode and anodic spaces. Immediately after achieving an x = 0.7 loading ratio, the electrolysis was interrupted. The Pd/PdOiDa, sample with attached CR-39 or thermal luminescent (TLD) detectors is placed under mechanical loading (m = 150 g) for one hour at T = 20°C. During this time the Pd/PdOiDz sample showed signs of heating up to 7.0°C caused by exothermic deuterium desorption. Loading ratio x = D/Pd has been measured using both thermal desorption and anodic polarization techniques. 2 In order to determine x = D/Pd value, the sample was underwent by vacuum heating or anodic polarization after each cathode loading time interval t. About 90% of initial deuterium content was found to be desorbed through Pd-PdO interface during t = 1.0 h. In control experiments a similar Pd/PdO sample electrochemically loaded with hydrogen in 1-M NaOH/H 2 0 electrolyte and exposed to CR-39 detectors has been employed. In blank/background experiments, unloaded Pd/PdO heterostructure samples were used with CR-39.Both open and filtered CR-39 track detectors have been applied in our experiments in order to estimate type and energy distributions of emitted

295

particles. The photo-insensitive X8 LiF TLD (Landauer) units used for soft X-ray detection were filtered by 1-4 layers of 15 /im polypropylene. 3. Experimental Results Kinetics of integral deuterium desorption from Pd/PdO:Da; and its rate for first 70 min after exposure are shown in Fig. la and b, respectively. As seen, the desorption rate demonstrate maximum near t — 10-15 min elapsed after the loading interruption. It was also found that about 90% of all deuterium absorbed by P d / P d O sample leaves heterostructure during 60 min of its exposure at room temperature. During D-desorption the ambient temperature and temperature of the sample were measured simultaneously using to independent thermocouples. It was found that from the start of exposure in air atmosphere (immediately after interruption of loading and drying the sample) the temperature of Pd/PdO:Dir sample jumps five degrees above the ambient one (Fig. 2). The temperature of the sample has tend to increase two degrees more during following 20 min and then exponentially decreases with decrease in loading ratio x = D/Pd and (Fig. la) and desorption rate (Fig. lb). Notice that shape of the Pd/PdO:D:r T(t) (Fig. 2) curve is roughly repeat the shape of desorption rate curve (Fig. lb). The coincidence of T(i) and desorption rate curves give rise to conclusion that observed heating of the sample is referred to exothermic deuterium desorption from the surface of Pd/PdO:Da; heterostructure in air (oxygen) atmosphere. In this condition the PdO surface may catalyze exothermic D + D —> D2 +Q moleculization reaction at room temperature. Pd/PdO:Dj; runs with CR-39 detectors showed a highly reproducible yield of 3 MeV protons from DD-reaction accompanied by energetic alpha emission in the range of 11-16 MeV. These emissions are not detected in the blank experiments with unloaded Pd/PdO heterostructure. Integral charged particle spectra obtained with open CR-39 detectors (without filter) during 12 runs with duration ~ 1 h 0,025

& 0,020 •

x=D/Pd measurement Exponential fit

1 '

3 ' "

0 3

• I •/ I 0,015 . \ 1

Ii

\

§ 0,010

i \ •

D.

° 0,005 o

I—J 1 0,000

0,0-

10

20

30

40

50

60

70

80

• ^

4.1.

i

10

20

—

>

—

i

—

i

30

—

i

40

—

i

—

i

50

Elapsed time (min)

Elapsed time (min)

(a)

(b)

—

i

—

60

70

Fig. 1. Integral deuterium desorption (a) and desorption rate (b) from 110 (an P d / P d O i D x heterostructure electrochemically loaded with deuterium versus elapsed time at T = 18°C. Notice that ~ 90% of absorbed deuterium escapes the sample during 1 h of its exposure.

296

OA m

y •s

0*3 • c.O "

9

2?-

3

•

s

• Sample temperature —•—Room temperature

/i

on. |<«. 0 £

1Q . 1Q , IO ' 17, I / "

11

,

L,_^

0

10

20

,_

30 40 50 60 Elapsed time (min)

.

70

80

Fig. 2. P d / P d O : D i and ambient temperatures vs. elapsed time: Notice that maximal temperature at the surface is ~ 7°C higher than ambient one.

(corresponded to effective time of D-desorption (Fig. 1) for reference (background) Pd/PdO and Foreground Pd/PdO:D.r samples, respectively, are shown in Fig. 3. As seen, background spectrum contains no tracks around 5 /im in diameter and only eight tracks with diameter d < 8.2 /mi. At d > 8.0 fan the background spectrum contains usual alpha counts from radionuclides of radon and toron series presenting in the ambient atmosphere. In contrast, the Foreground spectrum showed three peak areas at d < 8.2/an with total number of counts N = 132, while at larger track diameters the number of counts is quite comparable with background. Accordingly to our earlier data and accelerator calibration of CR-39 with proton

n 50-

I—T| Foreground measurement, open CR-39 Pd/PdO:Dx: ?=12x 62.5 min ^ H

E 40o. (0

30-

background measurement, open CR-39 Pd/PdO: r= 12x62.5 min 4.8 < d < 12.0 urn: ^(fg) _ 2 0 0 c m - 2 . w ( b j =

3 MeV p d(d P)t

'

c

20-

n

d<8.2m: A/(Fg) = 132 cm - 2 , A/(bg) = 8 cm - 2

I

u TO

100-

5 5 cm-2

$ nfl 7

fl „nii{1mn jnnJJin—JTlTTlrfl^in^nrflfr

8

9

10

11

Track diameter (urn) Fig. 3. Foreground and background counts from P d / P d O : D x and P d / P d O , respectively: open CR-39 detector. Pay attention to high foreground/background ratio, especially below d = 8/im.

297

and alpha beams 3 ' 4 the maximum near d = 5 fim belongs to 3 MeV protons; the group of counts near d = 6.2 fim can be ascribed to lower energy protons/deuterons ( £ , / E d ~ 1.7/2.8 MeV) and counts around d = 7.2 fim were associated with highenergy alphas in the range of 11-16 MeV. In order to confirm our assumption concerning presence of 3 MeV protons as DD-reaction signature we compared open CR-39 spectra for Pd/PdO:Drr and Pd/PdO:Ha; samples (Fig. 4). As seen from Fig. 4, the spectra of Pd/PdO:D.Tand Pd/PdO:Ha;look similar with only one exclusion: there are no counts at d < 6 /an have been found for Pd/PdO:Hx heterostructure. Thus, the group of counts associated with 5 fim peak belongs only to deuterated P d / P d O sample. This peculiarity confirms our assumption concerning emission of 3 MeV protons (DD-reaction signature) in Pd/PdO:Da; heterostructure. On the other hand, the groups of counts around 6.2 and 7-2 fim are appeared in both Pd/PdO:Dz and Pd/PdO:Ha; samples . This fact does not contradict to our earlier data showing presence of energetic alpha and proton/deuteron emissions independently on hydrogen or deuterium loading in Pd/PdO.

5040-

[Pd/PdO:Dx-Pd/PdO], open CR-39 (Pd/PdO:Hx-Pd/PdO], open CR-39

.•e 3 0 -

A4>

10

11

Track diameter (urn) Fig. 4. Comparison of P d / P d O : D x a n d P d / P d O : H x track distribution (with background P d / P d O counts subtraction): Main difference is t h e ~ 5/tm peak in P d / P d O i D * . No such peak in Pd/PdO:Hs.

In order to present further proofs of proton and alpha emissions in Pd/PdO: Dx and Pd/PdO:H.T samples we performed special runs with CR-39 detectors filtered with 11 and 44 fim Al foils and 25 fim Cu foil. In Fig. 5, the background Pd/PdO and foreground Pd/PdO:Dx charged particle spectra obtained with CR-39 detector filtered with 44 fim Al is presented. The main peculiarities of this Pd/PdO:Da; spectrum (Fig. 5) compared with that taken with open CR-39 detector are shift of d = 5.0 fim band (see Fig. 3) to the group of counts over d = 5.6-6.2/tm and splitting of d = 7.2 fim alpha band to 7.3-8.0 mn track diameters. The shift of 5 fim band for CR-39 filtered with 44 fim

298 3MeVp

I I

40 • E ~30

I Foreground: CR-39/44 um Al, Pd/PdO:DxTD, 1= 12 x 62.5 min I Background: CR-39/44 um Al, Pd/PdO, f= 12x62.5 min

14-16 MeV alpha 4.8 < d < 12.0 um: N(ig) = 214 cm" 2 , N{bg) = 48 cm - 2 ; d<8.2 um: A/(fg)=124; A/(bg) = 11

in

c

CD

•o J*

20-

u re

10-

11-12 MeV alpha

Dv 5

6

jllLrji 7

8

9

10

11

Track diameter (um) Fig. 5. CR-39 charged particle spectra of background P d / P d O and foreground P d / P d O : D i samples with 44 /im Al filter. Compared to open CR-39: shift of DD-proton track band from 5 to 5.6-6.2 /im diameters; splitting of alpha track band from 7.2 to 7.3-8 /im diameters. Note large F g / B g ratio at d < 8/im.

Al foil is in good agreement with 3.0 MeV proton stopping range in Al. The splitting of 7.2 /an maximum in open detector to 7.3 and 8.0 [im bands indicates appearance of two groups of alphas with the energies ranging near 12 and 14-16 MeV. This result is in agreement with our earlier data on energetic alpha emissions obtained for Pd:D(H) and Ti:D(H) foils.3-4 Presence of 1.7 MeV protons per 2.8 MeV deuterons in charged particle spectra of Pd/PdO:Ha; and Pd/PdO:Da; is supported by experiments with 11 /tm Al filtered CR-39 (Fig. 6). Shift of 6 /mi track band (open detector, see Fig. 4) to 6.4-6.6 /<m after application of 11 /im Al foil for Pd/PdO:H(D)a; is consistent with emission of 1.6 ± 0.2 MeV protons (Pd/PdO:Hx) and/or 2.8 ±0.4 MeV deuterons (Pd/PdO:Dx). The other example of charged particle filtering with 25 urn Cu foil for both Pd/PdO:Dz and Pd/PdO:Hz samples is shown in Fig. 7: As seen from Fig. 6 the 3.0 MeV proton band in Pd/PdO:D.T shifts further compared to the run with 44 /an Al filter to diameter ranging d = 6.2-6.6 /mi. This shift is expected accordingly to stopping range of 3.0 MeV protons in copper. Notice that no counts were detected in this range for Pd/PdO:H.T sample. The shifts and amplitudes of alpha particle spectra for both H and D-loaded Pd/PdO samples look similar and indicate presence of the same groups of alphas with energies 11-12 MeV (9.2-9.8 um band) and 14-16 MeV(7.4-7.6 /tm band) as were detected in experiment with 44 um Al filter. The shift of 5.0 um proton band (open CR-39) with respect to thickness of Al and Cu filters is shown in Fig. 7.

299

Pd/PdO:Hx, CR-39/11um A Pd/PdO:Dx, CR-39/11umA

307 25E o 20-

|

15H

I 1(H o ra

5lijin

0 -5^

6

7

8

9

10 ' 11

'1

Track diameter (um) Fig. 6. CR-39 charged particle spectra of P d / P d O : D z and P d / P d O : H i samples filtered with 11 )im Al foil.

This picture finally show that band of d = 5.0/zm detected by open CR-39 corresponds to protons of 3.0 ± 0.3 MeV initial energy emitted from near-surface layer of Pd/PdO:D.T. Estimated energies after passing the metal filters are consistent with the stopping power of these Al and Cu filters resulting in shift of d = 5 /an peak (open CR-39) to larger diameters. At the same time we did not find any direct sign of energetic triton (E ~ 1 MeV) emission in Pd/PdO:Da; that could be considered as an additional signature of d(d,p)t reaction. The absence of energetic tritons indicates that effective depth beneath the PdO:Dx surface where DD-reaction occurs would be h < 2.0/an. At depth h — 2.0/<m the effective energy losses of 1 MeV triton in Pd is estimated as A.E ~ 0.6 MeV resulting in very low initial energy

30 [Pd/PdO:DX-Pd/PdO], CR-39/25 (im Cu

25

1 20

f I

[Pd/PdO:HX-Pd/PdO], CR-39/25 (im Cu

15 10 5 0 Track diameter (um)

Fig. 7. Charged particle spectra for P d / P d O : D z and P d / P d O : H i filtered with 25 (im Cu (with background subtraction). Alpha particle spectra of both H and D-loaded samples look similar.

300

of triton bombarding CR-39 surface {Et = 0.4 MeV). The stopping range of this triton in CR-39 material is too small (several microns) compared to etched layer of detector at etching time t = 7 h (9.1 um). As a result we cannot detect triton tracks at this effective depth of DD-reaction. At the same time at h — 2.0 /zm in Pd/PdO:D.T the proton energy would be Ep ~ 2.85 MeV that is consistent with our estimate shown in Fig. 8. This explanation makes us still convinced in DD-reaction, which is occurred in Pd/PdO:D.T heterostracture at some effective depth. Thus, exothermic deuterium desorption from Pd/PdO:D.i-heteiostructure causes a reproducible yield of DD-reaction from near-surface layer with depth ~ 2 /im. Taking into account detection efficiency e = 1/2(1 —cos0 C ), where 0 C is the critical angle for 3 MeV protons (32-37°, Ref. 7) we obtain this yield as Yp(DD) = (1.15± 0.13) x 1 0 - 2 p/s-cm 2 . The yield of 3 MeV proton is by order of magnitude in agreement with 2.45 MeV neutron yield obtained with NE-213 detector pair for similar samples during D-desorption: Yn(DD) = (1.8 ±0.19) x 1 0 - 2 n/s-sample. 2 Notice that calculated mean D-desorption rate from Pd/PdO:D.i; surface (Fig. 1) or deuteron current (D+) from the sample is found to be {AN/At) = 20 niA/cm . The DD-reaction yield in that case was Y(DD) = 0.5p/C(D). This result suggests very high screening potential Ue > 1.0 keV in Pd/PdO:Da; that exceeds the value of Ue deduced for PdO from accelerator experiment. 6 The process of exothermic deuterium/hydrogen desorption is also responsible for triggering of energetic alpha (11 16 MeV) and 1.6 MeV proton emissions in Pd/PdO:D(H).x- heteiostructure cathodes. This finding only confirms our previous CR-39-open CR-39 + 11 umAI CR-39 + 44 um Al CR-39 + 25 umCu

3.0± 0.3 MeV 50-

1.85± 0.35 MeV 40(0 £ 0) T3 O (0

30-

2.8±0.2 MeV

1.3 ±0.3 MeV

2010-

!•••••••* 5,0

5,5

6,0

M 6,5

7,0

Track diameter (um) Fig. 8.

Proton band position versus CR-39 filter thickness and quality.

301

data on energetic charged particle emissions obtained for non-equilibrium metal hydrides/deuterides at electrolysis, glow discharge or laser bombardment. 3 Below we show briefly the results for energetic alpha emission during exothermic D/H desorption from Pd/PdO:D(H):r samples: • Using critical angles of 1-16 MeV alphas G c = 42° we obtain the yield of energetic alpha particles in Pd/PdO:Da; during exothermic D-desorption Ya = (5.5 ± 0.9) x 10" 3 a/s in 4TT ster. • Pd/PdO:Ha; samples during H-desorption demonstrate 11-16 MeV spectra that are very similar to that of Pd/PdO:Da;. The magnitude of alpha yield during H-desorption is also similar to that during D-desorption case. • Reproducibility of both DD-reaction and energetic alpha emissions during D-desorption is close to 100%. In this research we have found that nuclear emissions from the surface of Pd/PdO:Da; heterostructure cathode during exothermic deuterium desorption are accompanying by soft X-ray emission. The X-ray TLD measurements (five pairs of X8 LiF TLD with various filter thickness) performed with Pd/PdO:Dx sample showed non-negligible X-ray dose in foreground TLD chips (attached to the Pd/PdO:Dx sample) compared with background detectors. In Fig. 9, the transmission of PPE filters (that covers TLD pair) with respect to detected X-ray quanta is given as a function of PPE filter thickness: X-ray transmission dependence vs. PPE filter thickness allows to reconstruct initial energy of X-ray quanta emitted from the surface of Pd/PdO:Da; cathode

1

>~

•

s 1-22

•:

:

1.0- 1 ,

«5

:

s

:

;

X8-LiF TLD/PPE filters Fit: lh/l0 = exp(-nmhppE) nm(PPE) = 893 cm"1 .. <Ex> = 1.30 ± 0.15 keV = 8.0 ± 2.0 X/s-cm 2 in An ster.

1%, 0 , 8 c" o

0,6 -

8

0,4-

c

0,2-

-j-

11 1rv^^

<0

•"

_£

0,0-0,2-

1

10

i

i

1

1

1

20

30

40

50

60

PPE filter thickness, h (|im) Fig. 9. Transmission of polypropylene filters (a = Ih/Io, where 1^ is the X-ray dose in TLD filtered with P P E of h /an thick and IQ is the X-ray dose in an open TLD at h = 0) versus thickness of P P E filter.

302

during exothermic D-desorption (Fig. 9). The fit of transmission curve showed mass-absorption coefficient /i(PPE) = 893 c m - 1 , corresponding to mean energy of X-ray quanta (Ex) = 1.30 ± 0.15 keV. The open TLD showed dose D = 12 ± 2 mrad = 120 /uGy with background subtracted (£>(Fg) = 21.0 ± 1.0mrad, D(Bg) = 9.0 ± 1.0mrad). In SI system the equation connecting the dose Dx (Gy) absorbed by LiF TLD with area s = 0.04 cm2 and mean flux ($>x) would be written as follows:8 (*„,) = 2 D a ; p ( L i F ) / 1 . 6 x l O - 1 3 ( J / M e V ) x J E ; ; E X / i m x ( s / l c m 2 ) T ^ (8 ± 2)X - quanta/cm 2 - s, where /a(LiF) is the density of LiF, Ex = 1.3 keV is the X-ray quanta energy and r = 7 x 105 s is the total time of TLD exposure with Pd/PdO:Da; sample; /um(1.3keV) = 7 x 10 5 cm 2 /g is the LiF mass-absorption coefficient for 1.3 keV quanta obtained by extrapolation of known data in the range of 4-10 keV to lower energies.8 Note that estimated dose obtained from the charged particle absorption by LiF TLD (i.e., emitted from the surface of Pd/PdO:Da;) would be less than 1 mrad (below detection limit). Thus, here we first detected soft X-ray emission accompanying the exothermic deuterium desorption from the Pd/PdO:D:r heterostructure cathode alongside with charged particles and estimated energy of those X-ray quanta. 4. Conclusions Thus in this research the following new results have been achieved. • Good reproducibility of charged particle emissions during controlled exothermic D-desorption from Pd/PdO:Da;. • Relatively high 3 MeV proton yield indicating large DD-reaction enhancement during D-desorption. • No direct sign of 1 MeV tritons: means that effective depth where DDreaction originates is ~2 /an from the surface. This estimate is in good agreement with energy losses for 3 MeV protons • Identity between energetic alphas spectra resulting of D and H-desorption from Pd/PdO. • The energy of X-ray quanta emitted from Pd/PdO:Da; is in good agreement with Karabut's glow discharge results. 4 This suggests similar mechanism of X-ray emission caused by D-desorption. • Phonon energy of D-desorption focusing or/and concentration in some specific lattice sites near surface (the sites of a high internal strain?). • DD-reaction, energetic alphas and X-ray emissions suggest anomalous energy release via the "active" lattice sites of non-equilibrium metal deuterides.

303

Entire results showed t h a t exothermic D-desorption is t h a t obvious link between DD-screening, soft X-ray emission and high energy alpha generation from the surface of P d / P d O : D x .

References 1. 2. 3. 4. 5. 6. 7. 8.

S.E. Jones et al, in ICCF 10 Proc, Boston, MA, 24-30 August. 2003 A.G. Lipson et al, Fusion Tech. 38, 257 (2000). A.G. Lipson et al, in ICCF 10 Proc, Boston, MA, 24-30 August, 2003. A.G. Lipson et al., JETP 100, 1175 (2005). H. Yuki et al, JETP Lett. 68(11) , 785 (1998). J. Kasagi et al, J. Phys. Soc. Jpn. 71(12), 2881-2885 (2002). B. Dorschel et al., Rad. Measurements 3 1 , 103 (1999). H. Cember, Introduction to Health Physics, 2nd ed., Pergamon Press, New York, 1985.

C O R R E C T IDENTIFICATION OF E N E R G E T I C A L P H A A N D P R O T O N T R A C K S I N E X P E R I M E N T S O N CR-39 C H A R G E D PARTICLE D E T E C T I O N D U R I N G H Y D R O G E N D E S O R P T I O N FROM Pd/PdOtHa H E T E R O S T R U C T U R E

A.S. R O U S S E T S K I P.N. Lebedev Physical

Institute, Russian Academy of Sciences, E-mail [email protected]

Moscow,

119991

Russia

A.G. L I P S O N Department of Nuclear, Plasma Urbana, IL 61801, USA; Institute

and Radiological Engineering, University of Physical Chemistry, Russian Academy Moscow 117915, Russia

of of

Illinois, Sciences,

B . F . L Y A K H O V A N D E.I. S A U N I N Institute

of Physical

Chemistry,

Russian

Academy

of Sciences,

Moscow

117915,

Russia

Results of correct identification of energetic alpha and proton tracks, observed after hydrogen desorption from P d / P d O : ! ! ^ samples, are presented. Using CR-39 plastic track detector we unambiguously identified tracks of as minimum two groups of alpha particles with energies 10—13 and 15—17.5 MeV. It was also confirmed the emission of protons with energies ~1.7—1.9 MeV.

1. Introduction Earlier experiments 1 ' 2 have showed emissions of energetic charged particles (a-particles and protons) during exothermic H desorption from the Pd/PdOiH^ heterostructures. The occurrence of these emissions was confirmed by independent experiments using both Si-surface barrier and CR-39 plastic track detectors. Earlier we already showed that purified CR-39 plastic track detectors can be considered as an adequate scientific instrument, which suitable for detection of individual uniformly distributed charged particles and also for the groups of these particles being emitted from the active spots ("hot zones") attributed to the maximum internal strain area at the surface of Pd/Ti:D samples. The analysis of CR-39 data showed that in some cases energetic charged particle tracks (a-particles and protons) concentrated inside the small spots of detector. The typical "hot zone" with <~102 tracks within the area with the size of 0.25 x 0.5 mm 2 were found to be appeared during the hydrogen desorption experiments with Pd/PdOrH-,; samples.2 In present work we demonstrate the advance of track detection technique allowing perform an unambiguous identification of CR-39 tracks in order to obtain 304

305

full information about type and energy of detected particles as well as to distinguish them from usual background events and surface defects 2. Experimental Technique Track parameters (coordinates and diameters) measurements have been carried out with automated microscope facility (PAVICOM).2-3 In order to obtain correct particle identification, in-depth track etching and comparison of their parameters (including diameters and etching rates) with those for calibration tracks (obtained with accelerator alpha and proton bombardment of CR-39) have been performed. The detectors were etched in 6N solution of NaOH at 70°C, during the time intervals corresponded to 7, 14, 21, 28, and 35 h. After the etching during every specific time interval, the diameters were measured for each individually selected track. Thus, the measurements of parameters for individual tracks in the "hot zone" and calibration detectors were carried out after each 7 h of etching. Using the results of these measurements we plotted the functions of track opening diameter versus etching time and the rate of etching inside the track versus removed layer depth. 4 The results of calibration (the dependence of track diameter from etching time) for a-particles and protons are presented in Figs. 1 and 2, respectively. In this experiment, we used the sample of Pd/PdOtH^ heterostructure with the thickness of 50 ^m that was loaded by hydrogen during electrolysis in solution 1M Li2S04/H20 during 20 min (current density j = 10 mA/cm 2 ). After electrolysis, the sample was attached to the CR-39 detector with shielding of 11 fj,ra of Al. After ~ 1 h of exposition, the sample was repeatedly loaded by hydrogen during electrolysis. Then the cycle of measurements was repeated 10 times. Total time of exposition was 14 h.

Figure 1. Calibration dependence of track diameter of alpha-particles versus etching time with their logarithmic approximation.

306

13,5 13,0 12,5-] 12,0-1 11,5

11,(H 10,5 10,0-1 9,5 9,0-1 8,5 8,0 7,5 7,0-1 6,5 6,0 5,5 5,0 4,5 10

15

20

25

30

35

Etching time (h)

Figure 2. Calibration dependence of track diameter of protons versus etching time with their linear approximation.

3. Results and Discussion It was found that tracks of charged particles distributed both uniformly on the detector plane and concentrated in some zones with high track density ("hot zones"). The photomicrographs with tracks of a-particles and protons in the "hot zone" with dimensions of 250 x 500 /im 2 are presented in Fig. 3a,b. We detected ~200 tracks spaced on the small area. Such close displacement of tracks allows us correctly come back to individual each track after repeated etching and reconstruct track etch dynamic. After comparison this dynamic with that of calibration alpha-particles and protons, we can to unambiguously identify type and energy of individual particles. Figure 4 demonstrates etch dynamic of some spot in hot zone. The measurements were carried out after 7, 14, 21, 28, and 35 h of etching. We measured the diameter of tracks that have more circular shape so their angle of incidence was

Figure 3. Photomicrographs of tracks in "hot zone" with dimensions of 250x500 |im 2 . Image size~120x90 /im 2 .

307

ۥ 4**-

lb*

k •%&

(d)

(c)

(b) I

(a)

*r^

I

3r

&

(e)

Figure 4. Etch dynamic of spot with coordinates [-71, -1972] at etching time (a) 7 h, (b) 14 h, (c) 21 h, (d) 28 h, and (e) 35 h.

close to normal and we can to compare them with calibration tracks. Track 1 looks like proton candidate. The comparison of track etch dynamic of track 1 from Fig. 4 with that for 1 and 1.5 MeV calibration protons is shown in Fig. 5. Figure 6 demonstrates the comparison of functions track diameter versus etching time for track 1 with one of 1 and 1.5 MeV calibration protons. The dependence of track diameter from etching time for protons was found to be linear. According to our estimation track 1 belongs to proton with energy 1.35 MeV. Pictures in Fig. 7 demonstrates etch dynamic of another spot with coordinates [-116,-1621]. We choose track 1 as alpha particle candidate. The comparison of

1 MeV proton

I [-71 ;-1972], track 1

1.5 MeV proton

Figure 5. Comparison of track etch dynamic of track 1 from Fig. 4 with that of 1 and 1.5 MeV proton calibration tracks. Etching time: 7, 14, 21, 28 and 35 h from left to right.

308

Track diameters vs. etch time: proton-like tracks #

1 MeV proton

•

1.5 MeV proton

&, #1 [-71 ,-1972]

-Linear (1 MeV proton) -Linear (1.5 MeV proton)

10

20 Etch time (h)

Linear (#1 [71,-1972])

Figure 6. Comparison of function track diameter versus etching time for track 1 from spot [-71,1972] with one of 1 and 1.5 MeV calibration protons.

track etch dynamic of track 1 with one of 11 and 12.8 MeV alpha particle calibration tracks is shown in Fig. 8. The comparison of functions track diameter versus etching time for track 1 with one of 11 and 12.8 MeV calibration alpha-particles are presented in Fig. 9. The dependence of track diameter from etching time for alpha particles was found to be logarithmic. Another important function for track identification is dependence of track etch rate from removable depth. In simple model of track formation 4?5 track etch rate Vtj bulk etch rate VJ> connected with track diameter D and removable depth h by formula: Vt/V„ = phf

- D 2 ]/[(2/i) 2 + D'\.

It* ^ K ,

M

Figure 7. Etch dynamic of spot with coordinates [-116,-1621]. Etching time: 7, 14, 21, 28, and 35 h from left to right.

309

fe.#

'

-

• 12.8 MeV alphas

1

Trackl [-116,-1621]

^•IKSif

* 11 MeV alphas

Figure 8. Comparison of track etch dynamic of track 1 from Fig. 7 with that of 11 and 12.8 MeV alpha calibration tracks. Etching time: 7, 14, 21, 28 and 35 h from left to right.

Here h = Vbtj where t is the etching time. Vb = 1.3 /xm/h.

For our conditions of etching

Comparison of track #1 [-116, -1621] etching dynamics with that for 11 and 12.8 MeV alphas 30Alphas £=11 MeV

25 s,9?43 20 2

R ^ 0,9508

Alphas £=12.8 MeV

15

Track #1 [-116-1621]

10

Log. (alphas £=12.8 MeV) Log. (alphas £=11 MeV)

10

Figure 9. alphas.

20 30 Etching time (h)

—1

Log. (track #1 [-116-1621])

40

Comparison of track 1 from spot [-116,-1621] etch dynamic with that of calibration

310

The comparison of functions track etch rate versus removable depth for alpha candidate mentioned above and 11 and 12.8 MeV calibration alphas is presented in Fig. 10. We estimate that track 1 [-116,-1621] belongs to alpha particle with energy ~12 MeV. Another example of identification of high energy alpha track will be showed bellow (see Fig. 11). The comparison of etch dynamic of track 1 from spot [-433,-2285] with that of 12.8 and 16.7 calibration alphas is presented in Fig. 12. The comparison of functions track etch rate versus removable depth for alpha candidate mentioned above and 16.7 and 12.8 MeV calibration alphas is presented in Fig. 12. We estimate that this track belongs to alpha particle with energy ~16 MeV. The track diameter distributions of tracks inside hot zone for 7 and 35 h of etching are showed in Fig. 13a and b, respectively. There are three peaks for track diameter distribution with 7 h of etching (Fig. 13a). By longer etching time (35 h) they are shifted and splintered a few bands (Fig. 13b). Thus we can estimate the energies of these particles with more high accuracy. On the distribution in Fig. 13b the peaks, that corresponded protons with energy ~1.5 MeV, possible 1.35 MeV protons or 18.8 MeV alphas, alphas with energies 16.6; 16; 14.1; 12; 10.6; 10.2; 9.2 MeV, are observed. The main peak is under question because it is belongs to both alpha particle and proton range of diameters. The same track diameter distributions were obtained for all surface of detector

Rate of track etching Vt vs. removed depth of CR-39 for 11 and 12.8 MeV alphas and track #1 [-116,-1621] at Vb = 1.3 m/h Alphas, £=11 MeV Alphas, £=12.8 MeV Track #1, [-116,-1621] Log. (alphas, £=12.8 MeV) Log. (alphas, £=11 MeV) - Log. (track #1, [-116,-1621])

0.9422 10

20 30 40 Removed depth (jim)

50

Figure 10. Track etching rate versus removed depth for track 1 from spot [-116,-1621] , 11 and 12.8 MeV calibration alphas.

311

*%B.

5 : "A %w*t12.8 MeV alphas

mm mi &

•

"

«

[-433;-2285], track

'VST%

16.7 MeV alphas Figure 11. Comparison of track etch dynamic of track 1 from spot [-433,-2285] with that of 11 and 12.8 MeV alpha calibration tracks. Etching time - 7, 14, 21, 28 and 35 h from left to right.

~ 1 cm 2 (see Fig. 14). You can see that track diameters are distributed in the same bands like in Fig. 13. This is the proof of that the charge particle emission (with energies mentioned above) took place not only in "hot zone" but also was on all surface of sample.

Track diameter vs. etching time: comparison of high energy alphas and track #1[-433, ] kinetics: £(track#1)~16 MeV 22

A

^J

8

MeV

£

A

Alpha 16.7 MeV

I14

mm

—IBI— Track #1

T3

10

-*

18 27 Etching time (h) Figure 12. alphas.

Alpha 12.8

Alpha 20 MeV

36

Comparison of track 1 from spot [-433,-2285] etch dynamic with that of calibration

312

' F . ^ A I Pd/PdO'Hx, S=250«500 |im, CR-39/5.0nm Al | Exothermic H-desorptton Buret of emissions (photo)

j Pd/PdO:Hx, S=250x500 microns, etching time - 35 h

p1.35ora18.8MeV(?)

5

ft]

,JEL„ 12

14

16

Track diameter (urn)

Figure 13.

18 20 22 24 26 Track diameter (nm)

28

30

Track diameter distributions in "hot zone" after 7 h (a) and 35 h (b) of etching.

4. Conclusion • We unambiguously identified tracks of as minimum two groups of alpha particles with energies 10-13 and 15-17.5 MeV. The emission of such alphas was previously measured by CR-39 detectors with different shielding. • We confirmed the emission of protons with energies ~1.7-1.9 MeV during of exothermic hydrogen desorption from Pd/PdO:H K samples. • The comparison of track etch dynamic of calibration alpha particles and protons including functions D = /(£) and Vt = f(h) with that of individual tracks, unambiguously confirms the effect of energetic charged particle emission from surface of metals with high affinity to hydrogen. • Method of track depth measurement to improve the energy resolution and separation different types of particles is on the way.

Pd/PdO:H x , Sdet = 1 cm 2 , etching time - 35 h ! Pd/PdO:H x , Sdet = 1 crrT, etching time - 7 h 50 » 40 o |

30

CO

f 20-I z 10-

0 -t-i,.. -i X

flpPfr

6,0

7,0 7,5 8,0 8,5 Track diameter (urn)

6,5

an-

9,0

12

14

16

18

20

22

24

26

28

30

Track diameter (|im)

Figure 14. Track diameter distributions on 1 cm 2 of detector (including "hot zone") after 7 h (a) and 35 h (b) of etching.

313

References 1. 2. 3. 4. 5.

A.G. Lipson et al., Fusion Technology 38, 238 (2000). A.S. Roussetski, Proc. of ICCF-11, Marseilles, France (2004). A.B. Aleksandrov et al, Nucl. Instr. and Meth. A535 542-545 (2004). B. Dorschel et al., Radiation Measurements 31 103-108 (1999). D. Nicezic and K.N. Yu. Materials, Science and Engineering, R(46) 51-123 (2004).

I N T E N S E N O N - L I N E A R SOFT X-RAY EMISSION FROM A H Y D R I D E TARGET D U R I N G P U L S E D D B O M B A R D M E N T

G E O R G E H. M I L E Y , Y A N G Y A N G , A N D R E I L I P S O N , M U N I M A H A Q U E A N D IAN P E R C E L Department

of Nuclear, Plasma and Radiological Engineering, University 103 S. Goodwin Ave., Urbana, IL 61801, USA. E-mail: ghmiley@uiuc. edu

of

Illinois,

MICHAEL ROMER Department

of Electrical and Computer Engineering, University 1406 W. Green St., Urbana, IL 61801, USA.

of

Illinois,

Radiation emission from low-energy nuclear radiation (LENR) electrodes (both charged-particle and X-rays) represents an important feature of LENR in general. Here, calibration, measurement techniques, and soft X-ray emission results from deuterium bombardment of a Pd target (cathode) placed in a pulsed deuterium glow discharge (PGD) are described. An X-ray intensity of 13.4mW/cm 2 and a dose of 3 . 3 ^ J / c m 2 were calculated over a 0.5 ms pulse time from AXUV photodiode radiation detector measurements. A most striking feature is that X-ray energies >600V are observed with a discharge voltage only about half of that value. To further investigate this phenomenon, emission during room temperature D-desorption from electrolytically loaded Pd:Dx cathodes was also studied. The X-ray emission energy observed was quite similar to the PGD case. However, the intensity in this case was almost 13 orders of magnitude lower due to the much lower deuterium fluxes involved.

1. Introduction Karabut in the LUTCH Laboratory in Russia recently reported X-ray laser (~1.5keV) emission from metal targets such as Ti and Pd, which served as the cathode in a high-current pulsed deuterium glow discharge (PGD) plasma diode. 1 ' 2 Later, he vividly demonstrated the potential capability of this type of laser with a small follow-up 10 W "prototype" unit, which "drilled" a 9 mm diameter hole in a 3 cm thick plastic target. This remarkable unit is more compact and provides a shorter wavelength than any prior "table top" X-ray laser. Staff at the University of Illinois at Urbana-Champaign (UIUC) have undertaken theoretical and experimental studies of the mechanisms involved in this unique X-ray emission phenomenon. 2 ' 3 In UIUC's experiments, it was established that anomalous X-ray emission is observed during PGD operation at a pressure of 0.1-0.5 Torr and at a spacing of about 4.0 mm between the cathode and anode. The current pulses have a square shape 314

315

with 0.2-2.0 ms duration and a rise time of 0.1 /xs. The glow discharge operated at a voltage as low as 300 V with a pulsed current up to 2 A. These crucial conditions are similar to those in Karabut's earlier studies, 1,2 but the voltage operation down to 300 V represents a new region. This paper will briefly describe the UIUC pulsed deuterium bombardment glow discharge project. The X-ray diagnostics employed and their calibration will be discussed. The calibration will be applied to discharge data to determine the power, intensity, dosage, and efficiency of the X-ray observed. Finally a brief discussion is given of related experiments using a deuterium flux created by desorption of D loaded in a Pd target electrolytically. These experiments have much lower D-fluxes than PGD, but low level X-ray production thought to be related to the discharge phenomenon. 2. E x p e r i m e n t a l S e t u p The UIUC staff have designed and fabricated a unique new type of discharge chamber (Fig. 1), which contains a water-cooled cathode (the target can be mounted easily, and is capable of linear motion), a stainless steel anode (capable of angular motion), and a photodiode soft X-ray detector (which will be discussed in-depth shortly). A beryllium filter was placed in front of the detector to prevent detection of visible light. In order to reduce the electrical leakage current between the anode and the ground and to confine the plasma to a smaller volume, a glass tube is added to surround the electrodes, as shown in Fig. 1. On both ends of the tube, plates covered by insulating material are used to provide a sealed boundary for the discharge. Steady state I-V curves obtained after the addition of the glass tube showed that the applied voltage increased by 50%. A hole of 1cm diameter was drilled into one side of the tube to allow X-rays to reach the detector with minimum absorption.

pump Figure 1.

(a)

(b)

Experimental chamber diagram (a) and discharge view showing glass tube (b).

316

3. A X U V D e t e c t o r T h e o r y / O p e r a t i o n The AXUV-100 detector is a silicon p-n junction photodiode that is well suited for the measurement of soft X-rays. Incoming photons or charged particles create electron-hole pairs in the junction of the photodiode. The total number of electronhole pairs generated depends on the materials used in the photodiode and the incoming particle energy. For the AXUV, the average energy for electron-hole pair creation £"e-h is 3.7eV. 4 However, phenomenons that also require some of the incident energy include "dead" doped regions and surface recombination. The percentage of the total incident energy E\ going into electron-hole pairs is the "quantum efficiency" r/Q. Fortunately, the AXUV used has been engineered to approach theoretical quantum efficiency.4 Thus, the number of electron-hole pairs is E\ divided by -Ee-h- The p-n junction of the photodiode sweeps the electrons and holes across the junction and out through contacts. Thus, if the number of electronhole pairs is known, the current they create can be calculated, or vice versa. The measured current production characteristics of the AXUV are shown in Fig. 2. 4 The y-axis of Fig. 2 is the responsivity of the photodiode, which is measured in A/W. With the responsivity information, it is simple to backtrack from the measured current to calculate the power incident on the detector. However, an oscilloscope was used to measure the voltage created. Thus, a basic circuit consisting of the AXUV photodiode and the oscilloscope is needed to understand the measurement (Fig. 3). As seen in Fig. 3, the AXUV photodiode is modeled as a current source accompanied by an inevitable series resistance i?s - due to the silicon that the electrons

Photon energy (eV)

10

0.3

100

1,000

40,00

0.2

iC

0.1

0

'

Photons * " Electrons - Hydrogen ions

'••

100

1,000

10,000

40,000

Electron/hydrogen ion energy (eV) Figure 2.

AXUV photodiode responsivity in amps per watt. 4

317

RS

+

I

~5 Rl

AXUV

Vos

1 M or 50

Oscilloscope Figure 3.

Basic circuit of the AXUV (including a series resistance) and the oscilloscope.

and holes must travel through to escape. The series resistance is assumed to be 5 O.4 The oscilloscope has an input resistance i?i, which can be set at either 1 MO or 50 0. In the AXUV setup, the voltage read by the oscilloscope is Vbs = ^AXUV-RI,

(1)

where /AXUV is the current generated by the AXUV photodiode. The fraction of the total current that this corresponds to is

//AXUV =

Ri + Rsw

(2)

Equations (1) and (2) show that a large input resistance R\ gives a high amplification, hence an accurate reading. However, the photodiode is a capacitive device, and the rise time of its response is directly proportional to the resistance it is discharged over: r = 2.2(i? s + Ri)C,

(3)

where C is the capacitance of the photodiode. 4 The capacitance depends on the detailed photodiode properties, but a 4 pF value is assumed here. The fraction of the measured current and rise time calculation results for the 1 MJ7 oscilloscope input resistance are given in Table 1. As seen, the theoretical rise time for the IMilRi is rather large (/xs). However, the other option, i.e. the 50 il input resistance, reduces the fraction of the total current measured. For the initial experiments here, we elected to use the 1 Mil resistance to retain accuracy while sacrificing to some extent the time resolution. Since the X-ray output measurement duration is in the millisecond range, a rise/fall time of several microseconds should give reasonable detail.

318 Table 1. Current measurement fraction and rise time calculations for the high-oscilloscope input resistance Parameter Series resistance Oscilloscope high-input resistance Photodiode capacitance Fraction of measured current Rise time

Symbol

Units

Value

Rs

Q

5 10 6 4 ~1.00 8.8 x l O " 6

-Rl-High

n

C

pF

fl-lMfl TlMfl

s

4. Calibration The calibration of the AXUV photodiode was done with a 7.5 mCi 14 C source. Carbon-14 is a beta emitter with average beta energy Ep of 49.5 keV.5 Although 14 C is a beta source rather than an X-ray source, responsivity data is available up to 30keV for electrons. While this is 20keV short of Ep, the scale of Fig. 2 is logarithmic, and the electron responsivity slope at the highest graphed energy is nearly flat. Responsivity data from Fig. 2 is extrapolated to the energy of 14 C in Table 2. If the measurement techniques for 14 C are accurate, they should also be accurate for soft X-rays; the only difference being the responsivity of the AXUV. To match the measured results with the source intensity, the power that the 14 C source delivers to the collector must first be calculated: PB = AEpAB-^(W), (4) As where A is the source activity (decays/s), Ep the average beta energy (J), AD the detector surface area (cm 2 ), and Ag is the beta source surface area (cm 2 ). The oscilloscope voltage can then be calculated by VOS = 3 ? C I 4 P D J R I ( V ) ,

(5)

where 5R(^14 is the responsivity of the AXUV for 14 C betas (A/W), P D the power delivered to the detector by the 14 C source (W), and R\ is the input resistance of the oscilloscope (f2). The calculated oscilloscope voltage and associated parameters are given in Table 3 for comparison with measured values cited later. To eliminate background light, the photodiode was placed in a container that blocked out light on all sides but the entrance. The detector head was faced away from the entrance to minimize the light. A 20 MHz low-pass filter was used with Table 2. Electron Ep = 4 9 . 5 k e V 4

responsivity

data

near

Electron energy (keV)

Responsivity (A/W)

15 20 30 50

0.237 0.238 0.240 0.244 (extrapolated)

319

the oscilloscope to reduce the noise to a //V magnitude. The 14 C source was then placed in the container and gently pressed against the detector face. Since the 14 C source completely covered the detector face, essentially no light reached the AXUV. Several consecutive measurements were taken to find a stable, reproducible signal. The final measurement gave a voltage of 2.70 ± 0.25 mV. This result is about a fifth of the projected voltage in Table 3. However, a thin layer of glass covers the 14 C source, and this is thought to attenuate the emitted betas, resulting in the smaller measured voltage. Table 3. Projected oscilloscope voltage Vo s for the 7.5mCi 14 C source Parameter

Symbol

Units

Value

Activity Average beta energy Detector surface area Source surface area Power delivered to the detector Responsivity to 1 4 C betas Projected oscilloscope voltage

A

mCi keV cm 2 cm 2 nW A/W mV

7.5 49.5 1.0 38.3 57.5 0.244 14.0

£/3 AD AS PD

5RC14

vQs

5. Results from A X U V Photodiode X-ray Measurements Representative X-ray power measurements read are shown in Fig. 4. The first "step" in the figure at about 0.04 V is the background signal caused by pickup from the pulsed power supply. The sharp spikes at the beginning and end of the second rise are attributed to the extended rise time of the photodiode (due to the 1 MQ oscilloscope input resistance). The second sharp rise near the middle of the pulse is attributed to the X-ray emission. It demonstrates two very striking features. First is the delay before initiation. Second, as seen later (Fig. 6), the X-ray energy must exceed 600 V (due to the Be filter on the detector). Yet the discharge voltage was only ^300 V. This confirms the very non-linear behavior of this unusual X-ray generation mechanism. 5.1. Solid Angle

Considerations

For the solid angle calculation, it is assumed that the soft X-rays generated are between 0.5 and 2 keV. The average responsivity in this region is about 0.270 A/W. Next, the fraction of the source X-rays that the detector "sees" must be found. The cathode and anode were surrounded by a glass cylinder during the plasma experiment to prevent arcing problems. A hole drilled in one of the vertical sides of the cylinder allowed the X-rays to escape and be collected. A diagram of the glass cylinder/vessel system is shown in Fig. 5. (The geometry leading to this setup is shown in Fig. 1.)

320

The chord subtended by the hole was measured to be 400 mm. Then the total subtended angle #TOT is found to be 1.63 radians. To calculate the surface area of the vessel, hence detector, that this corresponds to, a solid angle surface area equation is used:

de

SA •#TC

2vr

sin(/>d0d6> = r227r( 1 - c o s f - ^ ) )•

(6)

The total angle subtended is divided by two here because the <j> angle is measured from the vertical (z-axis) in the spherical coordinate system. Next, SA can be used

0.20-

p = 500 mTorr

nal (vo

0.15-

0.25

cd c

5 o.io%

0.20 0.15

u> (0 0.10 o 0 05 V, tl)

JU 0.05

8 ^JUUUV\AJU

0.00"

8

0.00 -0.05

0.0&

-0.100.000

Q002

0.000

Time (s)

p = 5 0 0 mTorr •S2.

0.10

">

0.05

!

15 a

0.002

Time(s)

k

0.00

0.05

T i m e (s)

Figure 4. Three measurements of the X-ray emission pulse at 500 mTorr. Measurement 1 is the top left graph, measurement 2 is the top right, and measurement 3 is on the second row.

321

Surface area

Subtended

Hole in glass cylinder

X-ray laser vessel

Figure 5.

Geometry of the glass cylinder /vacuum vessel system.

to calculate the X-ray power at the source by using (7). A beryllium filter was used to prevent transmission of unwanted photons and charged particles to the detector (the detector's transmission curve is shown in Fig. 6). Therefore, a transmission compensation factor is included in the X-ray power calculation. Px-ray = V 0 s ^ ^ — j ~ - ^ S A - J - ( W ) , -Kl «X-ray JF ^-D JE

(7)

where V"os is the voltage read from the oscilloscope (V), R\ the oscilloscope input resistance (0), 3?x-ray the responsivity for the soft X-rays (A/W), / F the average transmission fraction through the Be filter, AD the surface area of the detector face (cm 2 ), SA the surface area subtended by the hole (cm 2 ), and / E is the fraction of X-rays escaping through the hole in the glass cylinder. Note from Fig. 6 that the Be window cuts off all X-rays below 600 V. Thus, as stressed earlier relative to Fig. 4, the observed X-rays must have energies >600V (despite the <~300V discharge energy). In view of Karabut's earlier work, 1 ' 2 it seems logical that these X-rays have energy of ~1.5-2.0keV. Once the power is obtained, the intensity of the X-rays is simply /X-ray = ^X-ray AT ( W / c m 2 ) ,

(8)

where AT is the exposed surface area of the target. Additionally, the dose over a pulse is defined as •Dx-ray =

/ -^X-ray d£ = ix-ray^X-ray ( J / c m 2 ) ,

(9)

where tx-ray is the duration of the X-ray pulse. Finally, the X-ray production efficiency (X-ray power out/electrical power in) can be defined as 77X-ray = ^ " f ^

100(%),

(10)

322

I.U

Be Thickness = 12.5 microns 0.8 "

/

0.6-

/

0.4 -

// //

0.2 "

00 500

1000

2000

1500

Photon energy (eV) Figure 6.

Beryllium filter transmission rate as a function of photon energy.

where Vm is the input voltage, I[n the input current, and t-m is the duration of the input pulse. Values for the constants are listed in Table 4, while the calculated values for the X-ray power, intensity, dose, and efficiency are tabulated in Table 5. Assuming an X-ray quanta energy of Ex = 1.3 keV, the 13.4mW/cm 2 intensity shown in Table 5 corresponds to 6.4 x 1013q/s-cm 2 . While the dose per pulse is small, the instantaneous X-ray power over the pulse is in the mW range. The X-ray efficiency is quite low, suggesting improved operation may be sought in future experiments. 6. Auxiliary X-ray Experiments using D-desorption One theoretical explanation for these observations proposed by the authors is that the deuterium slows down in the target, diffuses, and accumulates in dislocation loops. If so, the diffusion time constant could account for the delay time before X-ray emission (Fig. 4). X-ray emission from the high density in the "loop" cavities would explain the beamlet-like output reported by Karabut. 1 ' 2 It is also consistent Table 4. Constants required for the X-ray power, intensity, dose, and efficiency calculations Parameter

Symbol

Units

Value

Vessel radius Responsivity for soft X-rays Be filter transmission fraction Detector surface area X-ray escape fraction Exposed target surface area Input voltage Input current Input pulse duration

r

% - ray

cm A/W

/F AD

cm 2

27.5 0.270 0.75 1.0 0.05 1.0 250 1.5 1

/E AT

vin

lin tin

cm 2 V A ms

323 Table 5. Calculated values for X-ray power, intensity, dose, and efficiency averaged over three measurements at 500 mTorr (see Fig. 4) Parameter

Symbol

Units

Value

Oscilloscope voltage X-ray power X-ray intensity X-ray pulse duration X-ray dose X-ray efficiency

Vos Px-my -fx-ray ^X-ray Dx-r&y

mV mW mW/cm2 ms ^tJ/cm 2

??X-ray

%

90.9 13.4 13.4 0.263 3.3 8.9 x 1 0 " 4

with the observation of a very high density of deuterium (~ metallic hydrogen) in dislocation loop areas which approach superconductivity conditions. 6 In view of this theory, an auxiliary D-desorption measurement was carried out. Pd:Dx cathodes were manufactured from the Pd foil used in the glow discharge experiments and loaded with deuterium by electrolysis (current density J = lOmA/cm 2 ) to a concentration of x = D / P d = 0.7. The deuterium was spontaneously evolved from the Pd:D:r cathode at room temperature. The TLD detectors were placed such as to partly cover the sample face. The TLDs were mated with polypropylene (PPE) filters 0-60 /im thick to obtain some energy resolution. The soft X-ray attenuation properties at very low X-ray energies were extrapolated below 4 keV from existing data for polyethylene (PE), which is very similar to PPE. Results from the TLDs are presented in Fig. 7. Gamma-dosimetrical equations are used to analyze the TLD data. The total X-ray dose absorbed by a TLD having a surface area S' = 0.04 cm2 and a thickness 1.4. 1.2

X8-LJFTLD/PPE filters -Fit: / t // 0 = exp(-|+n/?PPE), \im = 893cm <E x ) = 1.30±0.25keV
1.00.8 0.60.4. 0.2. 0.0 -0.2-

,— 10

20 30 40 50 PPE filter thickness, h (urn)

~eo

Figure 7. X-ray spectral measurements from a Pd:Dx cathode using a set of TLDs with P P E filters 0-60 /im thick.

324

h = 1 m m can be expressed as: $xExfimS'

1-13 x 1.6 x 10" -

D =

2/A, ., , v (J-cm /MeV-kg),

,,..-. (11)

PLiF

where $ x is the X-ray flux ( c m 2 / s ) , fim the mass-absorption coefficient of a LiF T L D corresponding to the expected/measured X-ray q u a n t a energy, and puF is 0.00262kg/cm 3 is the density of a LiF T L D unit. According to (11), knowledge of the absorbed dose D allows a calculation of either the X-ray flux $x (if Ex is already determined) or the X-ray q u a n t a energy Ex (if the flux is previously known). For our TLD experiments, an average Ex of 1.3 ± 0.25 keV was estimated from the X-ray transmission through the P P E filters shown in Fig. 7. Then, the emission rate calculated from the TLDs d a t a is about 9.0photons/s-cm 2 . As expected, due to the very small D flux obtained in desorption, this value is many orders of magnitude lower t h a n the P G D case. However, the observation of soft X-rays in these auxiliary experiments provides added evidence for the proposal t h a t the P G D X-ray emission involves D diffusion and desorption. 7.

Conclusions

Strongly non-linear X-ray emission occurs and has been measured during intense D-bombardment of a P d target using a pulsed deuterium discharge method. It is noted t h a t there is a delay time preceding emission, but the key feature is t h a t the X-ray energy Ex is greater t h a n the discharge voltage. The P G D setup and diagnostics used in the experiment have been discussed in detail to aid others who may wish to adopt these techniques. Deuterium diffusion and desorption are thought to be vital steps in the X-ray emission mechanism. This seems consistent with the o u t p u t data, and an auxiliary experiment provides supporting evidence.

References 1. A.B. Karabut, Research into powerful solid X-ray laser with excitation of high current glow discharge ions, Proceedings, 11th Inter. Conference on Emerging Nuclear Energy Systems, Albuquerque, NM, pp. 374-382 (2002). 2. G.H. Miley, A.G. Lipson, and A. B. Karabut, ICFA-6, Novel Accelerators and LaserBeam Interactions, Oxford, England (2003). 3. P.B. Corkum, Phys. Rev. Lett. 71, 001994 (1993). 4. International Radiation Detectors Inc. (Oct. 2005), http://www.ird-inc.com/ frontpage.html. 5. Health Physics Society, Radionuclide decay data (Oct. 2005), http://hps.org/ publicinformation/radardecaydata.cfm. 6. A.G. Lipson, C.H. Castano, G.H. Miley, B. F. Lyakhov, A. Tsivadze, A. Yu, and A.V. Mitin, ICCF-12, International Conference on Condensed Matter Nuclear Science, Yokohama, Japan (2005).

E N H A N C E M E N T OF FIRST WALL D A M A G E IN ITER T Y P E T O K A M A K D U E TO LENR EFFECTS

A N D R E I G. L I P S O N , G E O R G E H. M I L E Y A N D H I R O M U M O M O T A University Plasma

of Illinois at Urbana-Champaign, Department of and Radiological Engineering, Urbana, IL 61801, E-mail: [email protected]

Nuclear, USA

In recent experiments with pulsed periodic high current ( J ~ 300-500 m A / c m 2 ) D2-glow discharge at deuteron energies as low as 0.8-2.45 keV a large DD-reaction yield has been obtained. Thick target yield measurement show unusually high DD-reaction enhancement (at E^ = 1 keV the yield is about nine orders of magnitude larger than that deduced from standard Bosch and Halle extrapolation of DD-reaction cross-section to lower energies) The results obtained in these LENR experiments with glow discharge suggest nonnegligible edge plasma effects in the ITER TOKAMAK that were previously ignored. In the case of the ITER DT plasma core, we here estimate the DT reaction yield at the metal edge due to plasma ion bombardment of the first wall and/or divertor materials.

1. Introduction So far, the evaluation of DD/DT-reactions at the first wall surface of fusion reactors like ITER has not taken into consideration nonlinear processes during high current, low-energy bombardment of the metal first wall. Indeed, accordingly to DD-reaction cross-section for free space the probability of DD-reactions at E^ < 2.0 keV would be negligible.1 During bombardment of a target, where the embedded ion density builds up in the lattice, conditions are quite different. It was recently shown that a majority of metal targets subjected by low-energy deuteron bombardment have a DD-reaction yield orders of magnitude higher than predicted by extrapolation of the standard (free space) DD-reaction cross-section to lower deuteron energies. These enhancement (nonlinear) effects came from a drastic increase in the deuteron screening potential in the metal targets at E& ~ 1.0 keV, especially at a high deuteron current density, where the ion density in the target can become quite large. Our recent experiments using a pulse glow discharge to simulate these conditions 2 showed about nine order of magnitude enhancement for the d(d,p)t reaction yield at E& = 1.0 keV in a Ti target, compared to an extrapolation of the standard cross-section to that energy. Strong enhancements have also been reported by several groups studying astrophysical phenomenon. 3_7 These reports suggest an enhanced DD-reaction yield may also occur during edge plasma wall bombardment of fusion devices like ITER since the energy range is consistent with deuteron accelerated by the electrostatic sheath at the plasma-wall.8 Understanding such effects becomes important relative to the possible wall damage. The enhanced 325

326

yield of alphas from DT reaction at the edge metallic sites, create vacancy sites, including stresses and allowing accumulation causing surface blistering. Knowledge of the magnitude of the enhancement effect in various metals will enable selection of reactors first wall materials that minimize such damage. We propose to simulate such phenomenon using a high-current pulsed Glow Discharge (PGD) in deuterium. Preliminary studies have shown that the PGD method can generate deuterons with energies ranging from 0.8 to 2.5 keV and a current density 300-600 niA/cm 2 . The corresponding deuteron bombardment current density on the cathode is about three orders of magnitude above that for the best lowenergy accelerators. This will enable detection of the reaction products down to E<\ < 1.0keV (using several tens hours of GD operation per data point). Moreover, this high-current bombardment should induce a measurable level of X-ray emission that is predicted for DD-reaction in the target lattice environment, 9 allowing it's detection using both X-ray and charged particle diagnostics. The correlation between the DD-reaction and X-ray yields will provide an important data base for an improved theoretical understanding of electron screening effects under these target conditions. 2. Background Recent accelerator experiments at (-E'pr)iab < 5.0keV 3 ~ 7 ' 1 0 - 1 4 show enhanced electron screening effects at the deuteron/electron densities encountered in a majority of deuterated metallic targets. These measurements show a significant increase ("enhancement") in the reaction rate (i.e. increased astrophysical factor S) at lower energies. Even for a low-density gaseous D2 target bombarded with lowenergy deuterons down to (-Epr)iab = 3.0 keV, the screening potential (measured as Ue = 25 ± 5 eV) was found to be remarkably higher than the adiabatic limit for DD-reactions in a deuterium molecule (fad. = 14.0 eV). 10 Raiola et al.6'7,11 systematically measured the low-energy (down to E^ = 5 keV) yields of D(d,p)T reactions and corresponding screening potentials for deuterated targets using about 30 different elements over the Periodic Table, including both metals and some nonmetal elements. (This extensive study was done at LUNA, the European astrophysical laboratory, as a part of their attempt to understand deuterium reactions at low energies and high electron densities). It was found that majority of the targets resulted in a "large" screening potential Ue > 100 eV, excluding, mainly, metals of group 4 (Ti, Zr, and Hf) and group 1 (Cu, Ag, and Au). The accelerator they used had a weak deuteron beam current, ranging from 1 to 54 j(iA. Therefore, reactions could only be measured at a relatively high energy (£iab > 5.0 keV). Still, the striking results provide strong motivation to extend these data to yet lower energies as proposed here. Kasagi et al.12'13 in Japan, operating with a higher-current low-energy accelerator (D+ beam current ranging 60-400 fiA), recently measured D(d,p)T yields in several metal and metal oxide targets down to E^ = 2.5 keV and found that the screening potential value Ue at such beam intensity is strongly effected by

327

diffusivity of deuterium in metals. Metals possessing a low deuterium diffusivity and a high activation energy of deuteron diffusion (Ti and Au,) were found to have low screening potentials, 65 ± 15 and 70 ± 10 eV, respectively. These screening potentials only two times above that for D 2 gaseous targets. However, for Pd and PdO targets having a high deuterium diffusivity, screen factors of Ue = 310 and 600 eV, were found, respectively.4 These high values could not be referred to "gaseous"—like valence electron screening. If diffusivity does play a role in the measurement, this must be sorted out to understand the reaction data. Thus, careful measurement of related properties such as target temperature and current are planned for the proposed measurements. So far, studies using accelerators had deal with relatively low beam currents (Jd > 400 mA) and deuteron energies E& > 2.5 keV. As indicated in Table 1, the DGD current density as proposed level can be about three orders of magnitude above that for the best low-energy accelerators. Table 1.

Comparison of high current, low-energy D accelerator and pulsed GD

Parameter

/ (range)

Ed (lab)

VKmax (W) keV, range

P (mmHg)

T, K (target) spread

D+ energy

a

10-400 ^A

100.0-2.0

2.0

100-350

± 1.0%

100-600 mA

2.5-0.40

200.0

5 x 10"7, vacuum 2.0-10.0, D 2

200-2000

± 10.0%

High current accelerator b Pulsed glow discharge a

T h e accelerator uses a duoplasmatron (E^ = 50 keV) ion source, decelerating system and magnetic focusing installation. 1 2 , 1 3 b Power supply is a rectangular periodic current pulse generator. Pulse duration can vary within 100-600 [is, different pulse on-to off ratio, typically in the range of 0.10-0.30. Anode is Mo. The distance between cathode and anode is varied between 4.0 and 6.0 mm. 2

The disadvantage of a larger energy spread in the PGD case, is outweighed by the higher current and lower voltage capability. Moreover, in the case of TOKAMAK's first wall bombardment the broad thermal energy spread should be taken into account, so the 10% energy spread in GD cannot be considered as a negative factor with respect to thermonuclear process simulation. In order to make sure that GD might simulate TOKAMAK edge effects below, we also present comparative parameters of ITER plasma flux at the first wall and high-current pulsed glow discharge. • ITER: power deposition at the first wall W ~ 1 kW/cm 2 ; at ion temperate Ti ~ 0.5-1.0 keV, the flux of bombarding ions with the energy Ei(i = d, t, 3 He) ~ 1.0-2.0keV would be Jt ~ 0.5-1.0 A/cm 2 . • High current pulsed glow discharge (GD) in D2 at p ~ 0.5 — 9.0 mmHg: pulses 0.2-1.0 ms duration (rising time < 1.0 (is), E^ ~ 0.5 — 2.5 keV, J - 0 . 2 ^ 2 . 0 A/cm 2 .

328

This comparison show that available high-current pulsed GD might well simulate the edge-plasma effects at the first wall of ITER. 3. DD-Reaction Enhancement in Glow Discharge Detection of charged particles from DD-reaction and X-rays was carried out insitu in a GD vacuum chamber during discharge operation at different voltages and currents. A diagram of the glow discharge apparatus with appropriate detectors is shown in Fig. 1.

H Figure 1. High-current pulsed glow discharge set up. 1: vacuum chamber; 2: cathode holder; 3: Ti cathode; 4: Mo anode; 5: Be window; 6: CR-39 detectors; 7: glow discharge area.

Due to the electrical noise during pulsing, a key to successful use of this technique is employment of CR-39 track detectors. With proper calibration these detectors provide a sensitive measure of the particle (protons in the present case) energy. The track hole diameter on particle energy entering the CR-39 provide this data while electrical noise is eliminated, some natural defects in the CR-39 are always present. These can be minimized by proper handling and annealing prior to use. Since the proton fluxes in this low-energy range are extremely low, the foils are left position for hours while the device is pulsed (as much as ten hours in present work). This provides a time integration of the signal which is essential. Fortunately the GD apparatus can operate very stably for long periods. 2

329

Schematic diagram of glow discharge set up. 1: vacuum chamber; 2: cathode support; 3: cathode; 4: Mo anode with holes; 5: 15 mm thick Be-foil; 6: CR-39 detectors; 7: discharge zone supply; 8: scintillator/X-ray detector. The distance between the moving Mo anode and removable cathode (thickness h = 0.01cm, area S = 0.64 cm 2 ) was varied over 4.0-5.0 mm. The current and voltage repetitive pulses had a square-like shape, duration A T « 200-400 /is, pulse repetition frequency of 5kHz and a short arise time (less than 1.0/is). The pulse parameters were continuously monitored upon the discharge operation by 2-channel 100 MHz memory oscilloscope. A stable glow discharge was achieved at P=2.0-9.0mmHg. without pulsations or instabilities within a 10 ns time resolution. For charged particles detection (3.0MeV protons from d(d,p)t reaction), purified Fukuvi Chemical plastic CR-39 track detectors were used. These detectors were calibrated using a Van-DeGraaf accelerator. Holes were drilled in the anode to allow reactionproducts to reach CR-39 track detectors located behind the anode (Fig. 1) at the distance of R = 3.0 cm from the cathode surface. Reference measurements with identical electrodes, but in a hydrogen glow discharge were used to obtain a background CR-39 tracking. A sensitive A1203 based thermo-luminescent detectors (TLD) with a set of 15-300/xm (2.8-55.5 mg/cm 2 ) thick Be-foils were employed for simultaneous X-ray measurements. The time correlation of X-ray emission with the GD current pulses was measured with a Photoelectron multiplier (PEM) and plastic (PMMA) scintillator (17mm diameter). Measurements with CR-39 track detectors covered with 11//m Al-foils showed statistically significant number of 3.0 MeV proton tracks, depending on the GD voltage and current. Typical distributions of charged particle tracks versus their diameters for deuterium GD for two different voltages U = 2175 and 805 V at the same current / = 250 mA are presented in Fig. 2. The position of DD-3.0MeV proton tracks at d = 5.2 mm is in good agreement with calibration data and previous measurement at U = 1.25 kV. Initial experiments were carried out from 0.8 to 2.45 kV with currents covering 240-450 mA using a Ti cathode as the target. The duration of each experiment was about 7.0 h Measurements with CR-39 track detectors covered with Al-foils showed a statistically significant number of 3.0 MeV proton tracks in this range of V-I. As reference values for the extreme case of a thick target, proton yields for a "thick" cathode bombarded with deuterons having energy E&, were calculated from:13

Yt(Ed) = J NB(x)alah(E)(dE/dx)-1dE.

(1)

o Here ND(X), u\ab(E), and dE/dx are the density of target deuteron in the Ticathode, the reaction cross section and the stopping power of deuterons in Ti, respectively. The Bosch and Halle (B and H) formulation was used to describe the cross section with an extrapolation to lower energies.1 The stopping power of

330

H H Ti/D2, U = 805 V, / = 250 mA, t = 7.0 h F " n Tl/D2, U = 2175 V, / = 250 mA, f = 7.0 h 250-

200

150

100

50-

4.5

5.0

I

5.5

Track diameter (|rm)

Figure 2. The 3.0 MeV proton yield detected by 11 p Al covered CR-39 detectors in deuterium GD at the same current and different accelerating voltages: U\ = 805 V and U2 = 2175 V.

deuterons in the Ti-target is assumed to be proportional to the projectile velocity at low deuteron energies. 14 ' 15 The yields of 3.0 MeV protons obtained at different deuteron energies ranging from 0.8 to 2.45 keV were normalized to those at maximal voltage U = 2.45 kV, taking into account the power of discharge or effective temperature at the target surface that both affect the change of effective deuteron concentration in the Ti (N-&(x)). This correction is needed to account for the change in deuterium concentration in the Ti-target surface. The correction coefficient k can be derived as: 2

k{W,T) =exp

£ d AT (Wm/Wx) k^TmTQ

(2)

where £d = 0.04 eV is the activation energy of deuteron escape from the Ti surface during bombardment; Tm = 1941 K is the Ti melting point, T0 = 290 K is the initial target temperature, A T = T m — To, Wm = 906.5 W is a max amplitude power at _Ed = e Um = 2.45 keV and 7m = 370 mA; Wx is a current amplitude power corresponding to any other (lower) voltage and current in GD with Ti-target. The value of Ed is determined from accelerator data 12 using an Arrhenius plot of 3.0 MeV proton yields for Ti-target at 180-195 K, Ed = 10.0 keV. Figure 3 shows the results of normalization of DD-proton yields Yx at lower energies to those at E
331

Ed (keV)

Figure 3. Experimental yield of 3.0 MeV protons at 0.8 < E^ < 2.45 keV normalized to that at E<± = 2.45 keV. The bare cross-section corresponded to B and H approximation to E^ <2.45 keV is marked by a solid line. The dashed line is a DD-reaction yield in accordance with a screening potential value Ue = 610 eV. 2

For comparative purposes, an enhancement factor, f(E), defined as the ratio of the actual yield to the bare cross-section prediction, is given as: 13 f(E) =

Yp(E)/Yh(E)=exp[ivr](E)Ue/E},

(3)

where YP(E) is the experimental yield of DD-protons in GD, Y\,(E) is the bare cross-section yield at the same energy determined by the B and H approximation; 2 2 2-KTJ = 31.29Z (n/Ey/ is the Sommerfeld parameter (here Z is the charge number of deuteron in the case of D+ projectile and target, /j, is the reduced mass and E-is the center of mass deuteron energy), respectively. Thus f(E) is directly related to the screening effect on the reaction rate. This is further illustrated in Fig. 4, where data obtained from accelerator experiments 9 (curve 1) and GD experiments with a Ti-target/cathode (curve 2) are shown. In accelerator measurements with the Ti-target at 2.5 < E& < 10.0 keV, the deduced screening potential is Ue = 65 ± 10 eV.4 However, for the PGD experiment, the screening potential is as large as Us = 620 ± 140 eV. Put another way, this experimental enhancement for GD in terms of DD-proton yield even at Ed = 1.0 keV is about nine orders of magnitude larger than that predicted with bare (B and H) cross-section (Fig. 4, curve 2). This striking result illustrates how important the higher deuteron/electron densities in the target (due to the higher currents in the GD) can be.

332

1l

io910 6 10 7 106' 10 5 10 4 10 3 10 2 10-

\ Y &

1

ue~- 610±150eV

/

i \ *

|

\ \\

AS

Ue=65±10eV

, ,

1

£ d (keV)

Figure 4. DD-reaction enhancement factor calculated with formula (4) for the Ti target during deuteron bombardment with accelerator 1 3 (curve 1) and glow discharge 2 (curve 2). The solid parts of the curves are corresponded to the deuteron energy ranges where DD-reaction yield was measured experimentally.

Available experimental dtat on deduced electron screening resulting in DDreaction enhancement in Ti target as a function of deuteron current and target temperature are shown in Table 2: Table 2. Parameters of DD-reaction enhancement under deuteron bombardment of Ti target with accelerators n>i 3 and glow discharge 2 Target/Ref.

A£d(lab), (keV)

J (mA)

T (K)

Ue, (eV)

Closest metal-host level

£(level), (eV)

Ti" Ti13 Ti (GD) 2

5-30 2.5-10.0 0.8-2.45

0.054 0.06-0.25 225-450

263 186 >1000

30 6515 610150

Ti(MII/MIII) Ti(MI) Ti(LII)

32.6 58.3 461

The screening potential Ue increases roughly logarithmicly with increase in deuteron current J. The various metal-host (Ti) electron shell energy is consistent with the screening potential values Ue.2

Thus, when the GD low-energy yields are analyzed in the same way as accelerator data, 12,13 they exhibit a larger enhancement at very low D-energy (Ed < 2.45 keV) than was expected from the accelerator bombardment. Further increase in current density (say in TOKAMAK devices) could lead to enormous enhancement of fusion reaction rate in construction metals from which the first wall is built. Note that the enhancement data on tungsten obtained even with low-current accelerator 7 ' n gives high screening potential value Ue = 220 eV. Thus, suggesting same logarithmic

333

dependence of Ue on current density the large enhancemnt of fusion reaction is expected at J ~ 1 A/cm in those construction material. These preliminary GD experiments also showed that Ti-cathode deuteron bombardment in the PGD in is always accompanied by intensive emission of the soft X-ray quanta. In the experiments involving TLD in GD with Ti-cathode at / = 200 mA and U = 1.25 kV, the high intensity (Ix = 10 13 photon/s in 47rsteradian), soft X-ray emission with quanta energy Ex = 1.1-1.4 keV was detected. It is important to note that the mean energy of X-ray photons emission is close to the bombarding deuteron energy. In order to establish the source of the X-rays a special movable design of the anode was employed, such that the anode position could be varied with respect to cathode This allowed runs with a "plasma"-anode (i.e. when the metal anode was shifted 20 mm aside with respect to cathode, Fig. 5a). Then the cathode area was fully opened toward a window viewed by a camera with X-ray film (recall Fig. 1). The X-ray emission image obtained showed a bright spot comparable with diameter of roughly the cathode area. Analysis of measurement with various anode displacements suggests that > 90% of the X-ray emission comes directly from the Ti-cathode surface.The energy of X-ray obtained from Be-shielded TLD measurements was roughly equal to the discharge voltage /deuteron energy in the range of 1.2-1.8 kV at constant discharge current J = 200 mA. To change the discharge voltage at constant current, the deuterium pressure was varied over 2.0-9.0 mmHg. At U < 1.6 kV, the X-ray quanta energy is about Ex = 1.30 ± 0.15 keV independent of the voltage applied, while at U > 1.6 kV the X-ray energy slowly increases with voltage, reaching Ex = 1.43 ± 0.15 keV.

(a)

(b)

Figure 5. (a)- X-ray image of the Ti-cathode using the pin-hole camera. The objective of 0.3 mm diameter is narrowed by use of a 15 (im Be shield in front of the camera. The image is a positive imprint, (b) - Correlation between X-ray and current pulses in GD (Ix ~ 10 1 4 . 1.5 keV).

334

The X-ray yield per deuteron increases exponentially with the applied deuteron current at E& ~ 1.5-2.0 keV as it is shown in Fig. 6

X-ray yield per deuteron versus effective 4.00E 04

power at p = 4.2 mm

3.50E 04 3.00E 04

^=0.977

2.50E-04 2.00E-04 1.50E-04 1.00E-04 5.00E 05 COOEiOO 40

Power p* (W)

Figure 6. Yield of X-ray quanta per bombarding deuteron from the Ti-cathode versus effective discharge power at p — 4.2 torr.

The results obtained in experiments with glow discharge suggest nonnegligible edge plasma effects in the ITER TOKAMAK that were previously ignored. In the case of the ITER DT plasma core, it is possible to estimate the DT reaction yield at the metal edge due to plasma ion bombardment of the loaded first wall and/or divertor material. Then the yield of 3.6 MeV alpha-emission (DT reaction charged product) near the surface of the wall would be enhanced during the metal bombardment (e.g. W as a divertor material) similarly to DD-reaction GD studies. This estimate indicates that during one year of ITER operation (maximal power deposition up to P ~ 0.1 GW/m 2 8 ) , about 1014 c m - 2 He4 atoms (formed from the stopped 3.6 MeV alpha particles) would be stored within the near surface metal (tungsten) layer of ~ 6 jiva depth. The helium atoms will be precipitated at dislocation cores or captured in dislocation atmospheres (Cottrell atmosphere) and serve as an obstacle with respect to dislocations motion. Thus, the helium capture could induce a micro crack formation at the metal surface caused by reduction of plasticity due to the decreased dislocation mobility. The first wall erosion by sputtering caused by low-energy d, t and He ion bombardment would be also enhanced by intense soft X-ray quanta during the bombardment of the wall by keV deuterons. This effect is expected due to full deposition of X-ray quanta energy in the thin layer of the wall. In this connection, the high current glow discharge could be considered as an ideal instrument for simulation of the plasma edge effects at the metal surface. Experiments performed with metals serving as construction materials of first wall

335 of I T E R would provide necessary information on DD and D T reaction enhancement and emission of accompanied intensive X-ray q u a n t a caused an excessive helium storage and radiation stimulated corrosion near their surface layers. 1 6 4.

Conclusions • At Ja > 1.0 A / c m 2 and E& ~ l - 2 k e V , the total yield of DT-reaction (scaled to GD with Ti target) for ~ 10 years of operation is found to be ~ 10 1 4 H e ~ 4 atoms, stopped at depth ~ 5.0 m m from the surface. This corresponds to ~ 10 1 7 c m ~ 3 H e - 4 concentration beneath the surface. • T h e 4 He-atoms will be precipitated along dislocations or captured in metal vacancies serving as obstacles for dislocation motion resulting in additional stress. • Reduction in plasticity (e.g. in W ) due to the He capture is caused a microcrack generation at the near-the surface layer and fracture of the first wall. • Intense soft X-ray emission at the surface may also enhance erosion/sputtering process at the surface of the first wall caused by X-ray energy deposition in the near-the-surface layer during charged particle bombardment. • T h e edge plasma effects at the first wall, including blistering, cracking and erosion, would be significantly underestimated because the enhancement of D D / D T reaction and accompanying radiation processes at very low deuteron energy are neglected. • T h e high current pulsed GD testing appropriate cathode materials (W, St. steel) could be a suitable instrument to simulate edge plasma effects at ITER'S first wall.

References 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16.

H.S. Bosch and G.M. Halle, Nucl. Fusion 32, 611-631 (1992). A.G. Lipson, A.S. Roussetski, A.B. Karabut, and G.H. Miley, JETP 100, 1175 (2005). M. Junker, A. D'Alessandro, S. Zavatarelli et al, Phys. Rev. C57, 2700 (1998). M. Aliotta, F. Raiola, G. Gyurky et al, Nucl. Phys. A690, 790 (2001). K. Czerski, A. Hulke, A. Biller et al, Europhys. Lett. 54, 449 (2001). F. Raiola, P. Migliardi, G. Gyurky et al, Eur. Phys. J. A13, 377 (2002). F. Raiola, P. Migliardi, L. Gang et al, Phys. Lett. B547, 193 (2002). D. Reiter, Edge plasma physics overview, Trans. Fusion Tech. 33, 249 (1998). V. Violante, A. Torre, G. Silvaggi, and G.H. Miley, Fusion Tech. 39, 266 (2001). U. Greife, F. Gorris, M. Junker et al, Z. Phys. A465, 150 (1995). F. Raiola et al. (LUNA collaboration), Electron screening in d(d,p)t for deuterated metals, Nucl. Phys. A719, 61C (2003). H. Yuki, J. Kasagi, A.G. Lipson et al, JETP Lett. 68(11), 785 (1998). J. Kasagi, H.Yuki, T. Baba et al., J. Phys. Soc. Jpn. 71(12), 2881 (2002). K. Eder, D. Semard, P. Bauer et al, Phys. Rev. Lett. 79, 4112 (1997). S.P. Moller, A. Csete, T. Ichioka et al, Phys. Rev. Lett. 88, 193201 (2002). For He-4 blistering in ITER first wall see: Fusion Sci. Tech. 47 (4), 821-1295 (2005).

G E N E R A T I O N OF D D - R E A C T I O N S IN A F E R R O E L E C T R I C K D 2 P 0 4 SINGLE CRYSTAL D U R I N G TRANSITION T H R O U G H C U R I E P O I N T (Tc = 220 K) A.G. L I P S O N A N D G.H. M I L E Y Department

of Nuclear, Plasma and Radiological Engineering, Urbana- Champaign, Urbana, IL 61801, E-mail: lipson@uiuc. edu

University USA

of Illinois

at

A.S. R O U S S E T S K I Lebedev Physics

Institute,

The Russian

Academy

of Sciences,

Moscow

117285,

Russia

A.G. L I P S O N A N D E.I. S A U N I N Institute

of Physical

Chemistry, The Russian Academy Moscow 117915, Russia

of

Sciences,

A new approach to develop a source of 2.45 MeV neutrons caused by polarization reversal in KD2PO4 single crystal (DKDP) during its passage through the Curie point (T c = 220 K) is presented. The background of this approach is referred to observation of neutron/proton emission in DKDP during paraelectric-ferroelectric phase transition to spontaneous polarization state (and vise versa) upon the heating/cooling of crystal through Curie point Tc = 220 K. The proposed source is based on earlier established proof of deuteron acceleration and neutron generation in the crystalline lattice of ferroelectrics during their transition to spontaneously polarized state (polarization reversal). In order to obtain neutron yield for practical application, the proposed solution foresees a separate DKDP crystals serving as cathode and anode and undergo to simultaneous ferroelectric phase transition in low-pressure deuterium atmosphere.

1. Introduction Naranjo et al.1 presented a desktop neutron generator based on deuteron beam ionized and accelerated up to 100 keV by electric field arising from the spontaneous polarization of ferro/pyroelectric LiTa03 crystal at a low-pressure deuterium gas adsorption in their Letter to Nature. The results of this work are appeared to be solid with respect to both experimental and theoretical aspects of 2.45 MeV DDneutron production. However, a certain early history exists on a deuteron fusion driven by a strong crystalline electric field. The fracto-fusion caused by a weak neutron emission has been observed during the fracture of deuterated dielectric crystals (i.e., induced polarization), where cracks serve as tiny accelerators. 2,3 Such crack propagation in crystalline dielectrics is accompanied by high-energy electron and X-ray emissions up to 100 keV (see Refs. 2, 3 and references therein), similarly to that emitted by pyroelectrics with 336

337

a large spontaneous polarization. l The secondary deuterons generated by fast electron emission can be accelerated up to keV energy range inside this cracks by a strong electric field (>10 8 V/m) released on the rapture of chemical bonds in these crystals. The DD-reaction in such crack is prompted by deuteron bombardment of "deuterated target" (i.e. crack's wall surface). The idea to use spontaneous polarization in deuterated ferroelectrics to obtain DD-fusion was first explored at the Institute of Physical Chemistry, The Russian Academy of Sciences, Moscow. 4 ' 5 The reason was a strongest electric field in the lattice (E ~ 1010 V/m) that arises in the course of spontaneous polarization during heating or cooling of KD2PO4 (DKDP) single crystal through the Curie point Tc = 222 K (i.e., exactly the same presupposition that is considered in Ref. 1, when explaining benefits of the spontaneous polarization for deuteron acceleration). In these articles, the neutron emission has been detected during DKDP crystal passage through the Curie point resulting in spontaneous polarization. KH2PO4 (KDP) single crystal (similar to DKDP one, but containing just hydrogen, instead) did not demonstrate neutron emission above the background level during transition through its particular Curie point (Tc = 123K due to isotopic effect.). In contrast to Ref. 1, in the prior experiments 4 ' 5 a deuterium atmosphere was not used because the hostdeuterium in ionic form is presented in the lattice. In such a case, the DKDP crystal serves both as a source of accelerated deuterons (suggesting no need for their field ionization) and the deuterated target, simultaneously. These DKDP crystals have generated reproducible neutron emission, though three orders of magnitude lower than that in Ref. 1. The cause of a high-neutron yield in Ref. 1 is referred to both full deuterium ionization provided by tungsten tip and deuteron source-target separation, resulting in significantly higher D + energy and current compared to those inside the cracks. Furthermore, later a team from Tokyo Metropolitan University, inspired by fracto-fusion works, 2_5 performed experiment on neutron generation during the fracture of piezoelectric LiNbC>3 crystals (with the structure similar to that of the LiTaOs) in a D2 atmosphere with pressure p > 30kPa. 6 ' 7 In this particular experiment, the ionization of deuterium gas occurred at the surface of the charged piezoelectric particles, similarly to Ref. 1, so the source of deuterium was a D 2 gas. Since the surface of the LiNb0 3 particles with adsorbed deuterium served as a neutron target (contrary to the separate ErD3 target in Ref. 1), the detected neutron yield was also much lower than that obtained by Naranjo et al. Here we demonstrate our results on DD-reaction (neutrons and tritium) in DKDP during transition through Curie point that are enhanced by recent measurements of in situ 3MeV proton emission using CR-39 track detectors. We also discuss a new approach to develop a source of 2.45 MeV neutrons caused by polarization reversal in K D 2 P 0 4 single crystal (DKDP) during its passage through the Curie point (Tc = 220K).

338

2. Experimental • Transitions of KD2PO4 (98% D purity) single crystals through Curie point Tc = 220 K by heating-cooling cycle using LN2 cryostate. Control of transition with thermally stimulated depolarization (TSD). • Neutron measurements with BF3 - seven counter proportional neutron detector. • Tritium measurements with liquid scintillator technique with dissolving of DKDP crystals in H 2 0 . • Recently done: 3.0 MeV proton measurement with CR-39 (open and filtered with Al foils) attached to DKDP plates cycled through Curie point. 3. Experimental Results The amplitude-differential spectra of neutron emission are presented in Fig. 1. As seen, the sum of spectra for DKDP exposed at the neutron detector during ferroelectric phase transition near 220 K are in good agreement with Cf-252 amplitude spectrum. 800

a

700

u,

600

'c

500

g

O

400 30

°"

-

200"

•g

100-

2 50 • 40

b

30 20 10 5

10

15

20

25

30

cChannel Figure 1. Distributiion of the pulses arriving at the neutron detector channels of the pulse height analyzer, (a) From the Cf252 neutron source; (b) during temprature cycling of DKDP crystals near T c .

This picture unambiguously confirms presence of neutron emission during transition through Curie point. The neutron counts are consistent with spontaneous polarization occurring in DKDP crystals during ferroelectric phase transition as it is shown in Fig. 2. Parameters of neutron emission, including flux intensity in DKDP crystals near T c , in comparison with KDP and those obtained outside the Tc temperature interval are shown in Table 1.

339

0

o 1 3 -2

220

221

222

223

7"(K)

Figure 2. (a) Spectrum of thermal depolarization during the heating of DKDP sample near T c ; (b) corresponding histograms of neutron bursts. Here L, a is the confidence level of the observed neutron bursts, and Nb is the average background level.

As seen from Table 1, the neutron emission is occurred only in DKDP crystals (not in KDP) and strictly in the temperature range corresponding to spontaneous polarization (219-223K). Generation of DD-reaction in DKDP crystals during transition through Curie point is confirmed by measurement of 3.0 MeV protons emission (d(d, p)t reaction) during similar transitions (Fig. 3). Tritium concentration in DKDP has been measured by liquid scintillation technique. The samples were 100 times cycled through Curie point in a glass capsule. After the cycling the crystals, glass, and gas atmosphere of the ampule were analyzed. The results (in units of 109 T-atoms per gram of DKDP) are presented in Table 2.

Table 1. Parameters of neutron emission in KH2PO4 and KD2PO4 single crystals in various temperature intervals Crystal

KH2PO4 KH2PO4 KD2PO4 KD2PO4 KD2PO4 KD2PO4

(m (m (m (m (m (m

= = = = = =

0.8j 0.8f 0.8| 0.5j 0.81 0.8 j

Temperature interval: A T (K)

Foreground— background (cps)

Neutron emission <£>n (n/s)

121-125 219-223 210-215 219-223 219-223 221.0 ± 0 . 5 ; 222.0 ± 0 . 5

0.000 0.001 0.001 0.012 0.020 0.025

0.40 ± 0 . 1 3 0.61 ± 0 . 1 6 0.75 ± 0 . 1 5

±0.005 ± 0.005 ±0.005 ±0.004 ± 0.004 ± 0.004

340

open CR-39 11 mAI/CR-39 44 mAI/CR-39

3.0 ± 0.2 MeV

18

2.75 ± 0.25 MeV

•f12j

1.85 ±0.30 MeV

S 107*5

8-

"

64

20

4,8

5,0

Jj 52

5,4

5,6

5,{

J 6,0

62

Track diameter (m) Figure 3. Three MeV proton emission: 40 transitions through Curie point in a row with attached open and filtered CR-39 detectors: the detected track diameters are consistent with 3 MeV proton energy losses in Al foils.8

Neutron and proton emission yields per transition through Curie point: • Neutron yield from d(d, n)He 3 reaction was found to be Y„ = 20 ± 4 (n/transition-g) in the range of 219-223 K. • Branching ratio between neutrons and tritium should be: Y„/Yt ~ 10 . • Recently measured (with CR-39) 3.0 MeV proton yield from d(d,p)t reaction, taking into account efficiency of CR-39 detection of 3.0 MeV protons (e p = 0.076) at (Np) = 0.5 ± 0.1 count per transition was found to be y p = 12 ± 3 (p/transition-g). Thus, there is no significant difference between DD-reaction channels when 3.0 MeV proton and neutron yields are compared. That is why, the seven order

Table 2. Tritium concentration measurements by liquid scintillator technique (in units of 109 T-atoms per gram of DKDP) # Sample

DKDP crystal

Cell glass

Cell atmosphere

Total

Control 100 cycles through T c

5.0 ± 0.2 5.9 ± 1.1

8.3 ± 1 . 3

9.2 ± 1 . 5

5.0 ± 0.2 23.4 ± 1 . 8

*The DKDP sample m = 0.5 g was subjected to 100 heating-cooling cycles in isolated glass cell at atmospheric pressure. Accordingly to this measurement the yield of tritium was found to be Yt = (1.82 ± 0.25) x 10 8 (t/transition).

341

enhancement of tritium channel compared to neutron and proton yield observed during DKDP cycling through Curie point cannot be explained by conventional DD-reaction. 4. Novel Neutron Source based on Ferroelectric Transition in DKDP Taking into account both results of works, 1 ' 4 , 5 we are presenting novel type of neutron source based on transition of DKDP single crystal through Curie point at Tc = 220 K (polarization reversal) and employed on principles of a high-voltage glow discharge in a low-pressure deuterium atmosphere (Fig. 4). In order to increase deuteron kinetic energy, the "paired DKDP crystal system" suggesting both ferroelectric electrode pair 9 operating as cathode and anode is proposed. The polarization reversal in both single crystal DKDP cathode (having a conic shape) and rounded shape anode separated by a spacing of ~ 1 cm is caused by heating/cooling through the Tc = 220 K. To this goal, both cathode and anode inserted inside metallic Cu frames that are attached with the dielectric epoxy composition to the cryostat wall. The liquid nitrogen (LN) cryostat is supplied with a heater allowing change in DKDP temperature near 220 K. In order to keep a constant positive electric charge at the cathode surface, the back face of the DKDP cathode is grounded via an ohmic contact (silver film) sputtered on top of the crystal attached to the epoxy layer. To keep negative electric charge at the surface of the anodic DKDP piece, a small positive potential is applied to its back face. The sealed cryostat chamber is filled with D2 gas at pressure about 10 mTorr. During simultaneous transition through Curie point both cathode and anode are triggered to a spontaneous polarization state. In such a case, the strength of electric field in the gap between their surface would reach a value E ~ 108 V/cm due to a large value of spontaneous polarization in DKDP (P s ~ 5.0 x 10~ 6 C/cm 2 ). This electric field will stimulate an intensive field emission of energetic electrons (up to hundreds keV range) from the cathode surface and X-ray generation during anode electron bombardment. The electron emission will produce mostly secondary D + ions from the anode because the binding energy of deuterons in DKDP lattice is very small (hydrogen bonds). The deuterons escaping from the anode will be accelerated in the electrostatic field in the interelectrode gap toward the surface of DKDP cathode and bombard it with energy about 100 keV in the laboratory system. At realistic time of the passage through Tc chosen as ~ 10s (e.g., AT = 222-220K and AT /At ~ 0.2 K/s, comparable with Ref. 5), the expected electron current density would be J e ~ 1.0/xA/cm2. Assuming a secondary ion emission coefficient ~ 1 and taking into account possibility of direct deuteron field emission from the DKDP anode tip, we suppose that the D+ current density would be the same order of magnitude as an electron emission one. Thus, at -Ed ~ 100 keV and Ja ~ 1/xA/cm2, the expected neutron yield can be estimated as 10 5 -10 6 n/s in AIT ster. Notice that the deuterons escaping from the anode surface would be fully substituted by deuterium ion adsorption at the DKDP surface and its ferroelectric properties could be

342

recovered, resulting in multiple usage of the source (passage through Tc) to generate neutrons. The proposed neutron source can be further modified resulting in production of enhanced stationary neutron yield by application of pulsed voltage (several kV) between cathode and anode at constant temperature T < Tc (e.g. T = 77 K). This application provides polarization reversal at spontaneously polarized ferroelectric state by triggering electric dipole moment orientation by AC electric field.

Figure 4. Diagram of cryo-set up of 2.45 MeV neutron source based on a high-voltage discharge between DKDP single crystalline cathode and anode during their passage through Curie point. 1 0

5. Conclusions Generation of DD-reaction resulting in neutron and 3 MeV proton emissions in DKDP ferroelectric crystal during passage through Curie point has been established. It was shown that neutron and proton channels in DKDP crystal give comparable nuclear yields. Large amount of tritium production ( ~ 2 x 10 8 T 3 at./transition) cannot be referred to usual DD-reaction. The factor of spatial separation of deuteron source and target in deuterated ferroelectrics can be used to obtain large neutron yield during transition of these ferroelectrics to spontaneously polarized state. New type of neutron source based on electric discharge between two ferroelectric KD2PO4 (DKDP) crystals during their polarization reversal at T = 220 K in D2/T2 atmosphere is proposed. No high voltage power supply. Small size. Projected intensity Yn = 10 6 (D 2 )-10 8 (T 2 ) n/s. Potential applications include Homeland security and oil exploration as a borehole source.

343

References 1. B. Naranjo, J.K. Gimzewski, and S. Putterman, Nature 434, 1115-1117 (2005). 2. V.A. Klyuev, A.G. Lipson, B.V. Deryagin et al, Sov. Tech. Phys. Lett. 12 551-555 (1986). 3. B.V. Deryaguin, A.G. Lipson, V.A. Kluev et al., Nature 341, 492 (1989). 4. A.G. Lipson, D.M. Sakov, V.B. Kalinin, and B.V. Deryaguin, Sov. Tech. Phys. Lett. 18, 90-95 (1992). 5. A.G. Lipson, D.M. Sakov, E.I. Saunin et al, JETP 76(6), 1070-1076 (1993). 6. M. Chiba et al, Nuovo Cimento A108(10), 1277-1280 (1995). 7. M. Fuji et al, Jpn. J. Appl. Phys., 41(4A), 2115-2119 (2002). 8. A. G. Lipson et al., Proc ICCF-10 (Boston, MS, 2003). 9. J.A. Geuther and Y. Danon, J. Appl. Phys., 97, 074109 (2005). 10. A.G. Lipson and G.H. Miley, A novel portable ferroelectric source of fast MeV neutrons for homeland security applications. Transactions of American Nuclear Society, 2006 (in press).

S T U D Y OF ENERGETIC A N D T E M P O R A L CHARACTERISTICS OF X - R A Y EMISSION F R O M SOLID-STATE C A T H O D E M E D I U M OF H I G H - C U R R E N T GLOW DISCHARGE

A.B. K A R A B U T FSUE

"LUCH"

24 Zheleznodorozhnaya St, Podolsk, Moscow E-mail: [email protected]

Region

14-2100,

Russia

Experimental results on X-ray emission characteristics from the cathode material in the high-current Glow Discharge (GD) are presented. The X-ray emission ranging 0.6-6.0 keV and more with the dose rate up to 0.01 J / s has been registered. Two emission modes were obtained in the experiments: (1) diffusion X-rays were observed as separate X-ray bursts (up to 5 x 1 0 s bursts a second and up to 10 6 X-ray quanta in a burst); (2) X-rays in the form of laser micro-beams were registered (up to 10 4 beams per second and up to 10 1 0 X-ray of quanta in a beam, angular divergence being up to 1 0 - 4 , the duration of separate laser beam about T = 3 X 1 0 ~ 1 3 - 3 X 10~ 1 4 s, the estimated separate beam power of 10 7 -10 8 W). The emission of the X-ray laser beams occurred during the GD operation, and, after the GD current switch off.

1. Introduction Experiments aimed at illuminating the anomalous high-energy phenomena in the solid-state cathode medium of the high-current glow-discharge were carried out for years. Earlier experimental results showed that the character of detected X-ray emission was essentially different from the known X-ray emission types. 2. Experimental Method and Results The experiments were carried out using a high-current glow discharge device (GDD) in deuterium, hydrogen, Ar, Kr, and Xe. The GDD operated on a pulse-periodic power. The power supply produced direct pulse-periodic current of rectangular shape of pulse. In the separate experiments the pulses duration were from 0.1 ms up to 1.0 ms, the period was from 0.3 ms up to 100 ms. The GD conditions were following: current (amplitude) was from 30 mA up to 200 mA, voltage 1300-2300 V, a gas pressure in the discharge chamber was 3-10 Torr. The X-ray emission registration was carried out by thermo-luminescent detectors, X-ray pinhole, and scintillation detectors with photomultiplier. The energy spectrum of the X-ray emission was registered with the help of a curved mica crystal spectrometer. The cathode samples made of Pd and other metals were placed on a cathode-holder above which a window for output penetrating radiation was provided. 344

345

The window was shielded by 15/im-thick Be foil for protecting the detectors from visual and ultraviolet radiation. Various detectors were installed by the window to measure the output penetrating radiation (Fig. 1). To estimate the intensity and evaluate the mean energy of the soft X-ray emission in the GD, thermo-luminescent detectors (TLD) based on crystalline AI2O3 and, covered by Be foils of varying thickness were used. The temporal characteristics of the penetrating radiation were determined with the help of scintillation detectors with the photomultipliers (PM). Two modes of radiation emission were observed in the experiments: (1) diffusion X-ray emission (Fig. 2) and X-ray emission in the form of laser beams (Fig. 3). The diffusion X-ray emission occurs mainly during the current running in the form of flashes and conforming to the law 1/r2. The value of X-ray emission energy was estimated for the experiments with using system scintillator- PM and the beryllium foil shields for the foil with thickness of 15 and 30/um (Fig. 2a and b). 8 Be =15-300um 9 view A *

A s

-

Figure 1. Schematic representation of an experiment, (a) pinhole, (b) TLD detectors and absorbing Be screens of various thickness, (c) PM-scintillator system, and (d) X-ray spectrometer. (1) Cathode sample; (2) anode; (3) discharge chamber, (4) Be foil screens; (5) X-ray output channel, (6) pinhole objective, (7) X-ray film, (8) absorbing Be foil screens with thickness ranging 15-300 lira, (9) TLD detectors, (10) absorbing Be foil screens for scintillator, (11) scintillator, (12) photomultiplier, and (13) mica crystal spectrometer.

By using the PM scintillation detector the relative intensity of the X-rays was determined as the total sum of the amplitudes HAH a n d H,A2j of all the X-ray bursts within the time interval of 1 second (Fig. 2a and b). The experiments using the scintillator - PM measurement system, and, 15 and 30 /xm-thick Be foil shields allowed to evaluate of the X-ray energy value as J5x- ra y ~ 1.3-2.5 keV (for different cathode materials). Then the relative intensity was reduced to a physical magnitude by the intensity value measured with the TLD detectors (.Ex-ray ~ 1.5-1.8 keV). The generation of X-ray emission in the form of laser beams and began when the GD operational parameters increased (duration of current pulses, current density, GD voltage) and was observed as powerful flashes. The production of X-ray laser beams occurred in pulse-periodic GD some time after ( A T delay time) the GD current pulse trailing. The temporal spectrum of the X-ray emission made up a

346

correlation: the quantity of pulses per a T period of time (T stands for the time period between the GD current pulses) versus the time period between the current trailing edge and the X-ray pulse leading edge. The temporal spectra are discrete in character, consisting of separate lines. The specific pattern of each spectrum is dependent upon the cathode material used. The secondary penetrating radiation (in the form of bursts of fast electrons with small angular divergence) occurred when the targets made of different materials were exposed to X-ray laser beams. The generation of electron bursts was observed in the experiment when the primary X-ray beams passed through Pb targets (of up to 3 mm thickness). Presumably, some multi-photon processes were initiated.

/(mA) 200

Figure 2. The typical oscillograms of the X-ray emission signal from the system PM -scintillator covered with the Be foil with the different thicknes: (a) with covered the 15 /^m Be shield and (b) with covered the 30/im Be shield. The system Pd—D2, the discharge current — 150 mA.

The X-ray emission spectra were measured using the curved mica crystal (50 mm diameter) X-ray spectrometer, the spectrum being recorded on an X-ray film (Fig. 4). Reflection and refraction spectra were registered in the experiment. Reflection spectra being used for data processing. The wave length and the energy of the X-ray were determined according to the expression The energy of the X-ray mX = 2dsin 0;

EX-ra,y = 1.235/A,

where m is the spectrum order, A stands for the X-ray emission wave length in nm, 2d is the constant of the mica crystal lattice (2d = 2.0 nm), and 6 represents the reflection angle. The spectra were repeatedly recorded during the GD operation and after the GD current switch off (for up to 20 h afterward). The spectra pattern

347

includes bands, dark and light spots (consisting of multiple tiny dark and light dots) and separate dark and light small spots. The bands and spots were located in spectral areas specific for a given cathode material used (Fig. 4). The registered energy of the X-ray emission bands and spots (the energetic position of the bands and spots within the spectrum) was dependent upon the cathode material used. The registered X-ray spectra in experiments was similar to characteristic X-ray spectra. It was assumed that the diffusion component of the X-ray emission was registered on the spectrum as a series of bands.

/x-ray,

photons/beam

1.2x1( Pd-D

0.8 x10s 0.4X10B

0 /(mA) 100 0 /x-ray, photons/beam 1.2x1080.8x10s

Pd-Xe

0.4 x10s 0 /(mA)t 100

/v. Photons/beam

/x- ray,

1.2x108 Pd-Kr

0.8x108 0.4x108 0 /(mA) . 100

-•• u4

o --

;

: ml;

Af=100us-«-l—i—

30401-35;

mZ

f(ns)

Figure 3. The typical oscillograms of bursts from X-ray laser beams (PM—scintillator) in the discharge for different kind of gases. The cathode sample is Pd, current: 50 mA. *The pulse peak was cut a discriminator of amplifier, (a) D2, (b) Xe, and (c) Kr.

The X-ray emission bands energy do not correlated with L, M energy of the electron levels (Fig. 4). The laser beams were recorded as dark spots and in case of the emission beam high density they assumed white color (solarization of the photoemulsion) (Fig. 5bd). In certain experiments radiation and thermal destruction of the X-ray film was observed (Fig. 5a).

348

8

*10 54 3

10 54 3 2.5-2 9keV

2.0 1.1-1.3keV _

2.0

10 54 3

2.0

10 54 3

2.0

1.0Q.< , 0.82-0.86keV

1.0 0.9

A

(^X-rayl)

,-J .3-1.5keV

B

0.8

0.7 0.68 0.66

^ 0.81-0.84keV

C

1.0 0.9 ,-,1.35-1.75 keV

0.8

0.7 0.68 0.66

1.0 0.9

0.8

0.7 0.68 0.66

^,1.2-1.8 keV

„

12 3 4 I i- -J 10 54 3

8 2.0

10

12

14

1.0 0.9

1€ 0.8

17

16

^X-ray

(A)

0.7 0.68 0.66

Figure 4. X-ray reflection spectra. Voltage GD: 2350 V, Current: 150 mA. Exposition time 18 000 s (a) X-ray spectrometer measurement diagram; (1) Cathode, (2) Be shield, (3) X-ray cathode emission, (4) spectrometer chamber, (5) slit, (6) curved mica crystal, (7) X-ray film, spectrometer, slit, (8, 9) reflected spectrum X-ray, (10) reflection spectra area, (b) Spectrum of Al-D Glow Discharge system, (c) Ni-D, (d) V-D, (e) Pd-D, (f) Mo-D, and (g) Ta-D.

349

3. Discussion Presumably, some long-lived excited levels with energies up to several keV are formed in the cathode solid-state medium when its surface is exposed bombardment

E E o

• T ^ ^ * *

1 - 2 9.0

8.5

8.0

^X-ray (A)

1.6

1.4

1.5

^x-ray(keV)

m

E. E • in

d

4

.<#* 14.0 0.88 £x-,*y(keV)

14.8

14.4 0.86

^X-ray(A)

0.82

0.84

14.6 0.85

t

0.67 ,(keV)

0.66

14.8 0.84

15.0 0.83

15.2 0.82

15.4 0.81

A.x.ray(A) 0.8

^x-ray(keV)

0.65

Figure 5. X-ray energy spectra areas with the spots from monoenergy X-ray beams (laser beams). Pd-D Glow Discharge system, Voltage GD: 2350 V, Current: 150 mA. (a) Area of X-ray film with the thermal and radiation destruction spots, (1) the normal darkness spots, (2) the spots of solarization of the photoemulsion, (3) the spots of X-ray film destruction; (b, c) areas of X-ray film with the normal darkness spots; (c, d) areas of X-ray film with the spots from intensity radiation X-ray beams.

350

by the discharge plasma ions. These levels are characterized by fixed discreet values of energy and lifetime. T h e registered X-ray emission results from re-excitation of these levels. T h e spectral energy values of the recorded X-ray emission differs significantly from L, M energies of internal electronic transitions for the given cathode material. T h e formation of excited levels may be associated with the distortion of the solid electron-nuclear system.

4.

Conclusion

T h e results obtained show t h a t it is possible to create in the solid body optically active medium with long-lived meta-stable levels with energy ranging 0.6-3 keV and more. T h e experimental research of this fundamental phenomenon has allowed to create a basically new type of the device: "The X-ray solid-state laser with 0.6-0.8 nm radiation wave length, 1 0 ~ n - 1 0 ~ 1 3 s duration of separate pulses, and, up to 10 7 W beam power in the pulses.

References 1. A.B Karabut, Research into powerful solid X-ray laser (wave length is 0.8-1.2 nm) with excitation of high current glow discharge ions, Proceedings of the 11 International Conference on Emerging Nuclear Energy Systems, 29 September-4 October 2002, Albuquerque, New Mexico, USA, pp. 374-381.

A NOVEL LiF-BASED D E T E C T O R FOR X-RAY IMAGING IN H Y D R O G E N LOADED Ni FILMS U N D E R LASER IRRADIATION

R . M . M O N T E R E A L I , S. ALMAVIVA, T . M A R O L O , M.A. V I N C E N T I ENEA,

Advanced

Physics Technologies, C.R. Frascati, 00044 Frascati (RM), Italy E-mail: montereali©frascati.enea.it

V.E. Fermi,

45,

F. SARTO ENEA,

Advanced

Physics Technologies, C.R. Casaccia, V. Anguillarese, 00060 S. Maria di Galeria (RM), Italy

301,

C. SIBILIA Universita'

di Roma

"La Sapienza", Dipartimento di Energetica, 00161 Roma, Italy

Via A. Scarpa,

16,

E. C A S T A G N A A N D V. V I O L A N T E Associazione

Euratom-ENEA

sulla Fusione, C.R. Frascati, Frascati (RM), Italy

V.E. Fermi,

45,

00044

A novel soft X-rays imaging film detector, based on optically stimulated luminescence of active color centers in lithium fluoride, LiF, has been used to obtain the image of radiation emitted from a nickel film, hydrogen loaded by electrolysis, under light coupling with an He-Ne laser.

1. Introduction An innovative film-like soft X-rays imaging detector, 1 based on optically stimulated luminescence of radiation-induced active color centers (CCs) in lithium fluoride (LiF) thin layers,2 has been used to obtain the image of radiation emitted from a nickel film, hydrogen loaded by electrolysis, under light coupling with an He-Ne laser. The novel detector, recently proposed 3 and developed for soft X-ray microradiography and microscopy applications, as well as for intense extreme ultraviolet sources characterization, 4 consists of a radiation-sensitive thin film of LiF, thermally evaporated on a glass substrate. Irradiation of this material with several kinds of ionizing radiation, like charged and neutral particles (electrons, ions, and neutrons) as well as gamma and X-rays, induces the stable formation of electronic defects, known as CCs. 2 Primary and aggregate point defects are stable at room temperature (RT) in LiF, and few of them emit intense visible photoluminescence from the exposed areas, even at RT. 351

352

The peculiar optical and spectroscopic properties of this material allow imaging with a sub-micrometric spatial resolution, simply by reading the green and red photoluminescence of F j" and F 2 centers (two electrons bound to three and two close anion vacancies, respectively) stored in the LiF-based imaging plate. Irradiation with blue light excites the visible photoluminescence of the FJ" and F 2 defects locally created in the areas previously exposed to the X-ray beam. The image can be directly read in an optical microscope operating in fluorescence mode. 1 ' 4 2. Experimental The LiF film (t = 1.9/zm) detector has been mounted in contact with the back-side of a 1 mm thick polyethylene (PE) substrate, covered by a 45 nm thick sputtered Ni film, previously loaded with hydrogen by electrolysis with 1 M Li 2 S04 electrolyte in light water (40min, current ranging from 10 to 30mA). 5 The sample has been positioned on a rotating support and, by selecting the proper incidence angle, a CW He-Ne laser (632.8 nm, 5mW) has been coupled in the black metallic layer trough a glass cylindrical lens placed in close contact with the Ni surface for an irradiation time of 3 h. In this configuration, the He-Ne light can be coupled in the Ni metallic layer by tightly focusing the laser beam in the contact region between the glass lens base and the black Ni surface and detecting a reflectance minimum through a Si photodiode. A rough scheme of the entire structure is sketched in Fig. 1. After removing the imaging LiF sensor, a carefully inspection of its surface has been performed in a conventional optical microscope operating in transmission

45 nm thick Ni hydride film 1 mm thick PE substrate 1.8 jim LiF film t nun thici< gtasi substrate Figure 1. Sketch of the layered structure exposed to He—Ne irradiation. The upper triangle represents the glass lens, and the underlying layer the Ni film surface roughness, responsible of light coupling.

353

mode with white light illumination and in conventional fluorescence mode, under blue light from a Hg arc lamp. A more complete and detailed optical investigation has been performed in a confocal laser scanning microscope (CLSM) Nikon Eclipse Cl-80i equipped with a Coherent CW Argon laser operating at 458 nm, utilized to excite the photoluminescence of active CCs eventually produced in this radiation-sensitive thin film. The CLSM system provides the opportunity to collect, acquire and store these images, and to reach a spatial resolution of few hundreds of nanometers at the used wavelengths.6 3. Results and Discussion Figure 2 shows the optical images of the exposed LiF film surface obtained in different microscope operation mode. Under UV light excitation, in reflection mode (Fig. 2b) a visible green-red photoemission from a limited region of the entire LiF film surface has been identified. The light signal in Fig. 2b often appears uncorrelated from the topographical features observed in transmission mode (Fig. 2a,c,d, see white arrows). Dust and/or other surface imperfections outside the light emitting areas of Fig. 2b are not bright at all.

Figure 2. Optical images of the exposed LiF film surface obtained in different microscope operation mode. Transmission mode, dark field, (a) Fluorescence mode, UV illumination, (b) Transmission mode, white light, (c) Transmission mode, phase contrast, (d) Reference line = 50/jm.

354

Figure 3. CLSM optical image in fluorescence mode of the exposed LiF film surface. Reference line = 100/im.

In the light-emitting areas of Fig. 2b, interesting features have been observed in confocal laser scanning mode. The higher sensitivity and spatial resolution allows us to identify several light-emitting spots, closely grouped, with typical spatial dimension from tens to hundreds of micrometers, which are shown in Fig. 3. The brightest areas are the same observed in Fig. 2b and could be attributed to light scattering phenomena from dust and/or other surface imperfections, while the observed fluorescent image appears ascribed to the photolumiiiescence of F j and F2 centers, created by ionizing radiation impinging the LiF-based imaging film during He-Ne irradiation of the Ni-Hydride film. Surface plasmons (polaritons) are quantum of plasma oscillations created by the collective oscillation of electrons on a solid surface. They may be generated by mechanisms able to produce charge separation between Fermi level electrons and a background of positive charges (i.e., lattice atoms). The coupled em wave can produce coherent oscillations of the Fermi-level electrons in the metal lattice, as its frequency is quasi-resonant with electronic plasma one. According with, 7 the excitation could produce local intense electric field, and soft X-ray emission at energies below the Ni Ka edge (8.333 keV) can take place. The transmission of a 1 mm thick PE substrate has been reported as a function of the X-rays energy in Fig. 4 and it is not negligible for X-ray energies above 3keV. 8 Depending on the X-rays energy, their penetration in LiF ranges from few tens of nanometers to several hundreds of micrometers. 1 ' 4 Our novel detector integrates all the emitted radiation and indicates that its production is confined in an area of spatial dimensions comparable with the coupling

355

1.0 0.8

I

tn to

0.6

E
0.4

0.2

2000

4000

6000

8000

10000

Photo energy (eV)

Figure 4.

Transmission of a 1 mm thick P E slab vs. X-ray energy.

region between the evanescent wave and the black Ni surface. T h e spot n a t u r e of the image in Fig. 3 would be compatible with localized radiation sources, as observed in Ref. 9. Acknowledgments We are indebted with G. Baldacchini, F. Bonfigli and F. Flora for fruitful discussions and with I. Franzini for useful suggestions. References 1. G. Baldacchini, F. Bonfigli, A. Faenov, F. Flora, R.M. Montereali, A. Pace, T. Pikuz and L. Reale, J. Nanoscience Nanotechnology 3(6), 483 (2003). 2. R.M. Montereali, Point Defects in Thin Insulating Films of Lithium Fluoride for Optical Microsystems, in Handbook of Thin Film Materials, H.S. Nalwa (ed.), Ferroelectric and Dielectric Thin Films, Vol. 3, Ch. 7, Academic Press, New York, pp. 399-431 (2002). 3. ENEA Patent TO2002A000575, G. Baldacchini, F. Bonfigli, A. Faenov, F. Flora, R.M. Montereali, A. Pace, T. Pikuz and L. Reale (International N: WO 2004/005906 Al). 4. G.Baldacchini, S. Bollanti, F. Bonfigli, F. Flora, P. Di Lazzaro, A. Lai, T. Marolo, R.M. Montereali, D. Murra, A. Faenov, T. Pikuz, E. Nichelatti, G. Tomassetti, A. Reale, L. Reale, A. Ritucci, T. Limongi, L. Palladino, M. Francucci, S. Martellucci and G. Petrocelli, Rev. Sci. Instrum. 76, 113104 (2005). 5. V. Violante, P. Tripodi, D. Di Gioacchino, R. Borelli, L. Bettinali, E. Santoro, A. Rosada, F. Sarto, A. Pizzuto, M. McKubre and F. Tanzella, Proc. 9th Int. Conf. Cold Fusion (ICCF9), Beijing, 19-24 May (2002). 6. A. Diaspro, Confocal and Two-Photon Microscopy. Foundations, Applications, and Advances, A. Diaspro (ed.), Wiley-Liss (2002). 7. V. Violante, A. Torre, G. Selvaggi and G.H. Miley, Fusion Technol. 39, 266 (2001). 8. http://www-cxro.lbl.gov/optical_constants. 9. D. Gozzi, F. Cellucci, P.L. Cignini, G. Gigli, M. Tomellini, E. Cisbani, S. Frullani and G.M. Urcioli, J. Electroanalyt. Chem. 452, 253 (1998).

OBSERVATION A N D MODELING OF T H E O R D E R E D MOTION OF H Y P O T H E T I C A L MAGNETICALLY C H A R G E D PARTICLES ON T H E MULTILAYER SURFACE A N D T H E PROBLEM OF LOW-ENERGY FUSION

STANISLAV V. A D A M E N K O A N D VLADIMIR I. V Y S O T S K I I Electrodynamics

Laboratory "Proton-21", Kiev National Shevchenko Vladimirskaya St. 64, 01033, Kiev, Ukraine

University,

The mechanism of the formation of a macroscopic periodic hollow channel created on the surface of a MDS-structure upon the execution of experiments on a hard-current vacuum diode is stymied. It is shown that the reason for the appearance of such a trajectory can be the interaction of a magnetically charged particle with paramagnetic and diamagnetic surface layers of the MDS-structure. Particles with magnetic charge can be formed during the shock action of a hardcurrent electron beam and the subsequent self-compression of the frozen magnetic field of a beam. It is shown that the source of a great specific energy release, dQtot/dJ ~ —106 GeV/cm, spent on the formation of this channel can be the processes of nuclear synthesis which are running with participation of MDS-structure surface nuclei and are stimulated by magnetically charged particles.

1. Introduction During the experiments at Kiev Electrodynamics Laboratory "Proton-21" on achieving the superdense state of the matter (the state of electron-nuclear collapse 1-3 ) by using the high-current electron driver, the traces of ordered thermomechanical impact on surfaces of the "metal-dielectric-semiconductor" (MDS) targets, remote from the collapse zone, were registered. By their configuration, these macrotracks are analogous to those observed on photoplates and presented in work.4 But the energy expenditures on the formation of the former turn out to be by many orders higher. The origin of these macrotracks can be ascribed to none of the wellknown particles. Below, we present the results of the analysis of the characteristics of these macrotracks and the properties of particles (particles with magnetic charge) which can form macrotracks. 2. Identification of a Periodic Hollow Macrotrack The mutual arrangement of main elements of the experimental setup is shown in Fig. 1. The passage of the electron beam described as a pulse hard current J(t) between the cathode and anode leads to the appearance of an azimuthal magnetic field Hq(r). These cathode and anode were produced from chemically pure Cu (purity of 99.99%), 356

357

Cathode Distant multi layer target (MDS-structure)

Azimuth magnetic field H(

Anode Figure 1.

Al Si0 2 Si plate General scheme of the experiment.

Under the action of the pulse current, the zone of a collapsing part of the anode substance is formed in the anode. 1 ' 2 A target was positioned at the distance of about 10 cm from the collapse region and was the standard MDS-structure consisting of a Si plate covered by both a thin layer of SiC>2 and a thicker layer of Al. On the surface of Al, we have found a very thin film of oil compounds (H, C), whose origin is related to the operation of an oil vacuum pump. The registered object was a macroscopic hollow track (channel) in the form of an oscillating trajectory with a constant period A s=s 60/Ltm. This track deepens periodically in the target volume through the Al layer (and partly through Si02) and appears on its surface, by simultaneously oscillating with an amplitude of about 20 /iin in parallel to the target surface. The total length of the continuous part of the track A « 2000/im, its width is 3.5 /an, and the thickness is about 1.3 /im (approximately equal to the Al layer thickness). On the target surface near the places of the periodic appearance of the track from the volume of melted and then solidified Al, a small amount of solidified Si is present. The direction of the symmetry axis of the trajectory of the main extended track (consisting of two segments) corresponds to the vector of the azimuthal magnetic field. The general view of the shape MDS-structure surface with an oscillating track and the separate fragments of the track on the surface and in the volume of Al coating the Si substrate are given in Figs. 2-4. It follows from Figs. 2 and 3 that the track is present only in those spatially separated regions of the target surface (regions 1 and 2), where the Al coating is present on the surface. Moreover, the tracks on these two regions were the obvious continuation of the trajectory of a single moving nonidentifiable particle. At the same time, we see no evidences for the interaction in the space between two regions with Al coatings. We note that the Al layer is a paramagnetic, and two remaining layers of the MDS-structure (Si

358

a)

-

b)

500 urn

<•• 100 urn *

Figure 2. The general view of MDS-structure with the tracks; (b) and (c) - fragments of track, 1 and 2 - thin Al layers on Si surface.

and Si02) are diamagnetics. Thus, the strong thermo-mechanical action occurred only in the scope of the paramagnetic. This effect is clearly demonstrated in Fig. 4, where we see the inlet of a track on the end surface of AL The volume and mass of melted Al in the scope of the macrotrack are, respectively, VAI ~ 10" 8 cm 3 . MAI ^ 2.7 x 10~~8g. The minimum energy which must be spent for the heating and melting of Al in the volume of the macrotrack is QAi = (CAT + AH)MAl

« 1.5 x 10~ 5 J « 105 GeV.

(1)

With regard for the additional energy spent for the heating and ejection of Si, the heating of the remaining unmelted part of Al, and the ionization of all the products in the region of the macrotrack, we can estimate the total energy as Qtot ^ 2 x 105 GeV. The specific energy release is very great and equals dQtot/dZ = -Qtot/L

« - 1 0 6 GeV/cm.

(2)

We note that results (1) and (2) differ by 106 times from the data presented in Ref. 4.

Figure 3. Fragments of a track on the surface of aluminium in area 2 at different magnification. Periodical "canyon" is the result of action of unknov/n particle.

359

1

«^

fettle

Figure 4. The photos of the same fragment of the track. Two l«ii photos present the inlet.of track in volume of a Si02 layer.

Below, we will show that the simple braking of particles (including those with magnetic charge) cannot ensure both the energy release (1) and (2) and the observed form of tracks. The natural question arises: Which particle can form such a strictly ordered track? The invariable value of the period of oscillations of the trajectory of the type of a "caterpillar trace" and the identical character of damages of the Al surface in the limits of all the parts of the track testify to that the average linear velocity of the nonidentifiable particle along the entire trajectory was constant. With regard for all the features of the trajectory and the great energy release it becomes obvious that the formation of such a trajectory can be related to two scenarios: • The target surface has interacted with a particle possessing a great kinetic energy W\ which exceeds the quantity Qtot by many times, and, therefore, the great energy release dQ/dl did not affect Wk, the character of the motion and interaction of the particle (e.g. this. particle consisted from 10 16 or more atoms with 0.1 eV moving energy which may cause totally more than 105 GeV energy). • The particle had a small velocity v and a relatively small kinetic energy Wk, and the very great energy release registered in experiments and the formation of a macroscopic track are related to that the moving nonidentifiable particle stimulated the running of energy-gained nuclear reactions along the trajectory of motion. The first scenario is logically contradictory and does not agree with experimental data. This is conditioned by the fact that a particle with great kinetic energy must have a great momentum. However, this contradicts the fact that the particle changed the own trajectory and the direction of motion frequently and in the ordered way. Moreover, we observe the very sharp change in the direction of motion (by an angle close to 180°) at a single point. Such a character of motion corresponds

360

to particles with small energy and small momentum. But such particles cannot execute the great work on the fracture of the target surface! The second scenario seems to be more grounded, and we consider it in detail. In the framework of this scenario, the hypothetical particle, whose interaction with the target forms a specific macrotrack, must satisfy a number of requirements: • The particle must stimulate the running of nuclear reactions with the very great energy release and the local fracture of a target. • The specific energy release stimulated by the particle should be the same along the whole track. • The particle must not participate in nuclear reactions, i.e. it must come into the reaction zone and leave it in the invariable form. • The particle itself must affect the formation of the own ordered trajectory. • Its motion must be different in the paramagnetic and diamagnetic media. It is obvious that such requirements do not allow one to identify the particle under consideration with one of the known neutral particles or particles with electric charge. There are very weighty reasons to assume that such peculiarities of the interaction can be related to the motion of a particle with magnetic charge (it can be one of the modifications of the Dirac monopole). Below, we will consider this hypothesis in detail. 3. Peculiarities of Interaction of Magnetically Charged Particles with MDS-structure The magnetically charged particles can appear (at least, in principle) in extremely strong magnetic fields, which takes place in a hard-current diode in the region of compression of the beam current in the anode volume. In this case, the micropinch is formed, and the magnetic field frozen in the superdense plasma of a spherical plasma layer is compressed to the size of the collapse zone. A minimum value of the elementary magnetic charge was determined by Dirac from the general principles of quantization: g/e

= (hc/e2)k/2,

where k = 0, ± 1 , ± 2 , . . .

(3)

The Schwinger model admits only even values of k in the quantization condition, which leads at once to the minimum charge of a magnetic monopole g « 137e. By leaving the collapse region, these particles undergone the action of the accelerating azimuthal magnetic field of the current, H(r) = 2 J/rc, and move along an untwisting spiral round the axis of the current J. For one turn round the current J, the particle can gain the energy A W J M = / gH{R)dL = gH(R)2ivR = AirgJ/c = 0.05 J (A) [MeV].

(4)

In particular, if the residual current in the diode J « 1-10 kA, we get A W J M = 50-500 MeV. At the orbit radius R = 10 cm, the rate of increase in the energy is dAI^jM/d/«l-10MeV/cm.

(5)

361

It is seen that dAWjjvi/dZ turns out 10 8 -10 9 times weaker than the experimentally registered energy release dQtot/dl on the target surface. Hence, the released energy cannot be directly related to the acceleration of the magnetic charge by the magnetic field. Consider the features of the interaction of such particles with a substance. The formula for the specific loss of energy of a magnetic charge dW^/dl

= -(ATrnee2g2/mec2)\n(4mev2/{e(t)))

(6)

follows easily from the standard Bethe-Bloch formula for the deceleration of an effective electric charge Q* = gv/c. This formula yields that the ionization losses of a moving magnetic charge do not depend on its mass and depend slightly on its motion velocity. For an Al target (ne « 7 x 10 2 4 cm - 3 ), we get the rate of loss of the energy of particles as dW^/dl « -(30-40) GeV/cm. (7) It is clear that the specific energy losses of a magnetic charge due to a deceleration, dW^/dl, exceed essentially the rate of increase in the energy dAWjM/dl of the same magnetic charge in the magnetic field (5). At the same time, the specific energy losses (7) of such a charge due to the deceleration are by many orders less than the experimental value (2) of the energy release dQtot/dl. Apparently, the other, more realistic source of a huge energy released upon the formation of a macrotrack should exist. This corresponds to the second scenario. One of the possible answers follows from the view of a macrotrack. An oscillating macrotrack is a result of the strong thermo-mechanical action on the Al layer, which causes the melting and the break of this layer and leads to the formation of distinctive channels (holes) periodically "diving" under the layer surface. The upper surface of the Al layer turns out to be splashed by drops of melted Al and Si. In our opinion, the formation of such a trajectory can be a result of the combined effect of forces related to the electrodynamic interaction of a hypothetical magnetically charged particle with separate layers, being on the MDS-structure surface, and the processes coupled with the direct effect of the nuclear reactions related to the magnetic charge on the magnetic properties of these layers. The outer layer of an MDS-target (Al) is a paramagnetic, and two inner ones (Si and Si02) are diamagnetics. The permeabilities of these media are the following: Xsi = -0.53 x 10" 6 ,

X si0 2

= -1.13 x 10" 6 ,

XAI = 1-65 x lO" 6 ,

Xvacuum = 0. (8)

The character of the interaction of a magnetic charge with the magnetic field is defined by that any diamagnetic is pushed out from the region with the strong magnetic field (this is equivalent to the repulsion of the magnetic charge from a diamagnetic), whereas any paramagnetic is pulled in the region with a strong field and, respectively, attracts the magnetic charge. This interaction yields that the Al layer is a potential well for the magnetic charge, and the layers of Si and Si02 are

362

Si

SiO„

Al

Si SiO.

MDS-structure before the interaction with magnetic charge

1 Geomentry of interaction

MDS-structure after the interaction with magnetic charge and after destruction of Al layer

V(x) x

Potential energy of MDSstructure before nuclear reaction

Potential energy of MDSstructure after nuclear reaction

Figure 5. Surface of MDS-structure and its potential energy before interaction with magnetic charge and after such interaction.

potential barriers with different heights (if we consider the sliding fall of a particle on the MDS-structure surface from the side of vacuum). To confirm the reality of this interaction, we determine the height of the effective potential barrier, which corresponds to the surface of a diamagnetic and is able to reflect a particle with magnetic charge, if its kinetic energy in the direction normal to the surface is less than the barrier height AW = iirxg2 /?*u- This value is defined by the difference of the total energy of the magnetic field H(r) = g/r2 of the particle with a magnetic charge g in vacuum and that in a medium with some specific value of the permeability x- Here, rn is the minimum distance from the magnetic charge to the medium, at which the idea of the permeability as a mean characteristic of this medium is valid. We may accept that it equals the classical radius of an atom (rn ~ 0.5 A). If we take into account that the typical value of |x| ~ 1 0 - 6 , then the height of the potential barrier for a magnetic charge on the boundary of a diamagnetic and vacuum is AW « 10 eV. Consider a possible character of the interaction of a magnetic charge with this structure (Fig. 5). We assume that the magnetic charge moves at first from right to left at a small (sliding) angle 6 in the direction to the surface (Fig. 5a), so that its relative kinetic energy (pg sin8)2/2Mg is less than the barrier height AW. While approaching the surface, the magnetic charge is pulled in the region with Al due to the attraction to the paramagnetic (Al) and then is pushed out away from the potential barrier formed by the layers of SiC>2 and Si. In the scope of the Al layer, this charge can stimulate the running of various nuclear reactions, including the synthesis reactions Al + P 1 = Si 28 , Al 27 -|-C 12 ' 13 = K 39 ' 40 with participation of Al, H, and C entering the composition of a very thin oil film on the surface of Al and release of a great energy (A_ER = 12-17 MeV). The running of these reactions is indirectly confirmed by the following.

363

"Usual" (free) spherical-like atoms without action of very strong magnetic field

Needle-like atoms in very strong magnetic field of magnetic charge

Nucleus

r

Typical electron shell of an atom

Figure 6.

Electron shell of the same atom in very strong magnetic field

Influence of magnetic charge on electron shells of atoms.

The detailed study of the isotope composition of the substance, being present on the surface of Al on both edges (banks) of a periodic track, with the help of a SIMS spectroscope revealed the presence of a very small amount of extrinsic elements, whose mass corresponded to the isotopes with mass number A = 39 and 40. 4. Possible Mechanisms of the Influence of a Magnetic Charge on Nuclear Reactions There are a lot of possible mechanisms of a strong influence of magnetic charged particles to nuclear reactions. • A value of the local magnetic field Hg (r) = g/r2, which creates a magnetic charge g in the region of localization of intrinsic atomic electrons (at re < 10 _ 9 cm) with velocity ve, can reach Hg > 10 11 Oe. The effective electric field in the same area Eeg ~ 137 eV e /r 2 c, whose value can exceed the screened electric field inside an atom Ea = Ze/r2, acts on moving electrons and sharply varies the configuration of the electron shells of atoms. Upon the application of a very strong magnetic field He (if Ee^(r) S> Ea{r) or if Z

364

1019 - 1020 V/cm is comparable to that of the electric field Ez « Ze/R2 « Z.10 18 V/cm created by the electric charges of all Z protons on the nucleus surface and essentially exceeds the field inside the nucleus. • If a magnetic charge g falls on the nucleus surface, the magnetic field of the charge exceeds the magnetic fields related to the spin-orbit interaction of nucleons by many orders. As a result, the processes related to the spinorbit interaction in the nucleus can be completely changed. In particular, the JJ-coupling of nucleons which is typical of nuclei becomes impossible. Thus, the mechanism of the stimulating action of a magnetic charge on nuclear reactions is conditioned by the effect of Hg and Ees on the spin-orbit and Coulomb interactions of nucleons, on the angular momentum of a nucleus, and, on the whole, on the binding energy of nucleons in the volume of a nucleus. This can lead to a sharp change of the stability line. The effect of a magnetic charge can stimulate the synthesis and fission on the basis of those nuclei, which are stable in the absence of the action of a superstrong magnetic field. In particular, to ensure the necessary energy release, each particle must stimulate about 5 x 107 reactions per 1 cm of its trajectory. As a result of the running of such reactions, there occurs the rapid fracture of the region of the layer of Al, which is located near the magnetic charge. In this case, the following situation is realized. Upon the heating and ionization of this region, the local system of Al atoms transits from the paramagnetic to diamagnetic state. As a result, the potential well in the region of localization of the magnetic charge disappears (this happens under the condition XAI > 0) and is transformed into a potential barrier (this corresponds to the requirement XAI* < 0) which pushes out the magnetic charge back in vacuum (Fig. 5b). Upon such an interaction, a great energy will be released. Therefore, it is natural that the Si layer adjacent to Al will be also partially melted and be splashed over the surface of Al. A special situation will occur in the case where the additional force acts on the magnetic charge and compels it to move along the surface in vacuum. Such a force can be the action of the residual azimuthal magnetic field of the diode current. The intensity vector of this field lies on the circumference positioned symmetrically relative to the diode current direction. The accelerating force will act in the same direction. Due to the presence of centrifugal forces, the trajectory of a particle with magnetic charge will be an untwisting spiral beginning in the collapse zone, where magnetic charges can be formed. In this case, the magnetic charge leaving the place of the first falling on the medium is accelerated along the surface and arrives at the place where the Al layer is intact, and its characteristics correspond to a paramagnetic. There the charge is again attracted to the layer, stimulates nuclear reactions in it, and then again leaves the layer. The repetition of this cycle leads to the periodic process of interaction of the magnetic charge with the surface and to the formation of a track in the form of a "caterpillar trace". In the region of the surface lying between the Al layers (in the middle part of Fig. 7), the particle is in the potential well such that its two walls are defined, respectively, by the

365

Areas of stimulated nuclear reactions

Figure 7. The trajectory of motion of a magnetic charge in a simplified form after its falling on the MDS-structure surface in several periods of the spiral.

repulsion from the diamagnetic (Si02 and Si) and by the action of the magnetic field of the current on the charge. In this region, a magnetic monopole moves along the surface of Si not penetrating into the volume and not inducing any damage, which is observed in experiments. It is worth noting one more circumstance. In view of the form of a macrotrack (great number of strictly periodic oscillations), we may conclude that the controlling magnetic field is approximately the same along the entire trajectory. This corresponds to that the duration of the formation of the mentioned part of the track is significantly less than the total duration of the current pulse equal to T « 30-50 ns. This allows us to assume that the duration of the formation of this part of the track with the length L ?» 2 mm is at most T\ < 10 ns, and the mean longitudinal velocity of motion of the hypothetical magnetically charged particle is greater than L/Ti > 2 x 107 cm/s. 5. Conclusion The above-presented scenario allows us to explain and to quantitatively substantiate the majority of the observed regularities of oscillating hollow macrotracks, by basing on the assumptions that magnetically charged particles are generated in the collapse region in a hard-current diode and these particles can be highly efficient catalysts of nuclear reactions. The periodic character of the macrotrack trajectory can be related to the specificity of the interaction of the hypothetical magnetic charge with the system of paramagnetic and diamagnetic layers on the MDS-structure surface. Basing on the general reasoning, we may assume that the particles with magnetic charge can be formed in the electron-nucleus collapse zone during the shock action

366

of a hard-current electron beam and the subsequent self-compression of the magnetic field frozen in the superdense plasma. A specific mechanism of the generation of a magnetic charge can be related to the topological features of the collapse zone. Starting from the above-given estimates, we can conclude that the power of nuclear transformations induced by one particle with magnetic charge in a target made of aluminum is at least Ptot > (Qtot/Ti) « 300 W! At the same time, it is obvious that the very hypothesis of the generation of magnetic charges in the collapse region, the formation of which is accompanied by an extreme deformation of the frozen magnetic field, requires the further theoretical analysis. References 1. 2. 3. 4.

S.V. Adamenko and V.I. Vysotskii, Found. Phys. Lett. 17, 203 (2004). S.V. Adamenko and V.I. Vysotskii, Found. Phys. 34, 1801 (2004). S.V. Adamenko, A.S. Adamenko, and V.I. Vysotskii, Infin. Energy 9 (54), 23 (2004). L.I. Urutskoev, V.I. Liksonov, and V.G. Tsinoev, Prikladnaia Fizika (Appl. Phys.) 4, 83 (2000) (in Russian).

E V I D E N C E OF SUPERSTOICHIOMETRIC H / D LENR ACTIVE SITES A N D H I G H - T E M P E R A T U R E S U P E R C O N D U C T I V I T Y IN A HYDROGEN-CYCLED Pd/PdO

A.G. L I P S O N * , C.H. C A S T A N O A N D G.H. M I L E Y Department

of Nuclear, Plasma and Radiological Engineering, Urbana- Champaign, Urbana, IL 61801, E-mail: [email protected]

University USA

of Illinois

at

B.F. LYAKHOV AND A.YU. TSIVADZE Institute

of Physical

Chemistry, The Russian Academy Moscow 119915, Russia

of

Sciences,

A.V. M I T I N P. Kapitza

Institute

of Physical Problems, The Russian Moscow 119334, Russia

Academy

of

Sciences,

Electron transport and magnetic properties have been studied in a 12.5 /Ltm thick Pd foil with a thermally grown oxide and a low-residual concentration of hydrogen. This foil was deformed by cycling across the Pd hydride miscibility gap and the residual hydrogen was trapped at dislocation cores. Anomalies of both resistance and magnetic susceptibility have been observed below 70 K, indicating the appearance of excess conductivity and a diamagnetic response that we interpret in terms of filamentary superconductivity. These anomalies are attributed to a condensed hydrogen-rich phase at dislocation cores. The role of deuterium rich dislocation cores as LENR active sites is discussed.

1. Introduction Recently Ashcroft has presented arguments that hydrogen dominant metal alloys may exhibit high-temperature superconductivity (HTSC) over a modest external pressure range. 1 The advantage of saturated hydrides in terms of achieving HTSC is that in a chemical sense it has already undergone a form of pre-compression and once impelled by further external pressure to enter metallic phase, the electrons from both hydrogen and metal may participate in common overlapping bands. 1 There is another approach to achieve a compressed, metallic hydride state with a high-coupling constant and this is the topic of the work presented here. Dislocation defects are strong, abundant traps of interstitial hydrogen and deuterium, as has been previously demonstrated in small angle neutron scattering measurements. 2 - 4 *Also at Institute of Physical Chemistry, The Russian Academy of Sciences, Moscow 119915, Russia. 367

368

A high-dislocation density (7Vd > 2 x 10 11 cm~ 2 ) can be created in Pd by cycling across the hydride miscibility gap. 2 At low-residual concentration (x) ~ 10~ 4 [H]/[Pd] hydrogen is strongly trapped (binding energy £H ~ 0.7 eV per H-atom), within approximately one Burgers vector (2.75 A) of the dislocation core. 5 The local concentration at the dislocation core under these conditions is estimated at ~1.4 [H]/[Pd].6 Assuming the local pressure at the dislocation core is comparable to the local bulk modulus of Pd (>100 GPa), 7 the conditions for hydrogen pre-compression will be fulfilled. The electron properties of hydrogen-dominant bulk Pd hydrides with x > 1 have not been studied previously because these compounds are unstable at ambient conditions. 8 ' 9 However, the effect x on the critical temperature, T c , of PdH^ over the range of 0.8 < x < 1.0 is to increase Tc from 1 to 8K. 10 ' n Within the context of this past work, further increases of x above 1 locally at dislocation cores is expected to increase T c well above the bulk PdH-j value. However, the volume fraction of the compressed hydrogen-rich phase must be high within the Pd matrix. Recently, a diamagnetic susceptibility contribution has been observed in hydridecycled bulk Pd with (x) ~ 10~ 4 [H]/[Pd].6 The volume fraction of this phase was estimated at ^10~ 4 . Because of the low-volume fraction the diamagnetic response was not observed directly, but only after subtraction of the host Pd paramagnetic susceptibility. We have increased the volume fraction by cycling a thin Pd foil with a thermally grown oxide layer. The oxide layer further constrained the Pd lattice during hydride cycling and prevented dislocation annihilation at the free surface. Both effects acted to increase the density of dislocation loops near the Pd-oxide interface, similar to the dispersive effect of internal precipitates. 12 2. Experimental Results and Discussions The cold rolled Pd foil, supplied by Nilaco Corp. of Japan, was 12.5/im thick with a purity of 99.95%. The concentration of ferromagnetic impurities (primarily Fe) did not exceed lOppm based on ICP analysis performed by the supplier. A 40 nm oxide layer was grown by heating the foil in an oxygen-propane flame at 1200°C for ^ 6 s . AES analysis showed that the oxygen content in the oxide layer below 1% at a depth 40 nm. The electrical resistivity and magnetic susceptibility characterization of the sample (~2cm 2 area, 30 mg) prior to hydrogen cycling constitutes the background measurement and is referred to as Pd/PdO below. The sample was then cathodically loaded with hydrogen to PdHo.7 at a current density of 5.0mA/cm 2 in a 1 M Li2S04/H20 (99.99% pure) electrolyte. Hydrogen was removed from the sample by reversing the current, resulting one hydrogen loading-unloading cycle. The sample used here was cycled five times. This procedure is known to produce a relatively uniform dislocation substructure as incoherent phase boundaries pass through the sample. 2 ~ 4 This substructure will be superimposed on the heterogeneous cellular substructure from cold rolling. The sample was finally annealed at 300°C in vacuum of 10~ 7 Torr for 2h to remove all but the strongest bound hydrogen. The electrical resistance and magnetic susceptibility characterization of

369

the post-cycle annealed sample constitutes the foreground measurement and is referred to as Pd/PdO:H x below. The residual hydrogen concentration (x) was determined by thermal desorption analysis (TDA) using a procedure described elsewhere6 after the foreground resistance and magnetic susceptibility measurements. Currentvoltage characteristics were measured with the standard four probe technique over a range of 4.2-295 K. The voltage was measured with Keithleyl82 digital voltmeter by passing rectangular current pulses of 1-10 s through the sample with fixed amplitude that varied over a range of 1-10 mA. Magnetic property measurements were performed with IT-SQUID Quantum Design MPMS-3 using both DC-magnetization and AC-susceptibility modes. Samples were mounted inside a gelatin capsule with the applied magnetic field both parallel (H\\) and perpendicular (H±) to the foil surface, the latter of which was measured with a sandwich of six pieces (resulting in an effective sample thickness of 75 /im) to increase the total volume of material. Thermal desorption analysis measurements of the Pd/PdOiHz and P d / P d O samples are shown in Fig. 1. A sharp primary release peak near 430°C superimposed on a much broader peak is evident in the Pd/PdO:Ha; measurement. The binding energies corresponding to the sharp and broad peaks are estimated as £H = 0.65±0.10eV and £H = 0.16±0.05eV, respectively, using the Garlick-Gibson model. 13 The higher energy is consistent with the result of Kirchheim for hydrogen trapping at dislocation core sites in cycled Pd. 5 The lower energy is consistent with

1.60x 10

1.40x 10

1.20 x 10

i£ I . O O x io 7

a> CO

-8

c/> 8.00 x 10 CD CL

1

6.00 x 108 4.00 x 10S

2.00 x 108 0.00 0

100

200

300

400

500

600

700

800

Temperature (°C) F i g u r e 1. solid line).

T h e r m a l d e s o r p t i o n m e a s u r e m e n t s of P d / P d O : H a ; (thick solid line) a n d P d / P d O ( t h i n

370

much weaker hydrogen trapping interaction, possibly at dislocations within in the underlying cellular dislocation substructure of the cold rolled foil Pd 3 and at oxygen vacancies in the PdO. The concentration of hydrogen corresponding to the primary release peak is estimated as (x) = 6.0 x 10~ 4 [H]/[Pd] based on calibration of the TDA system with TiH powder.6 This is the concentration averaged over the entire volume of the sample. The local concentration within one Burgers vector (2.75 A) of the dislocation core will be much higher and can be estimated as (x) ~ 1.8 [H]/[Pd] using simple geometric arguments with an assumed dislocation density of 2 x 10 11 cm~ 2 . 6 The underlying assumptions of this estimate, namely a trapping radius of one Burgers vector and a dislocation density of 2 x 10 11 c m - 2 , have recently been confirmed with small-angle neutron scattering measurements performed below 20 K. 14 Both the high-binding energy and local concentration imply significant band overlap of the Pd and H electron states compared to bulk Pd hydrides with x < 1. Neglecting by free hydrogen distributed far away from dislocation cores, 5 one can calculate an effective hydrogen concentration xefi at deep dislocation core (DDC) x eff = a([H]/[Pd])/7riVdrc2,

(1)

where a is the factor of the Pd atomic density change at dislocation core in deformed Pd f.c.c. lattice: 6 a ~ a0/b = V2(b = 2.75, a0 = 3.89 A), ([H]/[Pd]) = 6.0 x 1 0 - 4 is the average hydrogen concentration with respect to all Pd atoms, N^ = 2.0 x 10 11 c m - 2 , 2 and rc = b = 2.75 A denotes the radius of a segregated hydride cylinder around the DDC. Substituting these values into Eq. (1), we obtain xe^ ~ 1.8 that implies formation of superstoihiometric hydride clusters around the DDC at the Pd-PdO interface. Therefore, both high-hydrogen binding energy and concentration of hydrogen at DDC sites suggest a significant Pd-H common band overlapping at the Pd-PdO boundary The resistance versus temperature for both samples measured with a current of 0.1mA is shown in Fig. 2. The resistance of the Pd/PdOiH^ sample includes a temperature-independent defect component associated with cycle-induced dislocation formation (Matthiessen's rule) equal to 12.20 ± 0.15mfi. This value was obtained by overlapping the resistance curves for Pd/PdOiHa, and Pd/PdO above 200 K, where the contribution of the temperature-independent fraction of the full resistance is negligible.15 The third curve in Fig. 2 corresponds to the temperaturedependent component of Pd/PdOiH^ after the subtraction of the 12.20 mfi value and exhibits enhanced conductivity relative to P d / P d O below 70 K. This enhanced conductivity is best seen in the ratio of resistances shown in Fig. 2 (inset). The ratio of temperature coefficients of resistance (the normalized derivative) versus temperature are also shown in the inset of Fig. 2. The larger coefficient for the Pd/PdOiH^ sample is an indication of a more metal-like behavior. Both the reduced resistance and enhanced temperature coefficient are attributed to condensation of hydrogen at dislocation cores into a metallic-like phase. The enhanced electron transport properties of the Pd/PdOiH^ sample are supported by the V(I) characteristics shown in Fig. 3. The normalized voltage (Pd/PdOiH^ over Pd/PdO) is plotted versus DC current over the temperature

371

28.0

24.0

20.0

0) O

c

30

60

90

120

150

180

Temperature (K) Figure 2. Resistance versus temperature, -R(T), for P d / P d O t H ^ (solid boxes), P d / P d O (solid circles), and fl(Pd/PdO:Ha;)-12.20mn (open boxes, see text). Inset shows the ratios of resistance [it(Pd/PdO:Hj;)-12.20mn]/iJ(Pd/PdO) (solid boxes) and temperature coefficient of resistance d f i / d T ( P d / P d O : H a ; ) / d i ? / d r ^ ( P d / P d O ) (open boxes) versus temperature.

range 4.2 < T < 203 K. The non-linear behavior at low current (<0.0f mA) and low temperature (<50K) indicates enhanced transport properties consistent with uncorrelated supercurrents 16 that break down at high current and high temperature (T > 67K). In the present case, the non-linear behavior may be associated with the suppression of weak superconductivity along a network of condensed hydrogen at dislocation cores analogous to a Josephson medium. Similar filamentary superconductivity has been previously observed in high-Tc superconductors. 17 ' 18 DC susceptibility measurements of both samples are shown in Fig. 4. The zero-field-cooled (ZFC) measurement of Pd/PdOiH^ at 1.0 and 1.5 Oe exhibits a transition below ~70K, manifested as a reduction of the DC susceptibility (the sharp increase in susceptibility below 5K is due to ferromagnetic impurities 19 and non-stoichiometric oxygen in the PdO layer). This transition not present at larger applied field, in the field-cooled (FC) condition, nor in the Pd/PdO ZFC background measurement at 1.0 Oe. The transition is attributed to a diamagnetic contribution to the paramagnetic response of Pd resulting from condensation of the trapped residual hydrogen. Additional proof is found in the magnetization versus applied field

372

15.0 -*

4.2 K

-*

13.5 K

-m 23.5 K

34 K 40 K 47 K 50 K 67 K 90 K 100 K 203 K 0.00 0.001

0.01

0.1

Current (mA) Figure 3. Normalized voltage versus DC current characteristics, V(I), for the temperatures as labeled. The normalized voltage is the ratio of y(Pd/PdO:Ha;) to V ( P d / P d O ) . Non-linear behavior is observed below 0.01 mA for temperatures below 67 K.

shown in the inset of Fig. 4. The 5, 10, and 50 K measurements of the Pd/PdO:H x sample exhibit an inflection between 5 and 7.5 Oe that are not observed in paramagnetic materials. The change in slope is absent below 5 and above 50 K consistent with the paramagnetic response of Pd containing ferromagnetic impurities. AC susceptibility measurements were performed to provide a more sensitive verification of the diamagnetic contribution. Real and imagninary AC suseptibility components for the two samples are shown in Fig. 5. The real component of the Pd/PdOiH^ is weakly diamagnetic below ~40K, while that of the Pd/PdO sample is weakly paramagnetic. The imaginary components differ as well, with the Pd/PdOiH-E sample exhibiting a peak that is absent in the Pd/PdO sample. The onset of the weak diamagnetic behavior and the peak in the imaginary susceptibility coincide with a magnetic phase transformation. The diamagnetic response is enhanced by a factor of 30 when the Pd/PdO:Ha; sample is perpendicular to the applied AC field, as shown in the inset of Fig. 5a. One possible origin of the diamagnetic response from Pd/PdOiH^ is magnetic field expulsion due to skin effect under applied AC field. The skin depth is propotional to 5(T) <~ [cr(T)] — 1/2, where
373

1x10 -5 6.4x10

/

-5

5.6x10 1x10

/'2K

4.8x10

O•

^4.0x10 6 x 10 - —

-

(ft

CO

5K

'•

/

/lOK/

8o" O Q

/

£3.2x10

50 K ,

-/ ^•^

4x10'

100 K

2x10

0x10

if

0 0

-L 50

-L 150

-L 100

_L 200

250

300

Temperature (K) Figure 4. DC susceptibility versus temperature for Pd/PdO:Ha; under ZFC at 1.0 Oe (open boxes), 1.5 Oe (open triangles), and 5.0 Oe (solid diamonds), under FC conditions at 1.0 Oe (solid circles), and for P d / P d O under ZFC at 1.0 Oe (open circles). Inset shows low-field magnetization versus field at the temperatures as labeled.

thickness of 75 fan. Flux expulsion from the foil can account for at most 5% of the observed diamagnetic response in the perpendicular field condition. We therefore assign the diamagnetic transition observed in the AC susceptibility measurements to the presence of a minute fraction of superconducting phase in the Pd/PdO:H^ matrix. Accordingly, the behavior of the low-temperature AC susceptibility in the parallel- and perpendicular-field conditions is in agreement with two-dimensional type II superconductivity when the coherence length is larger than the width of the superconducting layer.20 The emergence of a superconducting network observed here is consistent with McMillan's estimate of the critical temperature; 21 Tc = ((hw)/1.2 kB) x exp

1.04(1 +A) A - / i * ( l + 0.62A)

(2)

where (fko) ~ 58-105 meV is the characteristic average of phonon energy in the condensed phase, A = A(Pd)+A(H) is the electron-phonon coupling constant from the Pd and hydrogen subsystems, and fi* ~ 0.1 is the Coulomb pseudo-potential

374

Figure 5. Imaginary (a) and real (b) AC susceptibility versus temperature for P d / P d O : H z (solid circles) and P d / P d O (open boxes) with parallel applied field. Measurements were performed with H = 0, a driving amplitude of 1 Oe, and a frequency of 992 Hz. The real component of the Pd/PdO:Hj; exhibits a slightly diamagnetic response below 40 K that is amplified by placing the foil surface perpendicular to the applied field (5a inset).

that accounts for the repulsive effect between electrons. The values for (fku) and fi* used here have been discussed previously.6 The electron-phonon coupling constant is estimated as A = 0.89 for (x) = 1.8 based on a linear extrapolation of coherent inelastic neutron diffraction data from Rowe et at6'22 The estimated Tc ~ 40-70K agrees with the onset of both excess conductivity and diamagnetism observed in the Pd/PdOtHz sample. 23 In summary, we have observed anomalies in the electron transport and magnetic properties in a deformed Pd foil with a thermally grown oxide layer and a small residual hydrogen concentration trapped at dislocations. The anomalies are

375

consistent with a filamentary superconducting network that we attribute to the condensation of the trapped hydrogen into a metallic-like phase within the dislocation core. This phase represents a hydrogen dominant metallic alloy, where both hydrogen and palladium atoms may participate in common overlapping bands. 1 Finally, we note that the presence of non-stoichiometric oxygen near the Pd-oxide layer interface may enhance electron-phonon coupling and therefore increase the critical temperature, similar to the cuprates. 23 Note that real critical temperature of weakly linked superconducting filaments of condensed hydrogen/deuterium phase would be much higher than Tc ~ 70 K, suggesting superconducting state at room temperature that is projected for metallic hydrogen. 1 In this connection, the superstoichiometric "metallic" hydrogen/deuterium sites at dislocation cores with respect to LENR's active centers must play an important role in origination of DD-reaction (including multi-body fusion24) in palladium deuterides in non-equilibrium conditions. 3. Conclusions and LENR Connection • DDCs in Pd could be considered as a H/D-dominant Pd hydride {x = H/Pd ~ 2.0) sites suggesting HTS properties. • Triggering of LENR at such sites should be easier than in regular lattice due to: — — — —

shortest-DD-distance (close to Bohr radius); highest D-loading and lattice compression; effective electron screening; large optic phonon energy {hJD > 100 meV) resulting in a most effective lattice-nuclei energy transfer.

• Metallic H/D superfluid25 suggests dramatic enhancement of quantum entanglement between deuterons at those sites Acknowledgments This work was partially supported by the NSF under Grant No. DMR-9982520 and by New York Community Trust. The magnetic property measurements were performed at the Frederick Seitz Material Research Laboratory at UIUC supported by the U.S. Department of Energy under Grant No. DEFG02-91-ER45439. The authors would like to thank Dr. A. Bezryadin (UIUC) and Dr. R. Prozorov (University of South Carolina) for useful comments. References 1. 2. 3. 4. 5.

N.W. Ashcroft, Phys. Rev. Lett. 92, 187002 (2004). B.J. Heuser and J.S. King, J. Alloys Compd. 261, 225 (1997). B.J. Heuser and J.S. King, Metal. Mater. Trans A 29, 1594 (1998). M. Maxelon et al., Acta Mater. 49, 2625 (2001). R. Kirchheim, Acta Metall. 29, 845 (1981).

376

6. A.G. Lipson et al, Phys. Lett. A 339, 414 (2005). 7. G. Elsasser et at, J. Phys.: Cond. Matter. 4, 5207 (1992). 8. B. Strizker and H. Wuhl, in: Hydrogen in Metals II. Topics in Applied Physics, v. 29, Ed., G. Alefeld and J. Volkel, Springer Verlag, Berlin (1978). 9. L. Schlapbach, I. Anderson, and J.P. Burger, in Material Science and Tech., v.3B Part II, ed. K.H. Jurgen Buschow, p.287, Weinheim, New York (1994). 10. J. Miller and C.B. Satterthwaite, Phys. Rev. Lett. 34, 144 (1975). 11. J.E. Schriber and C.J.M. Northrup Jr., Phys. Rev. B 10, 3818 (1974). 12. D. Wang et al., J. Alloys Compd. 348, 119 (2003). 13. G.F.J. Garlick and A.F. Gibson, Proc. R. Soc. Lond. Sect. A 60, 574 (1948). 14. B.J. Heuser, G.S. Danagoulian, and A. Lipson (to be published). 15. N.E. Alekseevskii et al, Physica B 163, 659 (1990). 16. A.A. Abrikosov, Phys. Rev. B 64, 104521 (2001). 17. P.M. Grant et al, Phys. Rev. Lett. 58, 2482 (1987). 18. C. Panagopoulos et at, Phys. Rev. B 69, 144508 (2004). 19. H.C. Jamieson and F.D. Manchester, J. Phys. F: Metal Phys. 2, 323 (1972). 20. M. Tinkham, Introduction to Superconductivity, 2nd Ed., McGraw-Hill, 1996, NY. 21. W.L. McMillan, Phys. Rev. 167, 331 (1968). 22. J.M. Rowe et al, Phys. Rev. Lett. 57, 2955 (1986). 23. A.G. Lipson, et al, Phys. Rev. B 72, 212507 (2005). 24. A. Takahashi, Proc ICCF 11 (Marseille, France, 2004). 25. E. Babaev, A. Sudbo, and N.W. Ashcrof, Phys. Rev. Lett. 95, 105301 (2005).

N E W P R O C E D U R E S TO M A K E ACTIVE, FRACTAL-LIKE SURFACES ON THIN Pd WIRES

F R A N C E S C O C E L A N I , A. S P A L L O N E , E. R I G H I , G. T R E N T A , G. D ' A G O S T A R O , P. Q U E R C I A , V. A N D R E A S S I , A N D O. G I A C I N T I INFN-LNF

Via E. Fermi 40, 00044 Frascati (Rome), E-mail: [email protected]

Italy

P. M A R I N I , V. DI S T E F A N O , M. N A K A M U R A , F . T O D A R E L L O , A N D E. P U R C H I EURESYS,

Via hero 30, 00129 Rome,

Italy

A. M A N C I N I ORIM

SpA,

Via Concordia

65, 62100 Piediripa

(Macerata),

Italy

P. G. S O N A Via S. Carlo 12, 20090 Segrate

(Milan),

Italy

F . F O N T A N A , L. G A M B E R A L E , A N D D. G A R B E L L I Pirelli Labs SpA,

Viale Sarca 222, 20126 Milan,

Italy

E. C E L I A , F . F A L C I O N I , M. M A R C H E S I N I , A N D E. N O V A R O CSM SpA,

Via di Castel Romano

100, 00129 Rome,

Italy

U. M A S T R O M A T T E O ST Microelectronics

SpA,

Via Tolomeo

1, 20010 Cornaredo,

Italy

In the framework of anomalous effects coming out because very close interaction of some specific gas [usually Deuterium (D), some times hydrogen (H)] with some specific solid materials [usually Palladium (Pd), some times Nickel or others] is an emerging evidence that the physical condition at the surface of the host element play a crucial role. It has been experimentally demonstrated, by Yoshiaki Arata at Osaka University, that nano-particles of Pd, embedded in a matrix of Zr02, are able to absorb extremely large amounts of H and/or D, at even room temperature and pressure. Because of such results, we re-analyzed some of our previous experiments under the new point of view and were convinced that most of our "positive" results in Condensed Matter Nuclear Science come because of lucky, specific condition of our Pd cathode. We decided to improve the quality of Pd, from the point of view of production of nanostructure at its surface as large (and stable) as possible, in a controllable way, using both electrolytic procedure and special preparation of Pd before the use. Some of our efforts seemed to give positive results, although the stability at long time as to be improved. 377

378

1. Introduction In the framework of Condensed Matter Nuclear Science, it has been recently shown, by Yoshiaki Arata at Osaka University,1 that nano-structures of metallic palladium, stabilized in a matrix of ZrC>2, can rapidly absorb surprisingly large amount of H 2 or D 2 . According to Arata's results and to the Akito Takahashi2 theoretical model, atomic ratios (H, D)/Pd ;§> 1 can be easily accomplished at a pressure of only a few bars into Pd nano-particles, stabilized in a Z r 0 2 matrix. In the Arata's experiments, together with the abnormally high D/Pd ratios, a remarkable excess heat and production of 4 He were detected. On the basis of such results (and new deeper interpretation of some of our previous experimental results 3 that, although quite interesting from the point of view of experimental effects, did not get at that time a satisfactory explanation), we are now convinced that most of the high loading ratios (H-D/Pd) and/or anomalous effects, both thermal and nuclear (by using D), obtained (generally in a not reproducible way) by the people involved in cold fusion experiments, can be reasonably attributed to the spontaneous and uncontrolled growing-up of fractal nanostructures on the Pd surface. In our opinion, even the Sr and Cs transmutations obtained in the experiments carried out by Iwamura et al.A at Mitsubishi Heavy Industries, Yokohama, Japan, which occur on the surface of the P d / P d - C a O / P d multilayer, could be due to the formation of fractal-like structures produced during the multilayer fabrication process. The present work deals with experiments aimed at the production of nanostructures on Pd wires both by anodic oxidation (in situ) and air oxidation (in situ and ex situ). 2. Experimental Procedures 2.1. Cells and

Electrolytes

The cell geometry and the experimental set-up were reported in detail in our previous papers.5"8Along the last year, about usual electrolytic experiments, we make two specific one in order to compare and cross check the results about new elements detected by ICP-MS, using light and heavy electrolytes. The cell and experimental set-up were almost the same as described in Refs. 5-8. We just changed the composition of cell (from chemical glass to quartz) in the last experiment with deuterium (b-type), as detailed in Ref. 8. (1) Hydrogen loading: Th(N0 3 ) 4 = 5 cm 3 (concentration 1 0 - 3 Fortuna) cell. (2) Deuterium loading: Th(N0 3 ) 4 = 6 cm 3

main solution 750 cm 3 (C 2 H 5 OH 95%, H 2 0 5%); (with 1 cm 3 = 1 mg of Th in D 2 0); Hg 2 S0 4 = 7 cm 3 M, in D 2 0) - Chemical glass (Schott Duran like, brand main solution: C 2 H 5 OD = 1005 cm 3 , D 2 0 = 89 cm3; (with 1 cm 3 = 1 mg of Th in D 2 0 ) ; Hg 2 S0 4 = 8 cm 3

379

(concentration 10~ 3 M, in D 2 0); NH 4 OD (0.16 M, in D 2 0 ) = 6 cm 3 - Ultra pure quartz cell. 2.1.1. Procedure for the anodic oxidations in situ The Pd wires were H, D loaded up the maximum of R/Ro (H,D /Pd ~ 0.75) by a current density of 5-10 mA/cm 2 . The wires were then anodically de-loaded with a current density of 1-2 mA/cm 2 and when the de-loading reaches the point R/Ro —1-1 or less, the current is raised to 5-20 mA/cm 2 and kept for a few minutes until full deloading. 28ago05a-10_17 1.8

120

1.6

E 8 1.4 Of -40 1.2 -80

-120

1 2.03 x 1 0 s

2.035 x 1 0 s

2.04 x10 5

2.045 x 1 0 s

2.05 x 1 0 s

Time (s)

Figure 1. R/Ro ratio versus time using optimized anodic oxidation and electrolyte composition. The solution is quite insulating (main liquid is vacuum-distilled andlOO nm filtered C2H5OH+H2O, few salt are dissolved): the cell voltage is 135 V even at only 30 mA with an anode-cathode distance of 4 cm.

2.1.2. Electrolytic

hydrogen loading after the anodic oxidation

in an alcohol

solution An example of very good result, using the combined effects of previous Pd anodic oxidation, proper electrolyte composition and effect of cathodic current, is shown in Fig. 1. The loading rate is extremely high and after 300 s the maximum of R/Ro is reached and surpassed. After that, the loading proceeds still at a surprisingly high rates up to values of R/Ro down to 1.2 (right-hand side of the Baranowski curve), within ~700 s, and down to 1.15 within 1500 s. It should be noticed that without the anodic oxidation the time for loading up to i?/i?o — 1.6-1.5 (right-hand side of the Baranowski curve) is measured by the tens of hours.

380

These results indicate that a proper anodic oxidation produces a very active surface. On the basis of Arata experiments, such activity could be explained as due to the formation, just at the surface of the wire, of something similar to Arata's true nano-particles (embedded in a matrix of ZrO^)2.1.3. Electrolytic deuterium loading after the anodic oxidation Generally, the loading experiments carried out with electrolyte b-type showed lower loading rates and lower maximum (final) loading with respect to the ones with electrolyte a-type. Typically the maximum loading did not exceed the one correspondent to R/Ro — 1-6 (right-hand side of the Baranowski curve). Anyway, deuterium-based electrolyte some times showed anomalous effects like excess heat and "new" elements as detected by ICP-MS (routinely) and (sometimes) SEM microanalysis. 2.1.4. ICP-MS results In consideration of the fact that all our previous electrolytic loading experiments in both (a) and (b) electrolytes, included anodic de-loading cycles, i.e., anodic oxidation, we routinely examined electrolytes, wire and sediments in order to check whether some transmutations had occurred. The main motivation of ICP-MS analysis was the results of Sr to Mo transmutation, shown in a very elegant experiment, by Yasuhiro Iwamura team (at Mitsubishi Heavy Industries, Yokohama, Japan), in 2002.4 We recall that, at that times and since 1998, we were using Sr as main electrolyte in our heavy water and/or heavy ethyl alcohol mixtures. We detected 9 some Mo in our Sr based electrolyte experiments, confirming the Iwamura results using a very different environment (liquid electrolyte instead of pure and pressurized deuterium gas). The latest results about main new elements, detected by a high resolution ICPMS, are reported in Table 1 and were presented at ICCF6. 8 See Table 1 comments for further details. 2.2. Deuterium

Self-loading

after Electrolysis

and SEM

Analysis

In many of the previous electrolytic D loading experiments, after some anodic oxidation cycles had been carried out, we found evidence (although not fully reproducible) of spontaneous deuterium self-loading, i.e. without applied electrolytic current, of the Pd wires immersed in the electrolyte. The deuterium was absorbed from the gas dissolved in the solution due to previous electrolysis. This assertion is demonstrated by the fact that the value of the loading is reversibly controlled by controlling the concentration of the dissolved D2 through alternatively bubbling Ar/D2 , as shown in Fig. 2. In Fig 2, at the time 269,500 s, the anodic stripping was ended (the current, from —9 mA was returned to 0 mA). Almost immediately, the wire started to absorb

381 Table 1. Main new elements detected in light alcohol-water (Scott Duran type) and heavy alcohol-water (quartz) cell. All the reagents Th(NOs)4 (at 1 rng/ml concentration) and Hg2S04 (10~ 3 M) are i n D 2 0 . BKG and reagents subtracted. 1 Count = about 5 X 10 1 0 atoms. In bold characters are reported value of new elements, about deuterium experiments, larger than a factor 10 in respect to hydrogen one. Element (isot. ab. %)

HJoading Exp. counts

D-loading Exp. counts

Comments

p

0 0 2.3 x 10 6 63/65 = 2.20 6.2 x 10 6 3.1 x 10 4 Normal 6.5 X 10 6 1.86 X 10 4 1.16 X 10 4 80 4.5 x 10 5 1.1 x 10 3 4.3 x 10 7

6.4 x 10 6 1.8 x 10 7 2.5 x 10 7 63/65 = 2.11 4.9 x 10 7 8.2 x 10 4 Depleted of 5% 2.6 x 10 6 1.31 x 10 5 4.42 x 10 4 900 1.38 x 10 7 1.0 x 10 4 10.8 x 10 7

BKG = 4E3 BKG = 1E6 Nat. 63/65 = 2.25

39

K

Cu Zn Rb 108 P d (26.5%) Ag 140 Ce(88.5%) W Tl Pb U 195 P t (33.8%)

Marker anode dissolution

19-20JAN05

2.68 x10 5

2.7 x105

2.72 x10 5 2.74 x10 5 Time (s)

2.76 x10 5

2.78 x10 5

Figure 2. R/Ro versus time (seconds) with the effects of D2 - ^ A r ^ D 2 intake and anodic stripping current (A). The values of R/Ro are "twin" because we introduced the procedure to measure also the Resistive Thermal Coefficient (RTC), see later.

382

the deuterium dissolved in the solution and the R/Ro increased from about 1.05 to about 1.405. At the time 273,500 s large amount of Argon gas was introduced, by bubbling it inside the solution. Immediately, the R/Ro started to decrease. At the time 275,500 s, after the R/Ro decreasing (because of argon effect) from 1.405 to 1.375, D2 gas was added again. The R/Ro value again increased, showing reversible and controllable effects. At the time 277,300 s, when the R/Ro increased to 1.45, the intake of D2 was stopped and Argon was added again. At the end, another anodic de-loading was carried out (at -6 mA) in order to fully de-load the wire. Moreover, observing Fig. 3, we would like to stress that there is unquestionable experimental evidence that the spontaneous self-loading following anodic oxidation reaches values of D/Pd over the well-known thermodynamic limit. In other words, we expected a R/RQ ratio less than 1.8 but we observed a value much larger, close to 1.95-2.0. Such value is equivalent to a deuterium pressure of about 8-10 times larger than 1 bar, i.e. the D2 pressure used in the cell (e.g. time 287,000-300,000 s). 19-20JAN05

0.002

- -0.008

2.8 x10 5 Figure 3. Fie. 2.

2.85 x10 5

R/RQ versus time. R/Ro

2.9 x10 5 Time (s)

2.95 x10 5

3x105

is about 2 instead of 1.8 expected. Other comments like

In Fig. 3, it is shown the spontaneous loading of deuterium gas dissolved in solution (time 282,000-300,000 s). At the time 279,000 s the anodic de-loading was ended in an argon atmosphere. At the end of the anodic cycle a weak selfloading was observed. Later (time 281,000 s) argon was again added for calibration purposes. At the time 282,000 s deuterium gas (at about NTP, overpressure of only 50 mbar) was finally added and self-loading started immediately. The R/RQ values are >2.0 (time 290,000 s) because of the effect of residual stress (R/Ro at D/Pd = 0 is increased to about 1.05 with respect to 1.00 at the time "0" at the beginning of the experiment). In other words, the wire was de-loaded (at the time 282,000 s) and intentionally we did not correct (by mathematic calculation)

383

the value in such experiment because we decided to "monitor" the value of the residual stress versus time. 2.2.1. SEM micro-photography and microanalysis In Figs. 4-6 are shown some pictures, by SEM microphotography, of Pd wire before (Fig. 4) and after (Figs. 5 and 6) D electrolytic loading. Elemental analysis (by microprobe) of some "white" area of Fig. 6 are shown in Fig. 7. Figures 4-7 are the same as presented at JCF6. The wire analyzed was about 10 cm long out of 60 cm total. The new elements are concentrated within about 15% of the total length, in a random like distribution.

Figure 4. SEM picture of Pd virgin wire, before electrolysis. The wire is contiguous to used one of Fig. 4.

It is clearly shown the problem coming out from anode dissolution and its deposit at Pd cathode surface. Such deleterious effect, in respect to H and D absorption in Pd, is not yet solved (despite our deep efforts). We recall that, unfortunately, the over-volt age of H and D at Pt surface is close to zero. We are convinced that one of most important reasons of poor deuterium loading into palladium, as reported from several researchers, is very often the platinum coating (from the anode) at palladium cathode surface, specially at large current density (over 500 mA/cm 2 in water solution). It is interesting to note that, apart sensitivity, the same elements are detected from both SEM and ICP-MS. In other words, the ICP-MS results are "safe" and are not instrumental fakes.

384

Figure 5. SK\! picture of a usf\l wire, heavy solution clc-tmlysis. The "new" HIMIUMIIS and P t deposit (from anode) are concentrated in few spot area (about 15% of wire length).

2.3. Air Oxidation

of Pd and

Coating

As we have shown, in our electrolytic loading experiments, we observed the phenomenon of spontaneous deuterium loading, i.e. without the application of any electrolytic current (self-loading). After several years of observations and specific

Figure 6.

Details of deposits as reported in Fig. 5.

385

tests, we realized that large self-loading occurred only at the end of certain anodic cycles, in specific electrolytes. In particular, we found that the self-loading effect obtained with water electrolytes was almost negligible (R/RQ « 1.1), while with hydro-alcoholic electrolytes, both a- and b-types, the effect was higher. By optimizing the anodic cycle it was possible to reach self-loadings up to R/RQ = 1.75 (left-hand side of the Baranowski curve) with H 2 and R/R0 = 1.95 (left-hand side of the Baranowski curve) with D2.

5000 Pt

Counts

0.000

keV

20.480

Figure 7. SEM elemental analysis of one of "white" area has shown in Fig. 5. The, unwanted, large deposition of Pt at Pd surface is clearly detected. Moreover, also Zn and Cu, detected by ICP-MS analysis, are re-confirmed.

SEM microphotography of the Pd wires, which presented strong self-loading effects, show the presence of thin porous structures on the surface of the wire. It was also observed that during the anodic cycles in hydro-alcoholic electrolytes a significant diffused pitting corrosion occurs both of Pd and Pt electrodes. ICP-MS revealed a consistent presence of Pt in the electrolyte, in the sediments and on the Pd surface. These facts suggested that in such electrolytes the anodic cycles produced strong oxidations of the Pd (useful) and Pt (deleterious, see previous discussion about over-voltage) wires. These considerations led us to try a high temperature air oxidation of Pd wires as an alternative and more practical mean for obtaining active palladium surfaces. Since the first trials we found out that this simple procedure is scarcely effective. As a matter of fact it produced slight and unstable self-loadings and only for once. We considered that during the anodic cycles, in addition to anions, negatively charged particles are electrophoretically deposited on the Pd electrode and that this effect is enhanced in an alcoholic environment, so we thought that for a significant self-loading to occur, the presence of an impurity layer, intimately adherent to the

386

oxidized surface, might be a necessary condition. So we resorted to artificially apply such impurities to the oxidized Pd wire in the form of colloidal silica. 2.3.1. Procedure for the preparation of the samples A thin (50 /xm diameter) and long (60 cm) Pd wire was Joule heated in air (=600 mA for 60 s) at about 700°C in order to get a thin layer of PdO.

01-03MAR05_KI

I a&%Stt)»»a«S&>

" Pac

|

*

1.8

-

0.8

0.6

1.6

cf? 1.4

- R/Ro_d

- 0.4

1

| 0.2

1.2

0

fe^SU^SSSUKSS*

5x10

4

1x10

5

1.5 x 1 0

s

2 x10

s

2.5 x 1 0

5

3 x10s

Time (s) Figure 8. Loading characteristic of a virgin palladium wire: loaded at room temperature with lbar of deuterium gas. In order to "activate" the Pd surface, it was made a preloading cycle (from time 0 to about 60,000 s) with D2 gas, 293 K, 1 bar and later allowed to decrease, very slowly, the deuterium content in the cell. Even neglecting the activation time, the time needed to reach the thermodynamic limit of R/Ro = 1-82 is as large as 220,000 s. Such values (i.e. R/RQ and time) are in agreement with data usually reported in the literature. As standard in our procedure from about 2 years, we cyclically inject electromigration ac current (square wave, 10 kHz) with low (about 10-15 m W ) and high power (700-800 mW) in order to calculate the Resistive Thermal Coefficient versus D / P d ratio.

After such a heat-treatment the wire was immerged into a diluted solution of colloidal silica, and then heated-^cooled^heated^cooled again several times. 2.3.2. Measurements Virgin Pd wires (no treatment) exposed to D2 gas at 1 atm and ambient temperature, usually reach a maximum loading, corresponding to an electric resistance ratio R/R0 « 1.82, in over 2 days (Fig. 8).

387

The wires, treated according to the reported procedure, exposed to hydrogen or deuterium in the same condition, instead, showed extremely fast, and quite larger, loading rates. In Fig. 9 is shown the case of a wire exhibiting an astonishingly high loading rate: the electric resistance ratio (R/RQ) of the wire exposed to a 1 atm D 2 gas, at 24° C, reached the value of 1.90 in about 100 s. The maximum R/R0 value of 1.98 (D/Pd S 0.75) was reached 2 min later, and remained stable for a long time. Further details, by the authors of this paper, are shown in the JCF6 proceedings. 19APR05.196

0.15

0.05

5.74 x 1 0 4 5.75 x 1 0 4 5.76 x 1 0 4 5.77 x 1 0 4 5.78 x 1 0 4 5.79 x 1 0 4

5.8 x 1 0 4

Time (s) Figure 9. (1 bar).

Loading ratio versus time of a Pd wire treated by oxidation and silica. D gas loading

It was also found that if during the treatment procedure of the wires, the step involving the immersion in colloidal silica is omitted, the loading rates are significantly lower and after a couple of hours R/RQ starts to decrease (de-loading). 3. Safety Rules-Procedures The following procedures have to be carefully followed to avoid explosions because possible mixing of hydrogen (and or deuterium) with oxygen and highly catalytic effect of palladium surface, activated because growing of nano-structure at its surface. We remark the safety procedures are quite easy in our experimental setup because we take fully advantage of our procedure to measure both the R/RQ value and the Resistive Thermal Coefficient (RTC) of Pd wire versus loading (see our

388

reports at, Asti5, ICCF11, and JCF6 for further details). In such a case, we used the ratio between the RTC value made by injecting alternatively low (about 15 mA equivalent to about 10 mW of power dissipated, called R/R0JL) and high (about 120 mA, equivalent to abut 700 mW power dissipated, called R/R0J1) AC current along the thin Pd wire. Because very different thermal conductibility of gas was adsorbed (H 2 , D 2 , He, Ar, Air, and "vacuum"), after proper calibration once for ever, it is very easy to understand the real composition of gas atmosphere inside the cell.

3.1. Typical

Situation

New Joule heating of the wire (0.05 mm diameter) that previously was H and D loaded. The aim is in situ new oxidation by air to get fresh PdO for further tests. The procedure is detailed, step by step, as follows. (1) Intake, and flux, Ar gas. * Measure continuously R/RQ-L and R/RQ-H. * End the large intake of Ar only when the ratio between R/RQJI and R/RO-L increases largely (and stabilize) due to the lower thermal (at 0°C, 1.013 bar) conductivity of Ar (16.36 mW/m*K) in respect of H 2 (168.35 mW/m*K) or D2(130.63 mW/m*K). (2) Increase, slowly, the DC I_electromigration (/.em), from 0 to 350 mA, keeping Ar flux at low values. (3) Observe deloading. (4) Wait for complete deloading (10-30 min, depending on wire coating). Decrease 7_em from 350 to 0 mA. (5) Check R/RQ-L value: if close to 1.0, go to step 6, otherwise wait until full deloading by injecting 7_em again at large value (350 mA). (6) Intake of He for test: the ratio of R/RQJI versus R/R0-L as to decrease largely in respect to Ar filling, due to the larger thermal conductivity of He(142.64 mW/m*K) in respect to Ar. (7) Make vacuum (e.g. oil-free membrane pump, limit about 10 mbar) to pumpout He. (8) Intake of dry air (thermal conductivity, at 0°C 1.013 bar, 23.94 mW/m*K) at STP. I.em = 0 mA. Measure R/R0-L only. (9) Increase Lem from 0 to about 600 mA. Wait 1 m at 600 mA. Observe the R/RQ instantaneous increasing due to large Lem: R/Ro about 3. At R/Ro = 3 the wire temperature is about 700°C. (10) Decrease slowly (in about 2 m) /.em from 600 to 0 mA. Repeat the cycle three times. (11) Check the R/Ro value and recalibrate the value, if necessary.

389

(a) Reintroduce the R/R0JL and R/R0JI cycles. (b) If all was correct, the values of R/RQJL and H, in air at NTP, are respectively: 1.00, 1.13 (input current of about 15 and 120 mA). (12) Make vacuum and check if the values of R/R0.L and R/RoJi have the proper values as expected. They are used the calibration data obtained at the beginning of the experiment. (13) Wash the cell with Ar or He. Later on, make vacuum again. (14) Intake of H2 or D2 and observe loading and cell temperature. By the way, we observed that some residual He gas, at the order of 1%, instead of usual Ar, has a beneficial effect about both maximum value of loading and anomalous effects generation. Such phenomena as to be more deeply investigated. (15) Stop immediately any current, and inject/wash with He or Ar, if cell temperature and/or pressure increase in an anomalous way. 4. Conclusions According to us, almost all of positive experimental results (excess heat, transmutation, and particle emissions) in cold fusion experiments (Fleischmann, Takahashi, Arata, Iwamura, Mizuno, Celani, McKubre, Swartz, Storms, Preparata-De Ninno-Del Giudice, Miley, Violante, etc.) can be rationalized as the effect of nanostructures at the Pd surface. It is very difficult to produce such nano-structures (almost all, except Arata, Iwamura, and Celani) obtained just by chance. Moreover, such nano-structures are not stable over time. We begin to develop a simple procedure to obtain nano-structures, both by electrolysis (routinely produced also during the usual cathodic regime: specific electronic circuit and procedure developed from our Group since 2004, patenting) and by addition of colloidal silica on oxidised Pd surface (since March 2005, gas loading). In some aspects, the latter method is similar to Yoshiaki Arata procedure that was the Pioneer about nano-particles production for cold fusion studies. The kind of colloidal silica (5-10 nm dimension, low Na content), that up to now gives the best results, was specially developed (after 5 years of efforts), by an Italian chemical company, according to our request. We think that the nano-structure interpretation of anomalous effect in deuterated metals will bring soon to some technological device: boiler using liquid electrolyte, even some turbine engine using pressurised high temperature gas loading method. More systematic work is necessary in order to elucidate all the possibilities that come because nano-size materials (specially pure Pd and/or Pd-based alloys) properly coated/embedded by a third element. Finally, as shortly shown also during ICCF12, we get indications that some anomalous heat seems coming out, from a new pressurised (4 bar) cell (SS), using even the hydrogen gas when the temperature of the wire, heavy coated by colloidal silica, was forced to reach about 200°C (by Joule heating).

390 Acknowledgements We are really indebted to Prof. Akito Takahashi (Osaka University, J a p a n ) , Prof. Yoshiaki A r a t a (Osaka University) and Dr. Yasuhiro Iwamura (Mitsubishi Heavy Industries, J a p a n ) , because stimulating discussions, critics and suggestions about the role of nanostructures in Condensed Matter Nuclear Science experiments. We cannot forget t h a t the pioneer work of Prof. A r a t a about nano-particles (starting with the use of "palladium black" at different grain sizes) which opened our eyes about new interpretation of some of our old d a t a t h a t never get satisfactory explanation. Other general and long discussions with Prof. H. Y a m a d a and S. Narita (both at Iwate University, J a p a n ) , Prof. A. K i t a m u r a (Kobe University, J a p a n ) , Prof. T. Mizuno (Okkaido University, J a p a n ) , Prof. S.E. Jones (BYU, Utah, USA), Dr. E. Storms (Lattice Energy LLC, New Mexico, USA) helped us to elucidate the very complex behaviour of P d surface during and after, very different, electrolysis operating conditions. Dr. W . Collis (Heidi Limited, 14055 Boglietto di Costigliole, Italy) helped us during the very long a n d tedious analysis of possible elements coming out by ICP-MS instrument. T h e special software program (ENSAT) he developed, about possible "transmutation" channels, was really useful to speed-up the analysis. References 1. Y. Arata, The formation of 'solid deuterium' solidified inside crystal lattice and intense solid-state nuclear fusion (cold fusion), II Nuovo Saggiatore (Bollettino SIF, ISSN 1827-6148), Vol. 20, No. 5-6, pp. 66-71 (2004). Also at: http://www2.sif.it/riviste/nsag/nsag-2004-05-06/07.pdf; ** Y. Arata and Y. Chang, Proc. of ICCF10, 24-29 August 2003, Cambridge, USA (Edited by P. Hagelstein and S. Chubb), World Scientific (ISBN 981-256-564-7) pp. 139-157 also at http://www.lenrcanr.org; *** Private Communications. 2. A. Takahashi, Proc. of ICCF10, 24-29 August 2003, Cambridge , USA (Edited by P. Hagelstein and S. Chubb), World Scientific (ISBN 981-256-564-7), pp. 447-454, 809818 also at http://www.lenr-canr.org; ** Conf. Proc. (Edited by H. Yamada) of JCF4, JCF5, JCF6 also at http://wwwcf.elc.iwate-u.ac.jp/jcf/;*** Private Communications 3. F. Celani, A. Spallone et al. Study of deuterium charging behavior in palladium and palladium alloy plates, changing surface treatments, by [is pulsed electrolysis, Proc. of ICCF5, Montecarlo, Monaco, 9-13 April 1995, pp. 411-418. 4. Y. Iwamura et al, Jpn. J. Appl. Phys. (2002) 4642; ** Y. Iwamura et al, Proc. of ICCF10, 24-29 August 2003, Cambridge. USA (Edited by P. Hagelstein and S. Chubb) World Scientific (ISBN 981-256-564-7) pp. 435-446; *** Proc. of IGCF11, Marseilles, France, 01-05 November 2004 (Edited by J. P. Biberian), World Scientific (ISBN 981256-640-6) pp. 339-350, also at http://www.lenr-canr.org; **** Conf. Proc. (Edited by H. Yamada) of JCF4, JCF5 also at http://wwwcf.elc.iwate-u.ac.jp/jcf/ 5. F. Celani, A Spallone et al. Proc. of ICCF10, 24-29 August 2003, Cambridge, USA (Edited by P. Hagelstein and S. Chubb) World Scientific (ISBN 981-256-564-7), pp. 379-397 also at: http://www.lenr-canr.org 6. F. Celani et al, Further tests on composition and isotopic anomalies when Pd thin cathodes are electrolized in acidic C2H5OD/D2O mixture added with Th-Hg salts at micromolar concentration, Proc. of the 5 Meeting of Japan CF Research Society,

391 15-16 December 2003, Kobe University, Japan. (Edited by H. Yamada), pp. 41-45, also at http://wwwcf.elc.iwate-u.ac.jp/jcf/ 7. F. Celani et al., Innovative procedure to measure, in situ, resistive thermal coefficient of H(D)/Pd during electrolysis and cross-comparison of new elements detected in T h - H g Pd-D(H) electrolysis cells, Proc. of the ICCF11, Marseilles, France, 01-05 November 2004 (Edited by J. P. Biberian), World Scientific (ISBN 981-256-640-6), pp. 108-127, also at: http://www.lenr-canr.org 8. F. Celani et al, Further studies, about new elements production, by electrolysis of cathodic Pd thin-long wires, in alcohol-water solutions (H,D) and Th-Hg salts. New procedures to produce Pd nano-structures, Proc. of the 6 Meeting of Japan CF Research Society, April 27—28 December 2005, Tokyo, TIT, Japan (Edited by H. Yamada) also at h t t p : / / wwwcf.elc.iwate-u.ac.jp/jcf/ 9. F. Celani, A. Spallone et al. Proc. of the 4 Meeting of Japan CF Research Society, 17-18 October 2002, Japan (Edited by H. Yamada), pp. 17-21, also at http://wwwcf.elc.iwate-u.ac.jp/jcf/

USING RESISTIVITY TO M E A S U R E H / P d A N D D / P d LOADING: M E T H O D A N D SIGNIFICANCE

M . C . H . M C K U B R E A N D F.L. T A N Z E L L A SRI International,

Materials

Research Laboratory, 333 Ravenswood CA 94025, USA E-mail:[email protected]

Avenue,

Menlo

Park,

The resistance ratio method is the most frequent technique used to determine the extent of interstitial loading of hydrogen or deuterium atoms into palladium electrodes, or extended structures used in electrolytic or gas phase cold fusion experiments. Specifically, advantage is taken of an empirical relationship between the measured resistance, R, normalized to that of the same body at the same temperature in the absence of hydrogen isotope, Rg, hence R/Ro, and the atomic fraction occupancy of octahedral interstitials, x = H / P d or D / P d . This method was first suggested and employed in cold fusion studies by the present authors, and received immediate and widespread acceptance because of the ease with which this experimental technique could be used to make in situ, real-time measurements of a parameter, D/Pd, anticipated or hypothesized at that time to relate to cold fusion heat excess or nuclear production. We take up this topic again 15 years later in an attempt to clear up some errors and misunderstandings regarding the resistance ratio method and its application in cold fusion studies. The relationship between R/Ro and x is empirical. That is, calibrations are only as good as the experiments that support the shape of the curve and cannot be used outside the range (P, T, x) in which data are taken. The original calibration (unaccountably and erroneously immortalized as the "famous Baranowski curve") involved an extrapolation of known data into the region of cold fusion interest in the D - P d system, at x > 0.6. Present theory and results focus new attention on the very high loading region as x approaches or even exceeds unity, where double occupation of octahedral sites, tetrahedral site occupancy, new phase formation or new electrical states, may be relevant to the underlying physical process of excess heat and nuclear production. Rather than simply using the resistance ratio as a qualitative tool to determine whether an electrode is better or lesser loaded, it is now important to obtain accurate quantitative information for x close to unity. With further experimentation and analysis of published data it is apparent that the curve originally published in 1990 is in error in the high loading condition. This paper describes how this empirical fit has been improved over the years for both H / P d and D / P d by employing new data, new analysis of old data, new experimental methods and results.

1. Introduction The first paper drawing attention to resistance ratio measurement as a means to quantify deuterium loading in Fleischmann-Pons electrolytic cold fusion experiments was presented by the present authors at the First Annual Cold Fusion 392

393

Conference held in Salt Lake City in March 1990, and published in the ensuing proceeding.1'* The authors of that paper made three introductory comments: 1. None of the "cold fusion" electrolysis experiments described to data contain any means of determining the D/Pd content in situ. Yet this ratio may be a crucial difference between those experiments that have produced a Fleischmann-Pons effect and those that have not. 2. The resistance of Pd metal is a function of its hydrogen content and is in principle, the easiest way of determining the state of the Pd electrode as the experiment proceeds. 7 3. The relationship between the resistance and the D/Pd ratio is known only up to 0.65. Comparison can be made with the H/Pd system which is calibrated in resistance up to H/Pd = l.l. 8 The first two comments proved to be prophetic. A clear distinction can be made on the basis of average D/Pd loading measured by resistance ratio between successful and unsuccessful excess heat production in electrolytic Fleischmann-Pons experiments. Resistance ratio measurements quickly became and remain the most widely used method of determining loading in situ. Here we expand point 3. 2. Experimental In 1990 the resistance versus composition function had been characterized for the light hydrogen system up to H/Pd = l.l. 8 This function was less well specified for D/Pd. Our initial attempt to estimate the curve based on known data 9 up to D/Pd = 0.65 combined with the assertion that the resistance ratio maxima would occur at the same composition of H and D, resulted in the somewhat distorted curve presented at ACCFl 1 and replotted here as Fig. 1. The fourth-order polynomial extrapolation plotted as a grey line in Fig. 1 formed the basis of all early estimates of D/Pd loading from resistance ratio measurements. Between 1990 and 1993 a campaign of measurements was undertaken to refine the calibration of the resistance curve for D/Pd. A number of methods were used to measure composition independent of resistance in the D/Pd system, each with important advantages and disadvantages. Some of these methods are briefly reviewed here: I. Macro-gravimetric. The most direct method to determine the extent of absorbed hydrogen isotope is to weigh the cathode after prolonged loading. Both the resistance and mass measurement can be performed ex situ after washing and drying the electrode. The primary disadvantages being relatively low accuracy because of systematic errors due to the presence of surface adsorbed non-hydrogen species and absorbed but non-interstitial hydrogen, and the lack of access to the high loading region because of rapid deloading. *Although the atomic ratio D / P d had been anticipated 2 and hypothesized 3 - 8 at that time to relate to cold fusion heat excess or nuclear production.

Micro-gravimetric. An in situ gravimetric measurement was reported by NRL also at ACCF1. 2 Cheek and O'Grady used a quartz crystal microbalance to measure the mass of a deposited palladium surface film operated as a cathode. A critical difficulty with this method is the lack of access to the high loading region due to buoyancy effects associated with the presence of internal D 2 filled voids and surface attached D 2 bubbles at current densities sufficient to produce high loading. This method is also affected by roughening and spallation of the Pd film from the quartz support at high loading and has seldom been used. Dilatometry. A number of people but notably Storms 10 took advantage of the lattice expansion that occurs when hydrogen isotopes occupy the octahedral interstitial sites in the fee Pd lattice. Either linear extension or volumetric expansion measurements can be used to estimate the extent of hydrogen isotope absorption provided this is wholly interstitial. A very important outcome of the extensive work by Storms using the technique was that a significant fraction of the hydrogen or deuterium atoms absorbed by palladium recombine in closed voids within the metal causing compressive stress and volume expansion greater than that attributable to the change in lattice parameter. Storms called this parameter "free volume". Electrodes with a large fraction of free volume tend to load poorly and to not produce excess heat. 10 Oxygen displacement in closed cells. The equations that govern the cathodic absorption of H (or D) in thermodynamically closed cells can be written for 2.1 2.0

•?

f

H D

1.9

\

\

/

1.8 1.7

CD

' '%

V

1.6

\ \

V_ \

CD

o 1.5 c CO 1.4 *—> c/j CO 1.3 CD

\

cr 1.2 1.1 1.0

i.

V ! --

0.1 0.2

-r -

r - 1 U .. rn J • i i I ill 111 LiH * "' - _ . 0.3' '"0.4 0.5 0.6 0.7 0.8 0.9 1.0 ^

Mole fraction (H,D)/Pd Figure 1.

Original calibration curves. 1

1.1

395

basic light water electrolytes as: Cathode: H 2 0 + e~ => OH" + H a d s Cathode recombination: Hacis + H a( j s =>• H2 Cathode absorption: Hads =4> H a b s Anode: 2 0 H " => H 2 0 + 2e~ + O a d s

(1) (2a) (2b) (3)

Anode recombination: O a a s + Oads => 0 2

(4)

Molecular recombination: 2H2 + 0 2 => 2H 2 0

(5)

In the absence of reaction (2b) the rates of production and recombination of H2 and 0 2 are stoichiometrically balanced. Hydrogen occluded in the cathode by reaction (2b) is not available to recombine to water on the catalyst surface (5), resulting in a net production of 0 2 gas. This gas can be measured as a pressure increase (at constant volume, V, and temperature, T) or a volume increase (at constant pressure, P, and T). One favored method is simply to displace an inert liquid onto a balance to be weighed. In the presence of an ideally performing catalyst this method is easily employed and relatively reliable. As is true for most of the methods discussed here, it is not capable of distinguishing between interstitial absorption and hydrogen occluded in free volumes within the Pd bulk. This method was widely used by Riley et al., at the National Cold Fusion Institute (NCFI). 11 The data obtained from their studies were used to refine the SRI resistance ratio versus loading curve. V. Hydrogen displacement in closed cells. In general recombination catalysts operate more reliably at gas concentration ratios well away from the stoichiometry point (2:1 H 2 :0 2 ). Method IV also has the disadvantage of making the environing and dissolved gas concentrations oxygen rich, thus lowering the H2 (or D 2 ) partial pressure and reducing the maximum loading. A method was developed at SRI 12 to precharge sealed and thermodynamically closed electrolytic cells with a controlled atmosphere of hydrogen gas. In this situation the net loading that results from Eq. (2b) reduces the moles of H 2 (or D 2 ) in the gas phase. This can be readily measured as a pressure change (at constant T and V) or volume change (at constant T and P). VI. Stripping coulometry. An anodic reaction process involving successively the reverse of reactions (2b) and (1) can be used very accurately to titrate loaded H (or D) from the lattice provided that the surface atom recombination reaction (2a) is avoided. This reaction can be effectively poisoned by electrodepositing heavy metals on the cathode surface. Since this also prevents absorption the co-deposition of metals such as Hg is best done at or near the end of hydrogen loading. A procedure of this type was developed for H and D loading of long thin Pd wires by Celani's group at INFN Frascati. 13 This method was further developed collaboratively by Tripodi at SRI for the purpose of measuring temperature effects on resistance. 14

396

VII. X-ray diffraction. The position of Pd atoms in their sublattice of PdH x or PdDz is a function of the loading, x. Although reasonably well established for PdHa;, particularly for x < 0.85, no reliable information exists for the condition of interest in cold fusion experiments, PdDx for x > 0.85. A collaboration between the groups at the US Naval Research Laboratory (NRL) and ENEA, Frascati in Italy has been established to redress this deficiency.15 As well as the expected increase in lattice parameter with increasing octahedral occupation, the researchers are also interested in pursuing evidence for tetrahedral site occupation, double occupation of octahedral site or new phase formation. VIII. Neutron diffraction: Cold fusion experimenters and theorists are more interested in the positions occupied by deuterons in the PdD x sublattice, as x approaches or exceeds unity, rather than in the relative positions of Pd atoms. In principle this information can be accessed directly in neutron scattering experiments. It is possible than no single experiment is of greater importance to the cold fusion community in the high-loading, heat-producing condition of PdDa;^ x . An attempt to perform an in situ electrolytic loading experiment in collaboration between SRI and Los Alamos National Laboratory, LANL, was unsuccessful for technical reasons in 1994 but further attempts should be considered. As the result of a large number of experiments to correlate loading and resistance ratio at SRI 12 and elsewhere11 made mostly using methods I, IV and V, the curve originally constructed in 1990 and shown as Fig. 1 was refined in 1993. Two versions of this curve were published; 12-14 these are replotted here as Figs. 2 and 3. Figure 3 also took advantage of data originally published by Baranowski et al., in 1990,19 but comprehensively re-analyzed at SRI in 1993. These data were also included in the SRI curve (Fig. 4) that sought to distinguish between successful heat producing cells (labeled in red) and unsuccessful heat producers (green) on the basis of the maximum loading or minimum resistance attained on the right-hand side of the resistance maximum. This curve provided important confirmation of the need to measure loading and the utility of the resistance ratio method. Absent a complete set of calibration data covering the entire range of D-Pd composition the curves in Figs. 2 and 3 were constructed according to the following rules: 1. Linear multiple relationship between the H and D loading curves. 2. The resistance ratio maxima for H and D occur at the same atom fraction. 3. The high loading data for D-Pd conform with minimum standard deviation to the 1990 data of Baranowski et al.19 A comprehensive review of the literature was undertaken to estimate better the position of the H-Pd resistance-loading curve and the results published as in Ref. 20. In addition a more extensive analysis was made of the Baranowski data for D-Pd published in Ref. 19. Based on these analyses and applying rules 1-3 listed above,

397

we have constructed new curves for H-Pd and D-Pd in the high loading region. These curves are presented in Fig. 5. Also plotted in Fig. 5 are the equilibrium gas pressures needed to achieve the specified atomic ratios. The square points in Fig. 5 taken from the Baranowski data 19 exhibit an interesting kink or second order transition at D/Pd > 1.02. The origin of this feature is not known although it appears not to be present for H in the same region of composition. Another attempt to specify the resistance/loading functions for palladium made by Zhang et al.21 resulted in the curves replotted in Fig. 6. While the difference between the Zhang and SRI curves is subtle we believe that Zhang's curves fall outside the uncertainty in the literature data for H 20 and the precision of the Baranowski data for D. 19 It is also notable, although not diagnostic, that Zhang's curves for H and D exhibit maxima at different atomic ratios (cf. rule "2"above). A test of accuracy of the H-Pd curve was made directly by Tripodi and the present authors. 22 The coulometric stripping method described in method V above was used to directly correlate resistance and loading of two sections of fine Pd wire cathodes (diameter 50 ^m, length 10 cm) loaded to H/Pd « 0.98, sealed by co-

0.00

Figure 2.

0.20

0.40 0.60 H(D)/Pd

0.80

Second calibration 1993, Version 1.

1.00

398

deposition of Hg 12,13 and then stripped at very small anodic current density. The results shown in Fig. 7 do not provide a strong basis to distinguish between the Zhang and SRI curves. The knee at H/Pd ~0.57 is interesting and appears to be a real feature. Because of this knee, Zhang's attempt to accommodate data at loading H/Pd < 0.6 (not attempted by SRI) appears to have moved their predicted resistance maximum to lower loading and higher maximum value. 3. Discussion The various attempts to characterize the position of the resistance versus loading curves for H-Pd and D-Pd can be summarized in terms of a few critical constants: 1. The maximum resistance value of the resistance ratio, -R/_Romax2. The value of the atomic ratio at the point of maximum resistance, x m a x 3. The value of the resistance ratio at a loading x = 1, R/Ro x=\. Table 1 shows how values of these constants have changed in 16 years of experimentation and analysis.

RIR

°

1 +3x-15.13x 2 +44.16x 3 -49.12x 4 +17.58x 5

0.00 0.10 0.20 0.300.400.50 0.600.700.80 0.901.00 H (D)/Pd Atomic ratio Figure 3.

Improved calibration 1993.

399

FURo T1-2.0HFI-3

2

Figure 4. Showing the correlation between maximum loading measured by resistance ratio and successful (red) and unsuccessful (green) heat production in Fleischmann-Pons electrolysis experiments performed at SRI.

Some changes have occurred in the curve for H-Pd; a small increase in the resistance maximum and a significant increase in the position of the maximum for the SRI curve but not for Zhang's. Of far more significance to cold fusion workers

R/flO (PdB*>fl/f?o (PdB*> R/R0 (PdH^ PH2 (atrffc)-PD2 (atm.) T 40000

0.7

0.75

0.8

0.85 0.9 0.95 Atomic ratio

1.05

Figure 5. Improved calibration curves based on new data, reanalysis of H-Pd literature 2 0 and Baranowski data for D-Pd (square points 1 9 ).

400 -*--R:R, iP&Hx) —Zhang & Zhang H —Stnp Upper —Strip Lower

1

o.2o

0.30

0.40

0.50

0.60

0.70

0.80

0.90

1.00

Atomic ratio Figure 6.

SRI 2 0 and Zhang et al.21 curves and Tripodi et al.22 stripping data.

the value of the resistance at H/Pd = 1, R/RQ X=I, has dropped from ~1.35 to 1.067 for the SRI curve and below unity to 0.926 for Zhang's curve. Turning attention to the D-Pd system the expected value of maximum resistance has changed very little with reanalysis. The position of maximum resistance in D Pd has increased following that of H-Pd for the SRI curve using rule 2. The increase in this parameter for Zhang's curve is even larger. Of much greater significance in cold fusion studies the expected resistance at D/Pd = 1 has dropped from 1.5 in 1990-1994 to 1.43 in 1996 to 1.245 in the SRI curve circa 1998. The value for Zhang calibration published in 2002 is even lower at 1.222. The combined effect of moving the position of the resistance maximum to higher loading, and the expected resistance at D/Pd = 1 to lower resistance value results in a much steeper calibration curve on the right-hand side of the resistance maximum. As a consequence, when comparing the old calibration to the new, resistance ratio values interpreted as loadings in the region of interest for Fleischmann-Pons effect studies (D/Pd > 0.85) have consistently overestimated the interstitial deuterium Table 1.

Changes in loading parameters

1990

1994

H/Pd fi/fio™ xmax R/Ro x=i

Ref. 1 1.79 0.725 1-34

Refs.16-18 1.78 0.729 1.36

D/Pd R/BomaI xmax R/Ra x=1

2.00 0.725 1.50

2.00 0.724 1.50

1996

Ref. 19 2.00 0.724 1.43

1998

2002

Refs. 20,22 1.809 0.760 1.067

Ref. 21 1.820 0.732 0.926

This paper 1.96 0.760 1.245

2.01 0.772 1.222

401

content of the palladium. This systematic error is not large, but it may have important physical significance. Table 2 recalculates the maximum loading based on the minimum resistance ratio measured on the right-hand side of the resistance maximum for five historic heat producing cells operated at SRI. 12 What had previously been interpreted as maximum average loadings at or above unity when evaluated with the new SRI calibration curve result in loadings D/Pd approaching unity. Only P l a indicates a D / P d m a x > 1. This cell was operated at 4°C where the calibration curve is likely to be different. In any case, the calculated loading maximum is not outside the estimated 1% uncertainty. Thus, in experiments conducted at SRI, we have no evidence that palladium cathodes can be loaded by electrolysis to atomic ratios greater than unity. At this point it is worth discussing what is the relevance of a resistance ratio measurement of deuterium loading. The evidence is overwhelming that deuterium does not load homogeneously into polycrystalline palladium. Observations made of Pd cathode surfaces reveal that different crystalline facets load and expand at different rates, and the grain boundaries absorb (and release) D at very different rates from the bulk. Electronic transitions observed at low temperatures in highly loaded thin wires clearly indicate the presence of small zones of very differently (presumably higher) loaded material. 14 Hot spots observed either in situ with thermal imaging or retrospectively by autoradiography, 1 and local melting or isotopic effects, all suggest that the Fleischmann-Pons effect, whatever its cause, occurs heterogeneously throughout the bulk or on the surface. Indeed, since deuterium flux appears with equal footing to loading in quantifying excess heat power,23 the existence of heterogeneity (or time variability) in surface chemical potential appears to be crucial in producing excess heat in electrolytic D-Pd experiments. Given these observations and the occasional solid report of excess heat at low loading one might question the deterministic power of four terminal macroresistance ratio measurements that necessarily access a volume averaged electrode property. What might be important is simply that this property is monotonically related to the chemical potential of deuterium in the sample. The various mechanisms involved in attempts to explain the Fleischmann-Pons heat effect, the existence of a new phase or band structure, atom or ion pairing, lattice deformation to produce occupiable host sites, all depend critically on the chemical potential of absorbed Table 2.

Corrected maximum loading values.

Cell

R/R0

Pla P17 P22 P19 P12

1.20 1.27 1.30 1.45 1.55

min

D / P d old

D / P d adjusted

1.06 1.04 1.03 0.99 0.97

1.01 1.00 0.99 0.96 0.94

402

deuterium. Furthermore, the very high permeability of palladium by deuterium ensures that adjacent regions of differing chemical potential will have only transient existence or will be associated with high deuterium fluxes, a known beneficial condition. It is therefore suggested that the important lattice characteristic measured by the resistance ration is deuterium activity, not loading, in the metal. Because of the very high diffusivity of D in Pd the average D activity very closely reflects the activity everywhere in the cathode and on it's surface. We therefore expect the bulk, average resistance ratio to be reflected in excess heat rates even if the site of heat generating activity is a special environment of, on or at the surface. 4. Conclusions and Recommendations The calibration of the resistance ratio versus loading curve for deuterium in palladium originally published in 1990 and refined between 1992 and 1996 is in error. A re-evaluation of this curve based on literature and new experimental data indicates that the D/Pd loading estimates in the region of interest for electrolytic Fleischmann-Pons experiments should be revised downward. With this downward revision, it is possible that electrolytic experiments performed at ambient temperature and pressure have not achieved volume averaged D/Pd electrolytic loadings greater than unity, even in successful heat producing experiments. In order to compare loadings obtained in different experimental setups or different laboratories, it is preferable to report data as resistance ratio values, R/Ro, on the right-hand side of the resistance maximum. In this way consideration of the shape of the resistance-loading calibration curve is avoided and any improvements in this function can be easily accommodated. The issue of temperature of measurement significantly complicates the simple interpretation of a resistance ratio as an average loading, particularly in the region of interest to those studying the Fleischmann-Pons effect. The calibration curves discussed extensively here apply strictly only when R and RQ both are measured at 298 K. The temperature coefficient of resistance is known as a function of loading, and a simple mathematical correction is often made. However, this coefficient is a strong function of composition 14 and is largely unknown for PdD-j as x approaches and exceeds unity. Thus it is difficult to apply the needed temperature corrections accurately. For this reason it would be helpful for future workers to express clearly what, if any, temperature corrections have been made to R and RQ, and state the temperatures for which both values were measured. References 1. M. McKubre et al., Calorimetry and electrochemistry of the D-Pd system, in Proc. First Annual Cold Fusion Conference, Salt Lake City, F. Will, Ed. (1990). 2. G. Cheek and W. O'Grady, Quartz crystal microbalance study of Pd/H interactions, ibid. 3. G. Preparata, Theoretical ideas on cold fusion, ibid. 4. P. Hagelstein, Status of coherent fusion theory, ibid.

403

5. S. Chubb and T. Chubb, Quantum mechanics of 'cold' and 'not-so-cold' fusion, ibid. 6. J. Schwinger, Nuclear energy in an atomic lattice, ibid. 7. D. Macdonald, M. McKubre, A. Scott, and P. Wentrcek, Continuous in situ method for the measurement of dissolved hydrogen, I&EC Fundamentals 20, 290 (1981). 8. B. Baranowski and R. Wisniewski, Phys., Stat. Sol. p. 539 (1969). 9. F. A. Lewis, The Palladium-Hydrogen System (Academic Press, New York, 1967). 10. E. Storms, Fusion Technol. 29, 261 (1996). 11. A. M. Riley et al., Measurement of absorption of deuterium in palladium during electrolysis of heavy water, NCFI Final Report II, 2-123 (1991). 12. McKubre et al, EPRI TR-104195 (1993). 13. A. Spallone, F. Celani, P. Marini, and V. Di Stefano, New electrolytic procedure for the obtainment of very high H/Pd loading ratios, Proc. ICCF8 (1990), p. 191. 14. P. Tripodi, M. McKubre, and F. Tanzella, Temperature coefficient of resistivity at composition approaching PdH, Phys. Lett. A (2000). 15. G. Hubler and V. Violante, Personal communication (2005). 16. McKubre et al., Loading, calorimetric and nuclear investigations of the D-Pd system, Proc. ICCF4 (1993), p. 5-1. 17. McKubre et al., Isothermal flow calorimetric investigations of the D/Pd and h/pd systems, J. Electroanal. Chem. 368, 55 (1994). 18. McKubre et al., Chemical and metallurgical issues in the loading of D into Pd, Proc. International Symposium on Cold Fusion and Advanced Energy Sources, Minsk (1994). 19. B. Baranowski, S. Filipek, M. Szustakowski, J. Farny, and W. Wornya, J. Less Common Met. 158, 347 (1990). 20. S. Crouch-Baker, M. McKubre, and F. Tanzella, Variation of resistance with composition on the /3-phase of the H-Pd system at 298 K, Z. Fur Phys. Chemie. 204, 247 (1998). 21. W.-S. Zhang, Z-F Zhang, and Z-L Zhang, J. Electroanal. Chem. 528, 1 (2002); 571, 81 (2004). 22. P. Tripodi, F. Tanzella, and M. McKubre, Unpublished results (1999). 23. McKubre et al, Concerning reproducibility of excess power, Proc. ICCF5 (1995), p. 17.

M E A S U R E M E N T S OF T H E T E M P E R A T U R E COEFFICIENT OF ELECTRIC RESISTIVITY OF H Y D R O G E N O V E R L O A D E D Pd*

ANTONIO SPALLONE AND FRANCESCO CELANI INFN-LNF,

Via Enrico Fermi, 00044 Frascati (Rome), Italy E-mail: [email protected]

PAOLO MARINI AND VITTORIO DI STEFANO EURESYS,

Via hero 30, 00129 Rome, Italy

As reported in previous papers, we performed many electrolytic loading tests using thin P d wires, achieving loading ratios of H / P d > 0.95 ( H / P d over-loading). In particular, we defined a reproducible "loading protocol" suitable for achieving such an over-loading level, based on the use of very diluted acid electrolytic solutions (with additions of tenths of micro-moles of Ca or Sr or Li cations and some hundred nano-moles of Hg ions) and operating with electrolytic current cycles from a few mA up to one hundred mA. By observing the d a y / n i g h t cyclic fluctuations of electrical resistance, as a function of the corresponding t e m p e r a t u r e variations, of stable, long term, H / P d loadings we were able to calculate the t e m p e r a t u r e coefficient of resistivity (Kg) of the P d - H system at very high H / P d loadings. Many years ago (in 1998), we reported an unexpected value showing t h a t the Kg parameter values increase when H / P d exceeds 0.75 (i.e. after t h a t R/RQ goes beyond the 1.8 peak value, i.e. to the right side of the R/Ro/K/Pd curve). This fact was confirmed by the ISR-Stanford Group (McKubre and Tripodi) and Pirelli-Research Group (Gamberale and Garbelli). In this paper we show several measurements of Kg at different overloading values of H / P d u p to = 1 (corresponding at R/RQ = 1.12) where Kg=(13 ± 1 ) x 10~ 3 K""1, i.e. more t h a n six times higher t h a n the minimum value achieved at the R/RQ = 1.8 peak value. This result can corroborate the hypothesis t h a t a new P d - H phase (full /3-phase or the beginning of j3 + 7 phase) could occur after the H / P d = 0.75 loading ratio (at the end of a + (5 phase), as claimed by many authors as the necessary condition for excess (anomalous) heat from P d - D system (at D / P d > 1).

*This work is supported by INFN-LNF, Frascati, Italy. 404

405

1. Historical Background 1.1. H/Pd

Loading

Measurements

It is common opinion that to observe heat in excess from Pd-D system it is necessary to obtain very high values (>0.95) of D/Pd atomic ratio. 1 _ 3 Starting from 1998 we decided to perform systematic tests in order to achieve very high H/Pd loading ratio using very diluted electrolytes and thin (50 or 100 /im in diameter) Pd wires as cathodes. 4 Different electrolytic solutions have been tested by adding to the acid solution very low amounts of Ca, Sr, Li and Hg ions. In this way high H/Pd loading ratios have been achieved with a satisfactory grade of reproducibility. Several loading procedures have been performed in a wide range of electrolysis current (from a few mA up to one hundred mA) and at different Hg ion concentrations. The obtained results allowed for the definition of a loading protocol capable to insure very high H/Pd over-loading. Stable R/RQ < 1.2 values (corresponding to H/Pd ratios >0.97) can be currently achieved with an extremely low electrolytic power supply (10 V; 5 mA). 5 This procedure is based on the increase of the cathodic over-voltage (which is known to be the main controlling parameter of the H(D)-Pd loading) obtained by modifying the nature of the cathodic surface (i.e. by inducing the formation of a very thin layer of an alkaline-earth carbonate on its surface).

1.2. Temperature

Coefficient

of Resistance

Trend

The temperature coefficient of electric resistivity (Kg) of a Pd-H sample is a wellknown curve in the literature (Kg is known to decrease from 4.1 to 1.8 m K - 1 with H/Pd increase from 0 to 0.7). 6 ' 7 During 1998, after the achievement of a very high and stable H/Pd loading (=0.95), we performed a preliminary measurement of Kg resulting in a value of (3.2 ± 0.2) x 10~ 3 K" 1 within a temperature range from 77 K up to 373 K. For the first time in the literature this value showed that at values of H/Pd higher than 0.7, Kg increases.8'9 Further, this fact was confirmed by the ISR-Stanford Group 10 and Pirelli-Research Group. 11

2. Temperature Coefficient Measure 2.1. Experimental

Setup

In an electrolytic cell (solution of one liter of H 2 0 + HC1 at 10~ 4 mol) the electrodes have been located in the form of two parallel wires, of length 25 and 6.5 cm apart from each other (the Pd cathode of diameter 50 /im, the Pt anode of diameter 0.5 mm); tenths of micro-moles of Sr and hundreds of nano-moles of Hg have been added to the solution. A junction for a pick up of the voltage divided the Pd cathode in two equal segments (named: "up" and "down").

406

2.2. Experimental

Data and Fit

After applying the procedure to reach H/Pd overloading (OFF/ON current cycles, as shown in Fig. 1), if the loaded sample is found stable, we proceed with the recording of the R/Ro variations following the day/night cyclic temperature variations. The measurement campaign may last for several day/night cycles. To complete the test, Pd-H wire is de-loaded either by using anodic current or by simply turning the current off for many hours (as reported in Fig. 1) and observing the phase transition at R/R0= 1.7 (H/Pd = 0.6).

1.8 1.6 1.4 1.2

1

Time (s) Figure 1.

R/Ro

3

data are meanly stable for a enough long time (from 30,000 to 90,000 s range

Generally, as in the latter case, it is possible to check the R/Ro curve tracing back to the peak value (R/Ro = 1-78, H/Pd = 0.75) and returning to the initial value of R/Ro = 1. By considering the data in the range where the loading is stable, it is possible to record the dependence of the wire resistance on the wire temperature (homogenous with the cell temperature) and once the linearity of these data is confirmed (Fig. 2), we can make a fit to calculate the Kg coefficient according the relation (A.l) reported in the Appendix. To be considered valid to our purpose, resistance data have to be repetitive after each temperature cycle. In Fig. 1, it is reported that the load/deload procedure (V-I ON/OFF) up to R/RQ = 1.1 and R/Ro fluctuation with temperature cycles ("measure"); evidence of the /3-transition occurs during the de-loading procedure.

407

1.18 y=08tU)0ni13AP-0PS4

1.17

- I ' «,=-!?. 8x 10 *t C )

1.16 r, 1.15

^

1.14 1.13 1.12 1.11 20

Figure 2.

2.3.

21 22 23 24 25 Temperature-cell (°C)

26

Partial data of a full temperature cycle (40,000-60,000 s) well fitted by a simple line.

Results

Out of several hundred tests, only a few tens have shown a loading stability suitable for the calculation of the Kg parameter. We report in Table 1 some values corresponding to different values of Pd loading. In this table, measured values of R/Ro are reported for each of the two wire sectors "up" and "down" (generally showing similar loading values); tests ranged along a period of a year during which different wires, electrolytes and procedures were used. Table 1. Values of Kg as resulting from several tests performed at stable loading conditions and ratios (ref. room temperature at 20°C). H/Pd R/Ro ± 0 . 1 0.00 0.85 0.88-0.90 0.91 0.92-0.93 0.96-0.98 0.97-0.98 0.99-0.995

Down

Up

1.0 1.75 1.58 1.52 1.44 1.19 1.18 1.10

Kg

1

(mK- )

4.1 ± 2.8 ± 7.2 ± Ri7± S8.3 ± 9.9 ± 10.7 ± =13 ±

0.1 0.3 1 1.5 1 0.5 0.5 1.5

R/Ro ± 0 . 1 1.0 1.75 1.61 1.52 1.46 1.24 1.21 1.13

KgimK-1) 4.1 ± 0 . 1 a 2.6 ± 0.3 b 6.7 ± 0.5 C C RJ7 ± 1.5 =•8.4 ± l c 9.6 ± 0.5 C 10.6 ± 0.5C 12.8 ± 0.5 C

(a) The first value is in agreement with the expected value for Kg = 4 . 1 . (b) At the R/Ro peak value the thermal coefficient is a little higher (30%) than the one reported in the literature (Kg = 2.0). (c) All the values, beyond the R/Ro peak, the thermal coefficient shows rapid increase.

408

H/Pd values reported in the table are taken from literature data up to R/RQ peak value and after this point we refer to Mc Kubre experimental and theoretical data, as previously reported. 12 In Fig. 3, we report known literature data ("+" points below the R/RQ peak) in addition to the new experimental data ("0" points beyond the R/RQ peak) which show the progressive increase of Kg as the H/Pd value increases (overloading); the arrows show the trend of Kg with increasing loading ratio. 14

14

•i

12 + r

1 0

CO

12 10 - ^

%

3 8 3

Q

y

<5 v**

6

\

CA

,!*«!*'«•!..

. CD

3 § c

*** '.B-l,

.•

4

n>

3 2

- i — i . - L - i i ,...., I. .i

1

i.....J..t-1-j-U-,

1.11.21.31.41.51.61.71.8

Figure 3. P d - H temperature coefficient vs normalized resistance of the wire. Experimental data are reported in addition to literature data.

Similarly, in Fig. 4 we report data from the literature and the experiments; they show clearly the rapid progressive increase of Kg at H/Pd overloading. 3. Discussion 3.1. Phase

Hypothesis

From the literature, 2,3 ' 6 it is known that at room temperature the system Pd-Hx occurs in different phase conditions (a-phase at H/Pd = 0-0.1 and a + ft phase at H/Pd = 0.1-0.6). Because of the change of dimension occurring for R/Ro at the peak value of 1.8 when H/Pd is ranging from 0.7 to 0.8,1 it is possible to suppose a phase transition is taking place as it is pointed by an arrow in Fig. 1 at R/RQ = 1.7. At this R/RQ peak we hypothesize a new phase, named "/3 + 7" phase. If, at high H/Pd loading, this R/RQ peak is surpassed, we can assume that a peculiar 7-phase

409

^

I

-16

$

1

-

rn c —*: CD

Figure 4. P d - H temperature coefficient vs normalized H / P d loading. McKubre tables, are reported in addition to literature data.

Estimated data, from

occurs in correlation with the change of slope of the Kg vs temperature curve (Fig. 4) so that this new phase is peculiar of H/Pd high loadings.

3.2.

Conclusion

In conclusion, we stress the following points: • We are able to achieve H/Pd = 1 staying stable for a long time. • We can calculate Thermal Coefficient of Resistance at high Pd-H loadings. • At high loadings as the R/RQ strongly decreases, the thermal coefficient of electrical resistivity strongly increases. • We can conjecture a new important phase occurring at high loadings. Because all tests were performed using Hydrogen (i.e. light water) instead of deuterium (i.e. heavy water) we do not expect any anomalous heat in excess produced by the wire (i.e. Fleishmann and Pons effect), in fact we never detect thermal anomalies using light water in electrolysis solution. If such an anomaly occurred, wire temperature increasing (in respect to solution temperature) could alter the thermal coefficient measurement, but just this change of expected value could be an indication of anomalous excess heat.

410

Acknowledgments We are indebted to Eng. Alfredo Mancini for his precious support. We are grateful to Dr. Daniele Garbelli and Dr. Luca Gamberale for their important help and we want to t h a n k Dr. Mike McKubre for his useful suggestions. We like to stress the expertness of Mr. Vincenzo Andreassi, our skill technician. Appendix We used the known formula to calculate Kg: R(x,6)

= R0(x)(l

+ Ke{x)

9)

(A.l)

where R (in fl) is the electric resistance of the wire (related to a fixed x = H / P d loading ratio) and depending on the wire t e m p e r a t u r e 6 (in Celsius centigrade); RQ is the wire resistance at 0°C of t e m p e r a t u r e . Kg is the t e m p e r a t u r e coefficient of resistance (in ° C _ 1 ) . We consider Kg constant within a large range of temperature; indeed we have checked this constancy (within 5% of variation) from 200 K up to 373 K with a overloaded wire. References 1. M.C.H. McKubre et al., Frontiers of cold fusion, Proc. ICCF3, 1992, Nagoya, Japan (1993), p. 5. 2. B. Baranowski et al, J. Less Common Met. 158, 347 (1990). 3. B. Baranowski and R. Wisniewski, Phys. Stat. Sol. 35, 539 (1969). 4. A. Spallone, F. Celani, P. Marini, and V. Di Stefano, Experimental studies to achieve H/Pd loading ratio close to 1 in thin wires, using different electrolytic solutions, Proceedings of the 9th International Conference on Cold Fusion, "Condensed Matter Nuclear Science" (Edited by Xing Z. Li.), Beijing (China), May 19-24 (2002), pp. 319-322. 5. A. Spallone et al., An overview of experimental studies about H / P d over-loading with thin Pd wires and several different electrolytic solutions, Proceedings of the 11th International Conference on Cold Fusion (Edited by J.P. Biberian), Marseilles (France), Nov. 01-05 (2004). 6. J.C. Barton, F.A. Lewis, and I. Woodward, Trans. Faraday Soc. 59, 1201 (1963). 7. M.C.H. McKubre et at, Galorimetry and electrochemistry in the D / P d systems, Proceedings of the First Annual Conference on Cold Fusion, Salt Lake City, Utah, March 28-31 (1990). 8. P. Marini, A. Spallone etal., XXISecolo Scienza e Tecnologia, AnnoX (1), 34-41 (1999). 9. F.Celani, A. Spallone et al., High hydrogen loading of thin palladium wires through alkaline-earth carbonates' precipitation on the cathodic surface. Evidence of a new phase in the Pd-H system, INFN: LNF-00/006 (P), 6 Marzo 2000, To be published by Physics Letter A. 10. P. Tripodi, M. McKubre et al., Phy.Lett. A 276, 122-126 (2000). 11. L. Gamberale, D. Garbelli, and G. Piana, Measurement of Heat Capacity of PdHx, Proceedings of the 9th International Conference on Cold Fusion, "Condensed Matter Nuclear Science" (Edited by Xing Z.Li), Beijing, China, 19-24 May (2002), pp. 105-108. 12. M.C.H. McKubre (Data reported at the same Conference and Private Communications).

M A G N E T I C I N T E R A C T I O N OF H Y P O T H E T I C A L PARTICLES MOVING B E N E A T H T H E ELECTRODE/ELECTROLYTE INTERFACE TO ELUCIDATE EVOLUTION M E C H A N I S M OF VORTEX A P P E A R E D ON P d SURFACE A F T E R LONG-TERM EVOLUTION OF D E U T E R I U M IN 0.1M LiOD

HIROO NUMATA Tokyo Institute

of Technology, 1-12-1 O-okayama, Meguro-ku, E-mail: [email protected]

Tokyo 152-8552,

Japan

MASANOBU BAN Tokyo Metropolitan

Industrial

Technology Research Institute, Tokyo 115-8586, Japan

3-13-10

Nisigaoka

Kita-ku,

Long-term electrolysis for well-annealed thick Pd rod (9.0 mm <j>) in 0.1M LiOD was performed. Microscopic observation of a postelectrolysis Pd surface showed that long-term electrolysis did not result in any cracking but surface voids, two long faults, voids arranged in a straight line and peculiar surface traces: vortex. N-cycle model was developed to explain the cold fusion reaction and the related phenomena resulting in improved reproducibility of cold fusion experiments. An important process in that model is the motion of deuterium from a vessel to other ones, which might occur the observed vortex patterns on a postelectrolysis Pd surface. However, there has been remained unsolved yet a phenomenological explanation for the process of the vortex formation. The lattice gas cellular automata method was utilized for simulating a simple 2D flow with the boundary conditions incorporating the motion of the coincidental flow of the hypothetical particles. The vortex pattern was obtained behind the obstacle, though the axis appeared along the electrode surface. However, by comparing the vortex patterns obtained by the Lattice gas cellular automata method simulation and a postelectrolysis Pd surface the vortex with the leaned axis along the electrode can only be acceptable to describe the motion of the hypothetical particles. The vortex of the massive electron appeared to be modified by Lorenz force during traveling the interface assuming a 2D circular motion.

1. Introduction Ever since the announcement of Fleischmann and Pons, and Jones et al. of the generation of neutron and thermal energy accompanied with electrolysis on Pd in 0.1M LiOD, there still has been remaining the questions about the mechanism of the cold fusion reaction. What kind of phenomenon occurs when deuterium is absorbed in Pd metal by electrolysis is unknown, it is believed, is one of the reasons never expelled from the above doubt. Numata 1 , 2 ' 4 proposed a nuclear reaction cycle model (thereafter shortened to N-cycle model illustrated in Fig. 3) to explain the 411

412

miscellaneous phenomena accompanied with the cold fusion reaction as a multiple cyclic process, similar to a natural phenomenon. An important process in that model is the motion of the hypothetical particles from a vessel to other ones and/or to surface. Microscopic observation of a postelectrolysis Pd surface after long-term electrolysis for well annealed thick Pd rod in O.IM LiOD showed surface voids, two long faults, voids arranged in a straight line and peculiar surface traces: vortex. 4,5 Lattice gas cellular automata method (LGCA) numerical simulation of the motion of the hypothetical particles having large kinetic energy accounted for the vortex pattern appeared on a Pd electrode surface.6 Thus, such anomalous phenomenon was proved to really occur during the cold fusion experiments, however, there has been remained unsolved yet the motion of the hypothetical particles between the electrified and magnetized interfaces. Recently, Lewis7 comprehensively discussed ball lightning experiments (also EV markings in the same subject) showing the various holes, markings and tunnels including tornado associated with cold fusion and transmutation effects. The morphology of tornado looks like the vortex pattern well. Anomalous surface morphology like volcano was first reported by Oomori et al. on Au 8 and Toriyabe et al. on Pd 9 in light water electrical discharge experiments. These various anomalous traces, markings, etc. could be explained with magnetohydro dynamics and quantum mechanical consideration. Our research endeavors are rooted to give an atomistic understanding of processes that occur the vortex on a Pd electrode surface after long-term electrolysis in O.IM LiOD. In this paper the role of magnetic interaction with the emitted particles at the electrode/electrolyte interface will be discussed premising the motion of the hypothetical particles mass like vortex in the atmosphere. The experimental details of the appeared vortex and the results of fluid dynamics simulation and finite element method are described to elucidate the vortex formation mechanism at the interface. 2. Experimental 2.1. Long-Term Evolution of Deuterium Electrode in O.IM LiOD

on Thick Rod Pd

Cold fusion experiments at ambient temperatures have been conducted by electrolysis of heavy water on a Pd electrode or the other stable metals, e.g., Ni, Ti, and Au electrodes. In Fig. 1, the electrolysis equipment, especially the geometrical shape and arrangement of the electrode, the counter electrode and an electrolyte are shown, and the measurement systems with respect to excess heat, neutron emission, and an isothermal water bath are not drawn. Using a potentiostat (or current supply) a constant cathodic current was applied to a Pd electrode on which an evolution of deuterium gas was occurred. By continuing a state where deuterium is strongly absorbed in a Pd electrode, heat generation or emissions of neutrons or charged particles is observed. We successfully performed non-intermittent electrolysis for two and ca. 6 months with two experimental runs, referred to Exp. 1 and Exp. 2, respectively. The characteristics of the experimental apparatus and

413

1. Pd rod cathode 2. Anode 3.0.1M LiOD electrolyte 4. Double jacketed transparent quartz cell 5. Addition tube 6. Thermocouple 7. Guide for Deuterium gas 8. Guide for Oxygen gas 9. Circulating water inlet 10. Circulating water outlet 11 - Current supply

Figure 1. Schematic diagram of electrolytic cell for deuterium absorption on a Pd electrode in 0.1M LiOD.

procedures are: (1) cast rod Pd electrode, (2) thicker rod Pd electrodes (rods with 9 and 21 mm diameters 3,4 ), (3) preparatory gas phase absorption of D 2 (D/Pd 0.36), (4) increase in electrolysis current density in a form of stepwise, and (5) temperature cycling. The experimental runs were conducted twice in 0.1M LiOD by using the rod Pd electrodes with a diameter of 9 mm referred to Exp. I, 5 and a diameter of 21mm referred to Exp. 2. 3 , 4 The surface pretreatment and electrolysis conditions are shown in Table 1 and the results of neutron measurement are described elsewhere. 3,4 3. Results and Discussion Description with respect to microscopic observation of a postelectrolysis Pd surface is made with the result of Exp. 1. Figure 2 shows an optical micrograph of the transverse cross-sectional area (shown as rectangular in the left), where the sample was taken from the apex of the electrode, embedded in epoxy resin and lightly etched. Figure 2, on the right, shows a peculiar grain structure, quadrified by two straight grain boundaries. In metallographic aspect the specimen as a whole is consisted of columnar crystals: long prisms, which is supposed to be grown longitudinally along the electrode center (also see Fig. 4). However, this microstructure of the Pd Table 1. Run no.

Current (mAcm

First

0.05-40 40-500 40 40 40

Second Third Fourth

2

)

Experimental conditions of Exp. 1 Pretreatment Cast, 800°C anneal (lO-* 7 torr) Acid treatment Polishing, acid treatment, evacuation, and D2 gas charge Evacuation, polishing, and acid treatment Evacuation, polishing, and acid treatment

414

Gold plated titanium wire I Gold electric leading wire Cross sectional area of electrode

Teflon sheath

9<|>Pd rod

Epoxy resin

*

TC

Figure 2. electrode.

Schematic of Pd electrode and optical micrograph of cross sectional surface area of

electrode is unexpected, since the temperature of the electrode and that out side of the counter electrode showed no significant change corresponding to heat bursts. Hence, this is well acceptable, only when the small heat evolution in the interior of the electrode lasted long time so as to promote abnormal grain growth. Coupland et a/.10 found the recrystalline grain near the area of electrical connection. Thus, during emission of neutron, the heat evolution in the interior occurred slowly showing the symmetrical crystal structure. Since the above result obtained by microscopic observation is not the in situ measuremnt, it is impossible to give an answer to the matter when such a microscopic structure appeared or to the time correlation with neutron count rate. However, it was possible to estimate such problems by an analogy with a natural phenomenon, as shown below.

•Reaction vessel: many regions surrounded by stained tough zone

Nuclear reaction cycle

Figure 3.

Schematic of a nuclear reaction cycle model.

415

3.1. Nuclear

Reaction

Cycle

Model

So far, endeavors have been exerted on understanding the individual phenomenon accompanied with the cold fusion reaction, which is a complicated phenomenon as a whole. Under such an idea, by considering phenomena as an energy engine, N-cycle model 1 - 3 was proposed from a point of view of its continuous operation (four reciprocating cycle). It consists of four sequential processes: intaking and compression-triggering-reaction-scavenging, taking into account of the correspondence to long-term electrolysis of a thick rod Pd (Fig. 3). The following two key points are beneficially realized: (1) enhanced reproducibility of the experiments resides in continuation of the cycle, (2) on systematic consideration the hindered factors might come to the surface. Let the correspondence be examined with the model in question to the phenomena of the experiment. In the absorption and compression processes of the reactants of the reaction (see Fig. 3), a barrier layer of deuterium migration by compression stress (also corresponds to the B side of the single-side electrolysis referred to the report 1 ' 2 ) is formed as absorption in progress, resulting in formation of a vessel composed of the interior and blanket as the barrier layer. In the compression process, the interior appears to make expansion owing to the continued absorption, i.e., a part of the generated deuterium is contributed to further slow absorption. However the compression pressure of the blanket brings a kind of enhanced pinch effect resulting in an increase of the internal pressure (in otherwise an increase in stress). In the reaction process a reaction should be caused by an external trigger that is applied to the inside (i.e., injection of high energy particles from the outside) or by an internal trigger. As an actual internal trigger, Cases I and II (also shown in the report 4 - 1 1 ) can be considered depending on a manner whether the role of the fault formation should be regarded as the final step of the reaction process or a reaction is induced by allowing the fault formation to provide the blanket with a path to expedite further absorption. 11 Very many holes concentrated on both the sides of the fault found in the experiment 4 were discharge ports of the reaction products in the process of scavenging. At this stage, discharge is made with the products of the reaction together with unreacting deuterium. 11 ' 12 In case of the internal trigger I, emission of the neutrons and charged particles at first occurs as a precursor phenomenon of the cold fusion reaction similar to an earthquake as listed in Refs. 1 and 2. Second, fault is formed simultaneously with reaction. In case of the internal trigger II, vessel is formed in the compression process, although the D/Pd ratio could be insufficient to the reaction. Therefore, fault is formed through a barrier layer (formation of this layer makes it for either absorption or desorption to occur), which allows the absorption to take an easy route. Thus, it is inferred that the D/Pd ratio is raised, resulting in occurrence of the cold fusion reaction. The resulting ca. 6% expansion confirmed during the first run (also see the left of Fig. 4 ) 1 - 4 suggests the occurrence of considerable internal pressure increase corresponding to the absorption/compression process of N-cycle model. Apart from the identification of the reaction vessels and emitted particles, the subsequent outflow

416

Top view of interface //~

~ N \ Simulate flow

<*0 H

Electrode

Electrolyte Obstacle

I 6% expansion 1 Absorption of deuterium

Figure 4.

Perspective view: outflow of hypothetical particle mass

Absorption of deuterium and resultant outflow of hypothetical particles mass.

of the hypothetical particles mass (once these particles were denned as charged particles, deuterium or reaction products) might occur toward 360° radial direction as the scavenger process of N-cycle model (also see the right of Fig. 4). Such motions of the particles mass might be realized from the geometry of the reaction vessel formed during the absorption/compression process shown in the left. That is, in a long prism crystal absorbed reaction products or deuterium under high pressure coincidently spout out with sufficient energy where the motion of the flows are expressed as 'simulate flow' vectors normal to the electrode interface as shown in the right. Importantly all the flows synchronize with the occurrence of the reactions. It is known that nuclear reaction instantaneously occurs during which the hypothetical particles surrounding the site coincidently gain momentum converted by the energy of force evolved multiplied by time in an adiabatic sense. In addition obstacles might be embedded under beneath the surface due to inhomogeneity. Thus, N-cycle model predicts that the flows occur coincidently through the electrode/electrolyte interface (formerly shown in Fig. 3 as the motion of reaction products and deuterium to neighboring vessels and/or surface of the electrode), however, phenomenological evidence has not yet been shown, which is substantiated next by a postelectrolysis Pd surface observation and numerical simulation of the fluid flow. 3.2. Vortex Appeared

on Pd Electrode

Surface

Figure 5 shows a significant morphology of a thick rod Pd electrode in 0.1M LiOD observed on the surface after long-term electrolysis. 1-4 This is not the substance adhered on the surface, but is a material on which the pattern was deeply impressed in a shape of a ditch. In Fig. 5(b), vortex is shown as masses of the high energy particles discharged taking a locus of vortex on the electrode surface. It is imagined that due to an electro-magnetic interaction with a magnetic field (i.e., a magnetic field generated by a current) attenuating from the electrode surface toward the bulk of the electrolyte, the pattern of the corneals (depicted in dots) different from each

417

other in their sizes were left on the surface. Thus, the locus of the vortex observed on the Pd surface after long-term electrolysis in 0.1M LiOD is considered to be an occurrence of energetic particles emission. At this stage the mechanism of such vortex evolution stayed in the guess.

Figure 5. Vortex appeared on Pd electrode surface after long-term electrolysis in 0.1M LiOD, (a) Duplicate of SEM picture, (b) Vortex evolved normal to electrode surface. Dashed line shows locus of vortex.

3.3. Lattice

Gas Cellular Automata

Method

Lattice gas cellular automata method is utilized for simulating the Poiseuille flow with the boundary condition incorporating the motion of the hypothetical particles fluid. An advanced LGCA simulation has been performed adopting the advanced Inflow and Outflow boundaries under particle generation and disappearance conditions. 13 This simulation showed that the flow creates a vortex behind a flat plate. In this case the flat plate is considered as an obstacle for the first approximation. Although the coarser simulation is unable to fully describe the phenomenon, it is shown that a vortex exists in the downstream as schematically re-drawn in Fig. 6. The LGCA simulation result showed that the vortex axis appeared along the electrode surface due to the coincidental flow of the hypothetical particles (shown as arrows in Fig. 6). However, by comparing the vortex patterns obtained by LGCA simulation and a post electrolysis Pd surface observation the vortex with the leaned axis along the electrode can only be acceptable to describe the motion of the hypothetical particles. This means that the force might exert on the vortex motion of the particles during these traveling in either an electromagnetic or magnetomagnetic sense.

418

Top view of interface

Axis of vortex along surface Interface

Vortex axis Figure 6.

Electrolyte

Schematic view of vortex with axis along electrode obtained by numerical simulation.

At the electrode surface, strictly the interface between the electrode surface and the bulk of the electrolyte, there is a potential difference, where electrons flow toward outside in the electrode and ions in the same magnitude transfer in the electrolyte. Under the circumstance of a constant current the induced magnetic field (obeying the Maxwell equation) was numerically analyzed using Finite Element Method (FEM). 6 The full 3-D FEM program (ANSYS) was used for the analysis of magnetic field in the vicinity of the electrode surface and of the electrolyte bulk in the electrolytic cell where the geometrical model (Fig. 1) was made for the boundary conditions. The values of the magnetic flux density of the electrolyte were in the range of 1.91xlO~ 3 T with some regional scattering, while those of the electrode in the range of 0.0055 T within narrowed region. Apparently the amplitude of the electrode vectors exhibits almost three times higher value than that of the electrolyte. 3.4. Force Exerted

on the Motion

of

Vortex

It is recognized that the electromagnetic interaction of charged particles possessing momentum with a given magnetic field yields the force, i.e., Lorentz force exerting on the orbit of particles. Without any interaction the LGCA result shows that given vortices are integrated to form a vortex string which morphology looks like arnt nest or tangled or coiled strings inside the electrode (Fig. 7a). In cold fusion experiments a big negative current is thrown to the interface, where the magnetic field asymptotically changes from an electrode to an electrolyte. Then, the obtained vortex pattern is seemed for a vortex string to be occationally appeared on an electrode surface. Therefore, some part of a vortex string locates exactly at the interface leaving the locus of moving particles mass. At the first stage hypothetical particle mass move coincidently (the scavenging of N-cycle model) and evolves a vortex string having a given circular radius (Fig. 7b). Next at the interface the radiuses are modified depending on the inherent particles velocity and the varying magnetic field. The maximum elctromagnetic interaction by external magnetic field

419

(a)

(b) Interface

\ + }<&' ->

*****

-?-

Electrolyte

Electrolyte Interface

Figure 7. Schematic of vortex string without magnetic interaction (a), locus left at the interface, where radius of circular motion is modified under influence of varing magnetic fields (b).

can be evaluated as r =

mv/eB,

(1)

where r is a circular orbital radius, and m and e are a mass and charge of a given particle, e.g., electron, and B is a magnetic flux density. The reasonable value of r is given under orthogonal velocity and magnetic flux vectors. Inspecting the appeared vortex (Fig. 5), the above events occurred several times leaving the accumulated circules. In Fig. 5 minimum radius was extrapolated taking into account all the circumferences projected on the leaned base plane. Using the experimental data: r = 41.7 ± 0.3 /jm the maxuimum velocities for electron mass and deuteron mass are calculated as 4.6 ± 0.33 x 104 and 12.5 ± 0.90 m/s, respectively. Although more accurate simulation might be needed to reach a definitive conclusion, it is noted that the motion of the hypothetical particles, e.g., electrons exhibits significant kinetic energy to account for the further interaction. 4. Conclusions The reality of the scavenging in N-cycle model (proposed by H.N.) was proved by LGCA and FEM numerical simulation methods. We investigated vortex pattern appeared on Pd surface after long-term electrolysis in 0.1M LiOD. The N-cycle model predicted that the hypothetical particle mass flow coincidently through the electrode surface/electrolyte interface. By LGCA method simulating the motion of such particles mass the formation of vortex along the electrode (not normal to the electrode surface) was proved. From the comparison of these vortices from simulation and the result of experiment it is elucidated that the magnetic flux density at the interface has the influence on the motion of these particles mass.

420

Acknowledgement I would like to t h a n k Dr. Naoki Takada at t h e National Institution of Advances Industrial Science and Technology for helpful discussion.

References 1. H. Numata and I. Ohno, Fusion Technol. 38, 206 (2000). 2. H. Numata and I. Ohno, Proc. 6th Int. Conf. Cold Fusion, Toya Japan, vol. 1, p. 213, NEDO, The Inst, of Appl. Energy, (1997). 3. R. Takagi et al, Fusion Technol, 19, 2135 (1991). 4. H. Numata et al, Proc. Conf. Sci. Cold Fusion, 33, p. 71, in: T. Bressani, E. Del Giudice, and G. Preparata (eds), SIF, Bologna, Italy (1991). 5. H. Numata et al, Proc. Mini Symp. Cold Fusion, Tokyo Metropolitan University, pp. 129 (1990). 6. H. Numata and M. Ban, Proc. JCF6, 32 (2005), http://wwwcf.elc.iwate-u.ac.jp/jcf/ file/jcf6/jcf6 _proceedings.pdf. 7. E. Lewis, Proc. ICCF10, MA, USA (2003). 8. T. Ohmori et al, Fusion Technol, 33, 367 (1998). 9. Y. Toriyabe et al, Proc. ICCF12, Yokohama, Japan (2005). 10. D. Coupland et al, Proc. 1st Annu. Conf. Cold Fusion, 299, Utah (1990). 11. H. Numata , in book "Cyber X" No.ll, pp. 37 (1999) Kougakusha. 12. A. Takahashi et al, Nuclear Reaction Study In Condensed Matter No. 1, Chapter 4, p. 124 (1999) Kougakusha. 13. Y. Matsukuma and R.Takahashi, Trans. JSME, 61-588, B, 2826 (1995).

U N U S U A L S T R U C T U R E S O N THE MATERIAL SURFACES I R R A D I A T E D B Y L O W - E N E R G Y IONS

B. R O D I O N O V Moscow

Engineering

Physical

Institute (State Moscow 115407,

University), Russia

Kashirskoe

shossse,

31,

I. SAVVATIMOVA Federal State Unitarian Enterprise Scientific Research Institute "Luch", Zheleznodorozhnaya, 24 Podolsk, Moscow region 142116, Russia E-mail: [email protected]

Some unusual structures on the surface of metals and films (various X-ray films and nuclear emulsions) caused by exposure to bombardment by low-energy ions in glow discharge plasma, in electrolysis and other low-energy processes (when energy of particles does not exceed several keV) have been f o u n d . 1 _ s The mechanism and model of the strange tracks formations and explanation of their structure change are suggested.

1. Introduction For a number of years in various laboratories of the world physicists discover strange tracks (which we call traces, whereas the objects that cause them are termed as tracers). 1 _ 5 The traces, as a rule, are characterized by a microscopic width (usually about 10 /im), but their length is presumably unlimited (mm and more). Sometimes the traces look like a repeated pattern, similar to the tread design of a motorcar tire or a necklace (Fig. 4). Sometimes the pattern forms a continuous line or a group of parallel lines, differing from the standard tracks left by heavy charged particles in nuclear photo-emulsions by their angularity or enormous length (up to cm). Occasional flaws of the samples containing traces (on the polished surface of metals or in photo-emulsions) do not explain the connected occurrence of the traces at the places of local energy generation: electrical discharges, particle accelerator targets, and the areas of natural disasters or technogenic ones, which are caused by the human activity. This feature of the phenomenon in question may be used to predict or to avoid the technogenic disasters, for example, the search of traces or tracers can help in analyzing the causes of the Chernobyl Catastrophe. 2. Experimental Results and Discussion We observed the unusual structures on the surfaces of metals after glow discharge exposure (Fig. 1) and on the films (various X-ray films, nuclear emulsions, 421

422

and others), placed both on the inside and the outside of the glow discharge chamber (Fig. 2). The similar tracks formations (with periodical repeating structure) were found on the nuclear emulsion films after the neutron generator exposure (Fig. 3). Such tracks structures as demonstrated in Figs. 1-3 (regular structures, spirals, chains, chains of voids, and others) need the comprehensible explanation from the viewpoint of material science and demand special physical interpretation. However, the classical approach to the study of physical phenomena requires not only substantiation of the principal possibility of the process in question, but also its detailed description including illustrative examples. The latter may become possible on the basis of a model of filiform (thread-like filament) matter, i.e. fluxes. Some components of the "flux theory" will be discussed below in application to the problem under discussion. Along with traces (in metals to the depth of 1-2 cm), changes in physical and chemical properties of underlying layers from the viewpoint of their composition and structure are observed (see table for Fig. 4). Under the surface of previously monolithic sample some micro-tunnels and "holes" appear (Figs. 1-4). On the surface of the samples examined before the exposure without any distinctive properties, not only traces, but also some microscopic structures - films, hollow spheres and cylinders, threads, spirals, complex spherical and cylindrical formations looking like "cabbages" or "sausages" - were discovered after the exposure to low-energy ions (Figs. 1-4), electrons or, ultrasound action . Sometimes these structures remind bacteria or a colony of bacteria, which may glow (fluoresce) in the dark. These objects move randomly and appear on the surface or "plunge" back into the depth of the previously monolithic material. This activity of "live" bacteria objects may continue for weeks after the energetic influence (after it has been finished).4 Each of these objects is unusual in the shape, surface structure, and the chemical composition. The chemical composition in these formations is sharply distinguished from the composition of the basic material on which these formations had arisen (table to Fig. 4 with chemical composition). We shall take into account that all these objects have been obtained under conditions of low-energy particles influence when the nuclear processes in materials from the traditional point of view could not exist. Therefore, at present there is no comprehensible hypothesis for the formation of such structures from the impurities. We shall also take into account, that the majority of the chemical elements forming unusual structures were not present in the initial material, and in the composition of the surrounding medium or in constructive details of the experimental installations. Thus, the shape, structure, and composition of unusual objects demands special explanation, probably, based on new physical concept. This unusual concept, as well as their possible practical application requires further examination of unusual structures.

423

;

•

>

*

n*^ (c)

(b)

(a)

*^P

(e)

(d)

(f)

Figure 1. Tracks on Pd surface after deuterium glow discharge exposure (optical microscopes (a, b5 d-f) - Pd surface after deuterium bombardment, (c) back side, marks (a, c, and e) 100 /xm, (b and d) 70 /im, and (f) 200 fim. (a) The micro-tunnels, (b-d, f) The spiral formations, (d) The spiral curve and straight lines formations on Pd surface, (f) The spiral broken lines formation.

3. Explanation and Possible Mechanism We can offer two approaches to the explanation of the formation of such unusual structures: integrated and differential approaches.

if^

(b)

(c)

•t (d)

(e)

Figure 2. The structure on the films placed outside of the glow discharge chamber with stainless steel wall (a, d) and quartz walls (b, c, e) after deuterium glow discharge with Pd (a, d), and with Zr (e), with W (b, c). (a) "Melting bubble" on X-ray film (RT-2 type) after deuterium glow discharge with Pd. (b) The parallel tracks on X-ray film (Kodak Bio Max) after deuterium glow discharge with W-W cathodes, (c) "Cylindroid" (like "sausage") on the nuclear emulsion after deuterium glow discharge with W-W cathodes, (a-c) Marks are 100 /xm; (d, e) 50 /xm.

424

3.1. The Integrated

Approach

In the view of long-range action concept in which development Feynman R.P., Yu. S. Vladimirov, and others participated in the second half of 20th century, formation of the complex objects, capable of leaving observable traces with complex structures (TRACERS) can occur instantly and at once.6""9 As from experimental researches in the end of 20th century, the traditional concept of philosophical reductionism (occurrence of big object from small parts) in many cases showed physically insolvent. The vivid example of this is the detection of fractional quantum effect of Hall (the Nobel Prize of 1998) and his theoretical interpretation by Robert Laughlin. 10 The observable fractional charge of current carriers in semiconductors appears as a result of the certain condition of all semiconductors. Self-similarity as direct consequence of long-range action explains any transformations of substance as quantum transitions in the Universe. So, occurrence of observable forms of life in the Universe or complex structures of unusual chemical compound (such as TRACERS) on surface of electrodes bombarded by ions are the next state of the Universe. Self-similarity of objects of the Universe could explain the process, but does not allow considering the dynamics of such quantum transitions.

(a)

(b)

Figure 3. The periodical structure track on the nuclear emulsion after neutron generator exposure (b) three-ray "star" (—•) is the results of fast neutron interaction with carbon nuclei with three alpha particles formation: 1 2 C + n -—> 3OJ + n. (a, b) Marks are 100 ^m,

3.2. The Differential

Approach

It is based on stage-by-stage formation of complex objects from more simple ones and allows considering dynamics of transitions from simple to complex. This second approach from reductionism position is traditional methodology, but, as against the first approach, in our case it does not allow "to skip" through the basic difficulties. The possibility of "cold" transmutation of atomic nucleus is not simple to explain from this position. We suggest overcoming these difficulties on the basis of consideration of a new hypothetical filamentary structure of matter. The basis of using such extravagant assumption is the astrophysical data on presence in cosmos of the so-called dark matter, which makes the most part of mass of the Universe.

425

The dark matter can have filamentary structure. If diameter of filament is closed to the diameter of atomic nucleus, they will easily pass through any dense substance of usual nuclear-molecular structure (through any solids, planets or stars). In the author's model such filaments - fluxes - can be cylindrical atoms. The nucleus of such a cylindrical atom can represent a quark - gluon filament stabilized by quanta of magnetic flux, and an electronic shell - an electronic Bose-liquid with properties of super fluidity and superconductivity. The diameter of flux electronic shell according to calculations is ~60 f.11 Fluxes can create an invisible grid, which wrap round not only far Cosmos, but also all our planets, penetrating all bodies (solids) existing on the Earth (including us with you) and influencing them in the various ways. Interaction of invisible fluxes with usual nuclear-molecular substance could be in the various ways. 11,12 The huge gradient of a magnetic field promotes an attraction to magnetic poles of particles with nonzero magnetic dipole moment (electrons, protons, neutrons, many atomic nucleus, atoms, molecules, and ions) which can enter in nuclear interaction. Elementary calculation shows that frequency of nuclear processes on magnetic poles of hypothetical filaments - fluxes should reach 10 14 -10 15 s _ 1 , which enables evolution of an output power of 100 W. The approximate, rough estimation (rough guess) is given below. Assuming the magnetic moment n of the shell of paramagnetic atom (molecule, ion with radius « 1 0 - 8 cm) to be of Bohr magneton and equivalent magnetic charge of the flux end (magnetic pole) to be minimal Dirac's magnetic charge em RS 70e (e is electron charge), one can estimate magnetic attracting force of the atomic particle to the flux end, F = 2 / ue m /a 3 ss 1 0 - 3 dyne, and the time of flight of the captured atomic particle with mass of ^ 1 0 - 2 3 g to the flux end to be about 10~ 14 s. This magnetic attraction determines the "self-aiming" of the atomic nucleus to the flux end. Besides, if the flux end is situated inside or on the surface of the dense (solid or liquid) paramagnetic matter, there may happen up to A x 10 14 nuclear interactions per second, where A is the mass number of the captured nucleus. At the nuclear distance, rN w 10~ 12 cm, the attracting force of the nuclear particle with a magnetic moment fiN nearly equal to the nuclear magneton (fi/fiN ~ 2000) to the flux end (magnetic pole) is FN = 2^Mem/riN ~ 5 x 105 dyne and the magnetic N N energy of one nucleon capture is F r ~ 1 MeV or A MeV per one captured nucleus (atom). For A ~ 10 this corresponds to the power of approximately 100 W. Nuclear reactions can also go on lateral surface of fluxes in an electronic Boseliquid, which shields the electric charges of nuclei. 11 In the end, plenty atomic nuclei in the usual nuclear-molecular substance forming lengthways ensembles of fluxes quanta with the cross sizes about 100 /xm 13 ' 14 can interact simultaneously. Thus, the problem of cold nuclear fusion and nuclear transmutations in the fluxes model is authorized by three ways: transformation of atomic nuclei on magnetic poles ends of fluxes, in electronic liquid on a lateral surface fluxes and in multinuclear reactions in associates of fluxes nuclear ensembles.

426

The analyzed place

Element

Atomic %

Fig. 4 (c), Point 1

Mg Fe Ga Pd 0 Mg Ca Pd 0 Al Fe Ga Pd Fe Ga Pd

2.43 ± 0.17 8.39 ± 0 . 2 6 2.48 ± 0.39 86.70 ± 0.48 54.36 ± 1.64 3.92 ± 0.32 2.73 ± 0.28 38.98 ± 1.61 10.20 ± 0.69 3.71 ± 0.17 4.75 ± 0.26 2.72 ± 0.36 78.61 ± 0.79 11.32 ± 0.27 1.43 ± 0.47 87.25 ± 0.52

Fig. 4 (b), Point 2

Fig. 4 (c), Point 2

Fig. 4 (d), Point 1

Figure 4. The structure formations (traces) on the P d surface after deuterium glow discharge, (a) Mark is 5 jtxm. (b) Mark is 10 //m. (c) Mark is 10 /im. (d) Mark is 20 /im.

Due to non-conservation of spatial parity in e-capture in the powerful magnetic field of fluxes, the main flow of arising neutrino is directed against the force lines of a magnetic flow. As the result of e-capture the filaments of neutrino at the northern magnetic pole create jet traction, which pulls the filament after North Pole (like a locomotive pulling its cars). At the southern magnetic pole force of reaction of neutrino pushes (compresses) the filament, because of which unstable movement of South Pole of the filament is possible. Due to output power of capacity during the nucleus transmutations, a part of "new" nucleus is formed on fluxes, in particular, nucleus with zero spin and, hence,

427

with zero magnetic dipole moment. They should scatter, forming a "hot" shell of these "new" nuclei near fluxes filament, which are inside dense nuclear-molecular substance. Due to melting and evaporation of nuclear-molecular substance with its subsequent condensation on cold parts of the sample, nuclear active fluxes leave their complex structured traces both on the surface and inside samples in which they are formed (Fig. 1). The nuclear active fluxes or complex fluxes object (we name such an object TRACER) can move along trace (trajectory) in the substance. The filamentary tracer of the structure can leave the trace without moving at all or moving, for example, in the perpendicular direction to a line. In Fig. 5 the presumed mechanism of formation of the various-shaped tracers is shown. The atom-molecular quantum ensembles surrounding fluxes (the grey colored cylinder in Fig. 5) push out the fluxes (the white colored cylinder) to the periphery of the ensemble where the temperature of ensemble substance is lower, the density of atoms is higher and probability of polynuclear reactions is the highest, too (Fig. 5b). Such pushing-out results in bending of flux and atomic-molecular ensemble surrounding it and interacting with it (Fig. 5c). In turn, the bend of ensemble with fluxes can lead to turning the ensemble with fluxes into a ring or a spiral (Fig. 5 d,e).

(a) (b)

(a) Figure 5. Fig. 5).

(c)

(b)

(d)

(e)

(c)

(f)

(d)

(g)

(e)

(h)

(f)

Flux model of strange tracks formation (5 a : top row of Fig. 5, 5b: bottom row of

Let us note that sometimes geologists found out such spirals of microscopic sizes, for example, of refractory tungsten inside various compact samples (in rock) in reality. Geologist Elena Matveeva found tungsten spirals inside 200,000-year-aged rock (Fig. 6). Formation of more complicated bodies of cylindrical or spherical symmetry during warming-up by nuclear reactions (Fig. 5b f,g) is also possible. The formation of hollow cylinders and spheres is possible as a result of oozed gases in chemical and nuclear reactions in environmental substance around fluxes (Fig. 5bh). Sometimes

428

it is possible that such elementary processes create hollow quasi sphere particles ("blobs") and extensive hollow "cylindroids" on surfaces of a metal sample (Fig. 5b a-c). "Blobs" and "cylindroids" can be broken off on the surface (or near surface) of the sample by internal pressure of gases contained in them, leaving in the local zones of metal surface the melt films formed near nuclear active fluxes. Helicoid atom-molecular shells of nuclear active fluxes in projection to the flat surface of sample frequently give the sine "paths" - "trajectory" with changed composition of the basic material (traces in Fig. 5b). From known mathematical Fourier's theorem it follows that the sum of sinusoids (or cosinusoids) with different amplitude and period can give a track of any shape, the geometrical pattern repeating periodically. Such kind of double spiral object we found on the X-ray film, exposed outside of glow discharge chamber after deuterium experiment (Fig. 2d). 2 In our opinion, the origin of mysterious periodic patterns (chains and more complex trajectories, Figs. 1-4) on the surface of the samples (Fig. 5b d-f) can be explained by such kind of processes. Thus, concentration of the fluxes earlier not participating in the process of nuclear interaction with substance (Fig. 5b e,f), but activated by electromagnetic and nuclear processes in various places of trace is possible. This secondary interaction of the fluxes can considerably complicate the trace figure. Especially the composite figure can arise from the cooperative action (combined effect) of several nuclear active fluxes, which form, for example, enclosed spirals (Fig. 5b f), and from activation of earlier passive secondary (tertiary) fluxes, transiting through a trace.

^

^*

4K

mmk

Figure 6. The tungsten spirals 200,000-year-aged inside the bore pit rock was found by geologist E. Matveeva.

4. Conclusion We hope that further investigations of these unusual strange formations on the surfaces of various materials subjected to various low-energy exposures, will allow

429 establishing the t r u e mechanism of unusual structures formation. Applied prospects of such examinations will naturally be defined by physics of probable unusual processes the examples of which we have considered.

References 1. T. Matsumoto, Steps to the discovery of electro-nuclear 060-0813, Japan (1999), p. 289. 2. I. Savvatimova, Reproducibility of experimental in GD. ICCF8, Italy (2000), p. 277. 3. M. Solin, Experimental facts of F initiation. 11th Rus. Conf. Moscow (2004), p. 90. 4. A. Agapov S. and L.I. Urutskoev, Proc.lSth Rus. Conf. on CF, Moscow (2005), p. 25. 5. B. Bogdanovich, Applied Physics, Moscow, MEPhI (2000). 6. J. Wheeler and R. Feynman, Rev. Mod. Phys. 24, 425 (1949). 7. Yu. Vladimirov, Moscow University Press (1996), p. 264. 8. Yu. Vladimirov, Theory of Phys. Interactions, Moscow University Press (1998), p. 448. 9. B. Rodionov, Proc. of 12th Rus. Conf. on CF 2004, Moscow (2005), pp. 136. 10. R. Laughlin, The Quantum Hall Effect (Springer, Heidelberg, 1987), p. 233. 11. B. Rodionov, Gravitation and Cosmology 8 (Supplement), 214 (2002). 12. B. Rodionov, CF of the 10th Rus. Conf. 2002. Moscow (2003), p. 50. 13. B. Rodionov, Proc. 11th Rus. CF Conf. Moscow (2004), p. 189. 14. B. Rodionov, Proc. 12th Rus. CF Conf, Sochy 2004, Moscow (2005), p. 110.

C O N T E X T FOR U N D E R S T A N D I N G W H Y PARTICULAR N A N O S C A L E CRYSTALS T U R N - O N FASTER A N D OTHER LENR EFFECTS

SCOTT R CHUBB Research

Systems

Inc.,

9822 Pebble Weigh Ct. Burke, [email protected]

VA 22015-3378,

USA

Two persistent questions have been: (1) Why is it often necessary to wait for a finite period of time before the Excess Heat effect is observed after palladium (Pd) has been sufficiently loaded with deuterium (D), that the near full-loading condition (PdDz, 0.85 ~ < x —> 1) that is required for Excess Heat, has been achieved? (2) Is it possible to identify physical properties of the materials and/or crystals that are used that might be playing a role in the interval of time associated with this phenomenon? Recently, I generalized conventional energy band theory to address both questions. The new theory can explain these experimental results but will be ignored by most scientists. I suggest that this is expected: The context of energy band and Ion Band State (IBS) theory is very different from the context of hot fusion theory. Even within the Low-Energy Nuclear Reactions (LENR) field, hidden, simplifying assumptions exist, which implicitly reflect biases associated with the context of hot fusion. A typical example is the idea that a single, particular form of reaction or environment can explain all LENR phenomena. As opposed to such a picture, involving a single "nuclear active environment" ("NAE"), the context of IBS theory and many-body physics suggests a more realistic and useful description of LENR involves a multiplicity of "nuclear active environments" (NAEs).

1. Introduction Context can profoundly affect discourse and debate. Facts taken out of context can significantly misrepresent opinions or statements. Also, incorrect assumptions, resulting from context, can result in false conclusions. Thus, context can profoundly affect communication: For example, if a man yells "fire" or a fire alarm goes off in a crowded movie theatre, considerably greater harm can result, through potential panic, than if the same thing happens in a movie theatre containing a small number of people. Over the years, Ion Band State (IBS) theory papers have focused on particular effects but have not included a complete description of the limitations and applicability of the theory. Thus, qualitative language, involving quasiparticles (for example) and other terminology has been used; while, in later discussions of the theory, a highly mathematical formulation was presented that many readers found difficult to follow. A useful context for understanding the IBS theory of Low-Energy Nuclear Reactions (LENR) and its relationship to other theories or effects involving either hot fusion or LENR has not appeared. In particular, despite the apparent successes 430

431

of the IBS theory, not only has the theory failed to be accepted, it has provoked unusual responses, including inaccurate statements, in separate Editorial comments in Nature magazine 1 and one of the ICCF conference proceedings. 2 ' 3 These responses have a plausible explanation: IBS theory follows from a known context 4 - 6 (hydrogen in metals) that should apply to Cold Fusion (CF) but is inconsistent with hot fusion. As the theory has evolved, more general ideas 7 - 9 have justified the underlying physics. Despite the fact that to date, no unifying theme or context for understanding the IBS theory in CF has appeared, the more general ideas relate to an important, unifying idea: The problem of relating crystal size to transport phenomena involving charged or neutral particles in finite lattices. 10 In particular, transport phenomena, in general, can become quite complicated in finite solids. But partial periodic symmetry can be used to identify a hierarchy of processes, in which all of the particles located in some "periodically ordered" region, or some subset of it, can "move" coherently in a perfectly rigid manner (similar to the rigid, lattice recoil, in the Mossbauer effect) that preserves the separation between each particle with the remaining particles. These effects are the basis of a known phenomenon (an Umklapp process) that occurs in phonon scattering and electrical conductivity. In infinitely-repeating lattices, this process is described by a resonant effect, in which momentum is not conserved between "quasiparticles." Instead, the momentum is transferred to the lattice elastically. But momentum conservation requires that quantitative bounds exist for the amounts of momentum that can be transferred to a surface or interface (and vice versa) through these kinds of processes. Traditionally, in models in which the lattice is infinitely repeating and periodic, these bounds have been poorly defined. In finite solids, at low, but finite temperature T, precise, size-dependent bounds can be identified. In larger crystals, collisions with phonons tend to reduce the magnitudes of these effects. In smaller crystals (or in optical lattices 11 ), this is not the case. In the case of palladium-deuteride (PdD), the effects can be quite large and can lead to coherent forms of interaction 12 and potentially LENR. Initial estimates of the magnitude of the effects suggest a particular time scale for triggering the coherence that can be related to the incubation time 13 associated with CF. But, as in the past, this material was not introduced within the context, of a more complete theory. 10 ' 12 The present paper includes a more detailed description, involving the context of the more complete theory. 10 ' 12 This material, which is presented in the next section, provides a useful context for understanding the importance of the complete theory and its application in problems involving LENR. It includes a discussion of some of the earlier motivating work that led to the theory and material that provides a context for generalizing earlier results to more general problems involving LENR. The next and final section summarize how the more complete theory can explain triggering in d + d —• 4 He in finite size PdD crystals.

432

2. Toward an Understanding of an Appropriate Context for LENR 2.1. Role of Context Theory

in Lack of Acceptance

of Successes

of IBS

Beginning with ICCF1, 2 we predicted 2,14 that by occupying IBSs, deuterons (d's) could initiate CF, without creating high energy particles, in a particular limit, involving "high-loading" (i.e., x —> 1 in PdD x ) in PdD. Here, IBS refers to a state that can be occupied by a deuterium nucleus (a "d"), in which the "d" effectively begins to behave in a wave-like fashion, similar to the way that an electron behaves in a periodically ordered solid; i.e., as a wave-like, "quasiparticle." In reality, this picture is a simplified description of the many-body physics, where the underlying effects occur in particular matrix elements associated with particular forms of overlap and rates of reaction. However, through this interpretation (involving quasiparticles), we suggested a number of effects, associated with the particular limit of full-loading, that can be used to justify a number of observed effects,14 follow from very general features of the underlying physics. In particular, the physics of the d IBS limit requires that in PF experiments: (1) 4 He should be the primary product. (2) This product and heat should be the dominant phenomena. 14,15 (3) The reaction should not create high energy particles. (4) Neutrons and tritium can be present but in amounts that should not account for the heat and should be negligible in comparison to the amounts of 4 He. (5) That periodic order should be required on some time-scale commensurate with initiating the effect. (6) High-loading should be required. 14,15 We also thought hard X-rays could be emitted 14 (during ICCF1) through the process that dissipates the heat. Six months later, 15 we suggested an alternative form of heat dissipation: That the lowest energy processes should occur through small fluctuations in D-loading that should approximately preserve periodic order inside a PdD host, the 4 He should occupy IBSs in the interior of the host, and that heating should take place in regions near the surface. As a consequence, based on a single physical picture (involving small fluctuations in loading in PdD), we suggested that the 4 He accounts for the heat and should be seen predominantly either outside heat-producing electrodes or in surface regions, near the boundaries of the electrodes. We made these predictions 18 in 1990 before experimental evidence was publicly disclosed (in 1991) that high-loading in PF experiments apparently was required 2 ' 16 and the initial observation 17 that a correlation appeared to exist between Excess Heat and residual amounts of 4 He found outside heat-producing electrodes. Two obvious limitations of the initial picture were: (1) It requires a particular kind of state (a quasiparticle band state), known to be useful in describing the behavior of electrons, but whether or not this state in an ionic form would be appropriate for describing CF effects as well as the behavior of d's in the limit of full-loading in PdD was not clear and (2) Even in the case of electron transport, the quasiparticle energy band picture is approximate and conventionally applies (in metals, where transport phenomena have been most widely studied) only over

433

large distances and when the externally applied fields vary sufficiently slowly, ft was not at all obvious, within this context, that the associated picture could apply in a problem involving d+d fusion, where large changes in external fields could be required over short distances. An important goal of the more complete theory 10 ' 12 was to address both of these limitations from the outset. In order to accomplish this, a mathematically rigorous formalism, based on a generalized form of multiple scattering was developed,7 that could apply in finite lattices, was derived that potentially can also explain why high energy particles are not required in CF reactions. This formalism provided a way to generalize conventional band theory to cases involving finite lattices. Within this context, it was possible to generalize conventional band theory by requiring that it apply to the ground state (GS) and lowest lying excitations and that the GS have minimal coupling to outside processes. Then, the lowest energy excitations of a solid, by construction, are required to conserve charge in some finite volume of the solid and are required to be unaffected by a symmetry: rigid translations (Umklapp processes) that preserve the separation between any two particles within this region. 10,12 ' 13 We have made other predictions that have not been tested: (1) That when 4 He is externally introduced into the surface region and the region immediately outside heat-producing materials, might catalyze the d + d —» 4 He reactions through a form of Bose-induced stimulation, similar to stimulated light emission in lasers 20 and (2) that the observed anomaly (associated with the substitution of PdD for PdH) in the value of superconducting critical temperature Tc (in which Tc is higher than in the case of PdD) might be the result of "Cold Fusion" at low temperature. 21 Because in the initial announcements, PF suggested that Excess Heat was the result of a colder version of conventional fusion, ideas, even tangentially related to cooperative forms of reaction, were entirely ignored. In an entirely unconventional and unjust manner, David Lindley1 explicitly criticized these ideas and our theory almost a year after he received our first paper, 22 without explicitly referring to our work, through his derisive commentsl (about Bloch and Wannier states, and Bose condensates): "[A] broad category of cold fusion theories rested on more sophisticated uses of collective effects [in solids]"... These theories had the special attraction that they could easily be decorated with the jargon, at once forbidding and enticing, of solid-state physics: Bose-condensates, Bloch states, Wannier functions... like the Paris fashions, they outface mockery... "Nevertheless they were all wrong, and for a straightforward reason. The fusion rate for two deuterons is calculated from their two wavefunctions, multiplied by the nuclear interaction rate. The latter is a very short-range force, only at separations of a few nuclear radii is the nuclear reaction rate significant. The only important contribution to the fusion rate, therefore, comes from the product of the wavefunctions when the deuterons are very close. But the wavefunctions in the Bose-condensed state are calculated explicitly by ignoring the nuclear interactions; they are valid everywhere except at close range." 1

434

During ICCF2, 2 Giuliano Preparata also criticized our theory 2,3 because it appeared to ignore the key problem (involving the Coulomb barrier) that seemed to be relevant in the CF problem. In fact, both sets of comments reflected biases, associated with conventional fusion. However, as opposed to Lindley's approach, which involved first ignoring the relevant science in our paper, not publishing the material, and then criticizing its ideas (based on incorrect information about the relevant physics), without appropriately referencing the material, not only did Giuliano Preparata allow our ideas to be published, but he actively participated in a useful scientific debate about their relevance. Lindley's comments had some value. He pointed out (as in conventional fusion) close proximity between d's, at a single location, is required for a nuclear reaction to occur, and effects of electromagnetism (EM) can be treated as being static, relative to the dynamical effects involving the nuclear forces (NFs). This picture applies to conventional situations involving higher energy incident particles in nuclear reactions, and especially in hot fusion, where deuterons have a sufficiently large incident kinetic energy. Then , the time- and length-scales involving EM and NFs are so different that the total wave function $ can be factored into the product of separate components $ n u c and $em (through the d-d separation variable r): * = $nuc(r)$em(r). 4

(1)

In ordinary d + d —> He + 7, in fact, at all times, the dependence of the coupling to the electromagnetic field must be included. 23 Although this fact has been known since the early 1970s, it does not appear in conventional fusion literature because the d + d —> 4 He + 7 occurs at a rate that is ~ 107 times slower than the comparable rates associated with the dominant (d + d —> 3 H + p and d + d —> 3 He + n) reactions. On the other hand, the reverse reaction, 4 He + 7 —> d + d has been studied in detail. Here, it is known in fact, as opposed to the reaction involving the simple form, associated with Eq. (1), a comparable factorization between NF and EM wave functions is not possible because the associated dynamics requires detailed information 23 about the coupling of the EM interaction with the NF. Lindley misquoted this as well as a number of additional facts, including the nature of the d + d —> 4 He reaction, which he had not investigated, and the fact that d's have unit spin. Also, at the time, important information about the nature of products was not known. With hindsight, his comments illustrate a misunderstanding of fundamental aspects of many-body physics. In particular, although in 1989, Bose-Einstein condensates (BECs) had only been observed in natural processes in cryogenic environments, involving near absolute zero T in helium, noncryogenic procedures involving laser-cooling were being developed for creating BECs. Beginning in 1995, these procedures made it possible to dynamically create BECs. Since that time, not only has it become possible to create, manipulate, and alter BECs, using lasers but to artificially stimulate phase transitions, in which states involving an initial configuration of localized bosonic atoms (that remain confined in regions of space, defined by particular lattice sites in an optical lattice) into delocalized

435

(coherent) states in which the bosonic atoms exhibit the kinds of wave-like behavior, that we suggested might be relevant, are produced routinely. 2.2. A Meaningful Symmetry

Context for LENR

based on Broken

Gauge

Although Lindley was conceptually wrong, his use of Eq. (1) illustrates an important source of confusion: Eq. (1) is based on a number of assumptions involving length and time scale. In particular, the associated picture assumes that because nuclear reactions are initiated, with high energy, initially, the effects of EM can be ignored. In hot fusion, this makes sense since in hot fusion, a form of perfect "SU2 symmetry" can apply, in which it is never possible to distinguish between protons and neutrons. In the normal nuclear physics scenario, then, to have protons and neutrons close enough together for reaction to occur, it is assumed they occupy a state involving asymptotically free nucleons, in which effects of EM can ge ignored, as Giuliano Preparata emphasized. In fact, when additional symmetries are present, this picture need not apply. At noninfinite temperature and energy, residual EM interactions are present that break SU2 symmetry. In all situations, the process of lowering the energy requires loss of symmetry. This occurs because of a general requirement: The GS, by definition, to be stable, must have the smallest overlap with outside processes. When many particles are present, however, as opposed to a gradual reduction in symmetry, involving de-excitation between states, near the asymptotically free state (assumed as the initial state in nuclear physics), an entirely different situation can occur, provided the overlap process involves changes in momentum and energy, involving the EM interaction. In particular, as opposed to de-exciting an initial state, involving asymptotically free particles, an initial state involving potential nucleon overlap can form through an approximate symmetry, and the de-excitation process can result from an instability associated with the symmetry. Within this alternative context, as opposed to nuclear reaction being initiated from an extremely excited state, involving a small number of particles, a combined motion of many particles, at or near the GS configuration, can take place and lead to nuclear interaction. From this near GS configuration, as opposed to forms of interaction that couple the highest possible states of excitation with an effectively asymptotically free state, the de-excitation process can involve many particles that all have effectively the same energy and momentum, in a configuration in which all particles actually have negligibly small kinetic energy. An important symmetry that can cause this is associated with the peculiar limit (involving the kind of rigid-body, Mossbauer-like, Umklapp processes, alluded to above) in which many particles, at once, move rigidly, in such a way that the separation between any two particles remains the same. This can be accomplished through a second observation, made by Preparata: That the zero of momentum can be altered, dramatically, by a classical motion, involving many particles moving in a particular way. An important point that Preparata did not fully appreciate, however, is that it is never possible,

436

a priori, to constrain a collection of particles within a particular volume, in such a way that the locations of the particles can be identified. Because the velocity of any particular, rigidly moving configuration, relative to the velocity of a second rigidly moving configuration, can be continuously varied, a large degeneracy exists, in principle, associated with many, closely related, rigidly moving configurations. In fact, in the absence of charge accumulation at the boundaries of a solid, these different configurations are related, in principle, to each other through a (trivial) but continuously varying change in a particular parameter (the center-of-mass momentum) that can be related to the choice of gauge, 12 associated with the vector potential. As a consequence, the associated symmetry is referred to as gauge symmetry. In the limit in which this form of symmetry becomes dominant, asymptotically, in a sufficiently large solid, it is possible to require that far from the boundaries of the solid, effectively, in the evaluation of any relevant matrix element (associated with a particular many-body process), Eq. (1) remains valid for any configuration involving nucleons, provided no change occurs in the relative separation coordinate (r) between the center-of-mass (CM) coordinates of different charged particles (associated with the behavior of $ E M W ) m regions located far from potential overlap with NFs; while in regions where the relative separation in CM coordinates overlap with NFs, changes are allowed to take place, provided the resulting changes in momentum are all transferred to a total change in the CM momentum of the solid, through an Umklapp process. From such a starting point, Preparata's idea that many particles can move at once can be generalized: Instead of one configuration moving classically, with a single momentum, all possible configurations, in which each configuration is related to the others by a fixed difference in momentum, can be allowed to take place. In all relevant interactions, all momentum from a potential LENR can be transferred instantly 12 to the CM without altering the relative energy or momentum in interior regions where the EM interaction is dominant. Formally, this requires that energy and momentum are conserved, but how this occurs is ambiguous since it is not possible to determine the locations of the charged particles within a particular volume. Within the constraints of this limit, the form of separable wave function, involving Eq. (1), can be generalized: Instead of particular pairs of d's (as we initially suggested), associated with conventional fusion, at far separation (through $ E M ( r ) , where r is large, relative to NF overlap) or at near separation (where $ n u c (r) applies, at locations where r has overlap with NFs), each function $EM(»") or $ n u c (r)) can be interpreted as involving a collection of charged and neutral nucleons. The requirement that changes in the nuclear coordinates only alter the CM momentum, in turn, and not lead to changes in the relative separations between charged particles, in the interior (bulk-like regions 10 ' 12 ) can lead to particular selection rules. In particular, in the early stages of the development of the IBS theory, we suggested an approximate selection rule: That the dominant d-d reactions involve changes in wave function through variations in nuclear coordinates (and potential nuclear reactions) not alter the wave function <&era(r) at locations

437

that are asymptotically far from the location of any possible NF overlap. In fact, in the more rigorous formulation, all possible forms of overlap become possible, and the comparable constraints need not apply except either near the GS or when the system is prepared appropriately. However, a generalized result also is appropriate: Eq. (1) still applies in the most coherent forms of reaction, provided the definitions of $ n u c (r) and <&EM(?") are generalized: As opposed to referring to the wave functions describing proton-neutron (p-n) pairs, in any particular reaction rate, the associated wave functions can be interpreted as describing the CM motion of collections of p-n pairs, or p-n pairs coupled to p's and/or n's, or, more generally, of collections of charged particles (p-n pairs, p-n pairs with p's or n's, or p-n pairs, with p's and/or n's and electrons). An important point is that although larger clusters of charged particles (in the relevant portions of a particular matrix element) can be viewed as generalized forms of quasiparticles, need not be forbidden, with increasing size, possible effects involving broken symmetry (through alternative forms of overlap in other matrix elements) become more likely and: The most coherent coupling involves simpler configurations, but these can cause greater degeneracy and greater instability. The key point is that the states that have the greatest overlap with the GS are required to not alter the relative coordinates between charged particles or clusters of particles in the regions (associated with EM interaction) far from the locations of nucleon overlap and NF interaction. From earlier arguments, 24 this more general context can be used to generalize the earlier selection rule. 14 ' 15 ' 22 The lowest energy excitations require that when &em(r) is a boson (i.e., its total spin is an integer multiple of h), $,iUC(r) is also a boson; and when <&em{r) is a fermion (i.e., when its total spin is an odd multiple of ft/2),
438

long that appreciable overlap with NF processes take place. In fact, whether or not a particular kind of reaction will take place involves a complicated reaction rate expression, based on a true many-body configuration. In particular limits, loss of symmetry and gauge symmetry (through broken gauge symmetry) can become important. But this certainly is not a requirement for LENR. 3. W h y Particular Nanoscale Crystals Turn-On Faster? In analyzing the possibility of transferring momentum rigidly from a nuclear reaction to the CM of a finite crystal lattice, without altering the energy of any of the particles in the lattice, I realized that a similar effect could be used to explain how an applied electric field E, potentially, could shift the momentum of many charged particles, at once, rigidly, without changing the relative separations between any of the particles. Limits of the associated picture can be quantified through a generalized form of multiple scattering 7 that I developed for the CF reaction problem. Applied to the £7-field problem, the argument generalizes the conventional Bloch (wave function), quasiparticle theory of electron conduction, 10 ' 12 based on energy band theory in infinitely-repeating, periodic lattices, to situations involving finite lattices involving charged particles (either electrons or hydrogen nuclei). In the new theory: (1) I generalized Bloch's theorem, to a many-body form; (2) the vague notion of transport phenomena involving quasiparticles is re-defined rigorously, through changes in the zeroes of energy for each set of indistinguishable particles; and (3) transport occurs through a change in the physical momentum involving each energy band state, which is a possible zero of energy, relative to the classical turning point of the kinetic energy. Here, reaction rates establish the relative time-scales of potential processes. The GS is required to have minimal overlap with states that are degenerate with it in the limit that far from the boundaries of the solid, a lattice exists, in which the net flux of particles into and away from the lattice vanishes. Since in the absence of accumulation of charge at the boundary, there is no way to distinguish the zero of energy of a particular many-body state from a second many-body state that is identical to it, except that it is moving, relative to it at a constant uniform velocity, a huge number of states can be degenerate with the GS as a result of implicit forms of invariance with respect to Galilean transformations (i.e., through Umklapp processes) that preserve particle-particle separation. As a consequence, Umklapp processes are defined uniquely and can provide large amounts of momentum coherently to the center-of-mass (CM). During the prolonged electrolysis of D2O by PdD a situation that mimics this limit can take place 9,10 ' 12,27 as a result of small fluctuations in loading (5 = ±0.03%) in finite PdDi +( 5 lattices. In finite PdDi +( 5 crystals, the associated loading-induced motion of Pd nuclei that results from these fluctuations has a small deuteron component that involves IBS occupation since each fluctuation extends throughout the solid and carries charge. In large lattices, the IBSs do not conduct appreciable ion charge because for all values of the wave-vector k, their energy e is the same:

439

e = e(jfc) = e (0).

(2)

W h e n Eq. (2) holds approximately, the collisions t h a t prevent coherent Umklapp processes are stifled, and the IBS effectively mimics the kind of state t h a t electrons occupy in an insulator. From this starting point, because collisions are stifled, it becomes possible for a phenomenon similar to Zener/Electronic breakdown 2 5 to take place, in which ions (as opposed to electrons) tunnel into a higher, conducting energy band state (an IBS), after a critical period of time. In this form of Zener/ionic breakdown, the tunneling time depends on crystal size. Crystals t h a t have characteristic dimensions smaller t h a n 6 nm, which have tunneling times microseconds, either are not capable of providing enough m o m e n t u m to create heat (through d + d —> 4 He) or conduct so rapidly t h a t collisions occur. Crystals with dimensions ~ 6 0 n m will create heat and load rapidly ( ~ 3 m s ) . But tunneling time scales by 1000 as t h e characteristic dimension increases by a factor of 10, a n d crystals with more t h a n ~ 6 0 fim have tunneling times t h a t are longer t h a n a month. This suggests t h a t the incubation times, observed in the experiments are the result of crystal size and (as suggested by A r a t a ' s results 2 6 , 2 7 ) t h a t nanoscale crystals turn-on considerably faster t h a n microscale crystals.

References 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15.

16. 17. 18. 19. 20. 21. 22. 23.

David Lindley, The embarrassment of cold fusion, Nature 344, 375 (1990). ICCF1 and ICCF2 were called ACCF1 and ACCF2. ICCF3 replaced ACCF3. G. Preparata, Editorial Note, in Proc. ICCF2 (see Ref. 2) (1991), p. 204 M.J. Puska et al, Phys. Rev. Lett. 51, 1081 (1983). C. Astaldi, A. Bianco, S. Modesti, S., et al, Phys Rev Lett. 8, 90 (1992). R.C. Casella, Phys. Rev. B 27, 5943 (1983). S.R. Chubb and T.A. Chubb, Proc. ICCF8 (2000), p. 385. S.R. Chubb and T.A. Chubb, Proc. ICCF9 (2002), p. 57. S.R. Chubb, Proc ICCF10 (2005), p. 735. S.R. Chubb, Spawar, T.R. 1862, Szpak et al. (eds.) vol. 3 (in press). I.H. Deutsch and P.S. Jessen, Phys. Rev. A 57, 1972 (1998). S.R. Chubb, http://arxiv.org/cond-mat/0512363. S.R. Chubb, Proc. ICCF11 p. 646 (2005) . S.R. Chubb and T.A. Chubb, Proc. ICCF1 (1990), p. 119. S.R. Chubb and T.A. Chubb, Lattice induced nuclear chemistry, in: S.E. Jones, F. Scaramuzzi, D. Worledge (eds.) Anomalous Nuclear Effects in Deuterium/Solid Systems, AIP Conference Proceedings 228 (AIP, New York. 1991), pp. 691-710. M.C.H. McKubre et al, Proc ICCF2 (1991), pp.419-444. B.F. Bush et al, J. Electroanal. Chem. 304, 271 (1991). T.A. Chubb, T.A. and S.R. Chubb, Fus. Tech. 20, 93 (1991). S.R. Chubb and T.A. Chubb, Really cold 'coldfusion', Proc ICCF7 (1998), p.78. S.R. and T.A. Chubb, NRL MR-6600, Naval Research Laboratory (1989). D.R. Thompson, Nucl. Phys. A154, 442 (1970). S.R. Chubb and T.A. Chubb, Fus. Tech. 24, 403 (1993). E. Storms, http://www.lenr-canr.org/acrobat/StormsEthenatureo.pdf

440

24. C.G. Beaudette, Excess Heat: Why Cold Fusion Research Prevailed (Oak Grove Press, Bristol, ME, 2002), pp. 365. 25. C. Zener, Proc. R. Soc. A145, 523-529 (1934). 26. Y. Arata and Y.-C. Zhang, Proc. ICCFIO (2005), p. 139. 27. Y. Arata and Y.-C. Zhang, Proc ICCF12 (in press).

MODELS FOR ANOMALIES IN CONDENSED MATTER DEUTERIDES

P E T E R L. H A G E L S T E I N Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA 02139 , USA and Spindletop Corporation, Mountain View, CA 94040 E-mail: [email protected]

Models based on phonon exchange for excess heat production in Fleischmann-Pons experiments are considered. In the case that sufficient phonon exchange occurs to stabilize intermediate states containing a neutral, then a model in which excitation is transferred from the D 2 / 4 H e system to a strongly coupled quantum system made up of an oscillator (highly excited phonon mode) and a Dicke system (ground state and excited state receiver nuclei) seem appropriate. We find that a coupled Dicke system and oscillator can support energy coupling in the case of strong coupling. We present evolution equations for resonant coupled Dicke systems, augmented with loss. An update is provided on phonon exchange in nuclear calculations.

1. Introduction In 1989 there were announcements made of observations of anomalies in metal deuterides: Fleischmann and Pons presented observations of an excess heat effect in PdD, 1 and Jones presented observations of low-level neutron emission in TiD. 2 Since then, considerable experimental and theoretical work has been reported on these and on other anomalies. As has been noted often over the years, the existence of any such effects would require a significant revision of our understanding of nuclear physics to explain. We have focused our efforts on the implications of these new experiments on theory, as well as on the development of models that may be relevant.3~5 In the nuclear physics literature, the predominant view is that nuclear fusion reactions that occur in condensed matter can be understood from idealized models in which the local environment is replaced by vacuum. The basic argument is that in order to react, nuclei must approach to within a few fermis, and the resulting reaction is completed with fast-moving well-separated product nuclei long before information concerning the reaction can reach neighboring atoms on an atomic scale. Such a picture cannot be relevant to the excess heat effect in Fleischmann-Pons type experiments, in which a large amount of energy (apparently of nuclear origin) appears and commensurate 4 He is detected. The experimental results are consistent with some new kind of reaction mechanism that acts as if 441

442

Do

n + 3He

Aj*

I

_>L.., 4 He

Macroscopic excited mode

Conversion \ of nuclear / energy to other modes

AZ

Figure 1. Scheme proposed for excess energy production. Molecular deuterium in condensed matter makes transitions to 4 He states through intermediate n + 3 H e states, with stabilization of the intermediate state through large angular momentum transfer associated with phonon exchange. The excitation is transferred to other species, which undergo fast phonon-mediated excitation transfer reactions among themselves, transferring energy to the excited phonon mode a few tens of phonons at a time.

d+d —> 4 He + 23.8 MeV (heat). In vacuum, two deuterons can react to produce 4 He. However, energy and momentum conservation requires the reaction energy to be carried off by an energetic gamma. No such gammas or other energetic particles are present in association with the Fleischmann-Pons excess heat effect. In our view this indicates that the lattice participates in the reaction in some way, and that vacuum models will not be relevant. Then, Our approach is based on including the lattice (or more generally, the condensed matter environment) in the initial formulation at the outset. 3 ~ 5 In such a formulation one finds that phonon exchange can occur during the fusion process. For conventional (incoherent) fusion reactions, the exchange of a phonon or two does not impact the fusion rate or products in a significant way, so that the predictions of vacuum models are preserved within the new formulation. The new model opens the door to a coupling between nuclear reactions that occur at different sites, as long as two or more phonons are exchanged at each site with a highly excited common phonon mode. In this case, there is the possibility of new second-order or higher-order quantum processes. We have discussed these ideas in some detail in our earlier ICCF conference papers, 3 ~ 5 to which the interested reader is referred. 2. Model for Excess Heat Production At present, we are considering a model for excess heat production that is illustrated schematically in Fig. 1. There are a number of ideas that are incorporated in this scheme. All transitions are mediated by phonon exchange (or by the exchange of similar quanta of a macroscopic condensed matter system that produces local

443

acceleration of nuclei). In order to couple to the lattice, all individual nuclear transitions must involve a neutral, such as n+ 3 He —> 4 He, so that the initial and final states appear to the lattice to have different mass (since the lattice does not see neutrals). In the case of AZ, the excited state (AZ)* is one in which there is a neutron or neutron cluster and a lower mass daughter with charge Z. Excitation is transferred from the D2/ 4 He system on the right to the receiver nuclei on the left. In our early work we focused on 4 He as a candidate receiver nucleus in this sense, but other nuclei such as Pd or other host lattice nuclei should be able to participate, with neutron-rich isotopes being able to couple more easily to the lattice. As in our earlier publications, we consider the initial fuel to consist of molecular D2 in condensed matter (we note that a similar scheme should be possible for HD). To analyze this kind of scheme, we require two different basic tools. On the one hand, we need to analyze the microscopic interactions between nucleons in order to understand phonon exchange and develop estimates for transition matrix elements. In addition, we would like to understand the structure of the intermediate n+ 3 He state, and the stability of excited neutral plus daughter states in general that are involved in the fast excitation transfer on the receiver side. On the other hand, we need models that are relevant to the many-site version of the problem. For example, we have discussed in previous papers that such models give rise to Dicke enhancement factors, and that tunneling in the coherent version of the problem appears through a rate linearly dependent on the Gamow factor, rather than through the square of the Gamow factor as in the case of incoherent transitions. In what follows, we will consider both problems.

3. Coupled Oscillator and Two-level Systems To address many site issues, we have been investigating models made up of two-level systems and an oscillator. The simplest example of a model that implements the ideas outlined above is given by H = ^ S « h z 2 +

+ ^ S ^ h z

JLs^(a + a^.

+ fiwoa^a + ^ e " G S « ( a + x h

a ^

(1)

In this model the D 2 / 4 He system is represented by the first set of two-level systems, under the assumption that sufficient phonon exchange is present to allow transitions through the n+ 3 He intermediate state with negligible loss. The D 2 and 4 He states are modeled as equivalent two-level systems (superscript I here), with transitions between these states represented with a hindered (by a tunneling factor e _ G ) transition involving the exchange of up to mi phonons. The receiver side nuclear states are also modeled as equivalent two-level systems (superscript 2) with unhindered transitions involving the exchange of up to m 2 phonons.

444

Coupled Dicke system and oscillator

»U

Q

Figure 2. In the limit that the receiver-side two-level systems are strongly coupled to the oscillator, then it is useful to think in terms of two-level systems coupled to a coupled oscillator and Dicke system hybrid.

3.1. Receiver

as Coupled

Two-level

System

and

Oscillator

In this model, the receiver-side system alone is composed of two-level systems that is strongly coupled to an oscillator. Since transitions involving the first set of two-level systems are weak, we can think of the system in terms of weak transitions from two-level systems (the D2/ 4 He systems) to a hybrid coupled oscillator and Dicke system. This is picture schematically in Fig. 2. If we adopt such a view, then we become interested in understanding the hybrid system. The receiver-side Hamiltonian is

Hr = ^-S™

3.2. Localization

+ hw0a)a + ™S™ (a +

tf)m>

(2)

Issues

The models under discussion are relatively complicated, and it is appropriate to make use of all tools available to gain understanding of how the models work. In the case of the coupled oscillator and Dicke system, there is an interesting and relevant limit that we need to consider. In the limit that the number of oscillator quanta is very large, and also that the number of excited states of the two-level system is also very large, then it is possible to develop analytic solutions. For simplicity, we focus on a version of the model with single phonon exchange (777-2 = 1), in which case the limit of the coupled oscillator and Dicke model approaches Hr - • AEM

+ fnuon + gAE^

+ <5™)(<5f + 6™).

(3)

445

This Hamiltonian has localized even eigenfunctions given by -M,n T

f

(M-M0+n-n0)/2

[~

J

2gAE A E + hLjQ

\ )

f J(M-M0-n+n0)/2 [~

0,

2gAE A E

_ ^

\

„

) >M + n

even

>

M + n odd. (4)

The associated eigenvalues are given by EMo,n0

= M0AE + n0fuj0.

(5)

Very similar eigenfunctions occur for M0 + n0 odd. One sees that in this limit, the coupled oscillator and Dicke system have a comb of eigenvalues spaced uniformly every HLOQ. 3.3. Static

Solutions

and

Derealization

We have an important analytic solution for the limit of the coupled model in which localized solutions occur. Specifically, this means that the system will develop fluctuations in n and M that are on the order of the coupling constant g. The coupling strength g is essentially the interaction matrix element divided by the transition energy. It can be on the general order of the number of receiver-side two-level systems (if we are able to arrange for half to be excited), since the underlying interaction strength per nucleus is probably on the order of a few MeV. Hence, the coupled system in this kind of model can be very strongly coupled, and fluctuations will be very large. For a net conversion of nuclear energy into phonon energy, simple fluctuations may not be helpful. We would like large numbers of oscillator quanta to be converted (probably more than g), not simply for the system to possess fluctuations. Consequently, we need to understand the connection between the eigenfunctions and the associated dynamics. For example, we would ideally like to see eigenfunctions that are localized around the constant energy line, and extend over large regions in (M, n) configuration space. Localized eigenfunctions represent the opposite. Some derealization can be obtained by working in a regime in which the coupling coefficients are not constant. For example, the time-independent Schrodinger equation for coupled two-level systems and oscillator can be written as

Ei>M,n

AEM

+ hio0n i>M,n + uU[S(S

+ 1) - M{M + l)](n + 1) 4>M+i,n+i

+ ^[S(S + 1) - M(M + l)]n V M + I , „

+ V[S(S + 1) - M(M - l)](n + 1) VM-i,n+i + y/[S(S + 1) - M(M - l ) ] n ^ M - l , n - l J-

(6)

446

30

c20 < 10

*

"-8

-

^

-

—

6

^

*

-

*

^

4

^

^

-

m

*

2

—

0

m

^

2

^

+

4

6

8

<M> Figure 3. Calculation of the spread in oscillator number A n (upper curves) and spread in Dicke number A M (lower curves) for the distinct even eigenfunctions with £ = 8, AE/fiwa = 15, and g = 1.5. A solitary point at M = 0 marks the analytic result for the localized Bessel function approximate eigenfunction.

In the large n limit, the coupling coefficients are nearly constant around M = 0, but they vary increasingly as one moves away from M = 0. Localized eigenfunctions are obtained near M = 0, but away the eigenfunctions become more delocalized. This is illustrated in Fig. 3 where we show the spread in oscillator number An as a function of the average Dicke number (M). Near M — 0, one sees that the spread in both n and M approach the constant g result, with minor deviations seen since the eigenfunctions extend slightly into regions where the coupling coefficient depends on M. Away from M = 0, one sees a significant spreading in n, which is an indication of derealization. The spread in M becomes reduced as the boundaries are approached. This result is interesting since it illustrates that if the local symmetry of the coupling constants is broken, that delocalization can result. Also, that the amount of delocalization is stronger the more that the symmetry is broken. However, the resulting eigenfunctions do not closely follow the constant energy line. For example, we illustrate in Fig. 4 a representative eigenfunction that is close to the M-boundary. One sees a relatively large spread in oscillator number. Such behavior is typical for coupled systems with a modest number of two-level systems.

3.4. System

Dynamics

We have done a significant number of simulations of the linearly coupled oscillator and Dicke model, from which some intuition has emerged. We see localized states

447

Figure 4. Example of eigenfunction for coupled two-level system and oscillator for large n limit. The vertical axis is the associated spin quantum number M, and the horizontal axis is relative oscillator number n = n - no-

that correspond to the analytic solutions discussed above, which are static. The coupled system is capable of large scale energy exchange between the two degrees of freedom, as is completely clear from the numerical results that we have seen (and is also completely clear from the literature on this kind of model). We can construct what amount to classical states of the system from a superposition of the eigenfunctions in the large n limit, and track the resulting dynamics (since wavepackets in the configuration space can keep their shape approximately). We see net motion that is oscillatory in the two dimensions, with wavepacket motion in M very roughly oscillatory with a frequency on the order of AE/li, and wavepacket motion in n with a frequency on the order of UIQ. We can understand the results in terms of simple notions of potential and kinetic energy in the (M, n) configuration space. In these simulations, the wavepacket moves from one position with an associated potential energy (AeM +frwoii),with the velocity of the wavepacket associated with the system kinetic energy. Hence, if the wavepacket follows a trajectory that goes between regions with different amounts of oscillator or Dicke excitation, because of the system kinetic energy the wavepacket. will shortly move on.

3.5. Slow

Dynamics

These complicated dynamics are interesting, but they do not correspond well to our intuition about how energy is transferred between the two degrees of freedom

448

in experiment. We seek slower dynamics in which the two-level system energy is transferred to the oscillator, which would correspond to eigenfunctions that lie along the constant energy line. We do not see such eigenfunctions in numerical simulations with a relatively small number of two-level systems, and modest integer ratio of oscillator energy to two-level system energy. If we tune the relative energies, we are able to match the eigenstate energies between neighboring eigenfunctions which differ in energy by one two-level system quantum. In this case, we observe a weak mixing which corresponds to a slow exchange between two-level and oscillator degrees of freedom. In the event that the associated coupling strength is on the order of the oscillator energy, we would expect to see free exchange of energy between the two systems at a maximum rate on the order of AEuo at threshold, and at higher rates for stronger coupling. Such a rate of energy transfer can be commensurate with experiment. It is also consistent with the energy exchange mechanism discussed in our ICCF11 proceedings, although the associated model would be more complicated. 4. Dynamics of Coupled Dicke Systems Based on the discussion above, we are motivated to consider a new kind of model to describe the dynamics of the D2 system and the coupled receiver system. If we assume that significant conversion of excitation on the receiver side to phonons is slow, then it seems productive to neglect it completely in order to develop a description of the excitation transfer dynamics associated with the populations. There is the question of resonance. On the one hand, there is no reason to expect there to be receiver nuclei transitions that are matched to the energy difference between D2 and 4 He. On the other hand, there is no excitation transfer between unmatched Dicke systems in the limit of hindered coupling and no phonon exchange. This sharply limits the possibilities. If the energy of the nuclear excitation is fixed and off of resonance, then the energy difference must be made up through phonon exchange in the strongly coupled oscillator and Dicke system on the receiver side. Alternatively, it may be the case that the nuclear excitation energy on the receiver side is determined by the energy involved in the excitation transfer. The argument in support of this is that one would expect the nuclei to have a very broad energy response (perhaps roughly proportional to the giant dipole response, but not the same since our excitation is not dipolar) under the conditions of excitation transfer. After all, if a quantum of energy is transferred, and if the nuclear system does not lose the energy, then it should be available for transferring back. Overall in this scenario the transfer process would create a precise resonance. From our perspective, either scenario is consistent in principle with the discussion which follows. There is a price to be paid, however, if the energy difference must be made up by phonon exchange. That price is a substantial reduction in efficiency, since it would be that the associated "oscillator strength" of the hybrid system must have a large energy spread.

449

4.1. Evolution

of Resonant

Coupled Dicke

Systems

Excitation transfer between resonant Dicke systems is governed by the Hamiltonian

H = — £ « + —S&

-e-G sPsW + sVs™

+

(7)

The development of evolution equations for expectation values of the pseudospin operators is nontrivial in the general case. We have had success developing an approximate Ehrenfest calculation by adopting a restricted basis composed of degenerate states. The results of the Ehrenfest analysis, augmented empirically with loss, results in the following coupled equations:

~ni(t)

= Vl(t),

d .. n2(t) ^n2(t) + - ^ i

,. = v2(t),

^jUi(t) + ^

= a(t),

d , . V2(t) -v2(t) + -^=

-ait),

(8)

(9)

where a

W =

p

{ [Nl ~ Mt)\[N2 ~ n2(t)][n2(t) - nx(t)] +ni{i)n2{t)[Nl

- ni(i) - N2 + n2(t)]

+ [Ni - rn{t)]n2{t) - [N2 - n2(t)]m(t)\.

(10)

Here n\{t) and n2(t) are the average number of excited states in system 1 (D2 side) and system 2 (receiver side), and v\{t) and v2{t) are the associated velocities. The acceleration is a{t). The Dicke number for the two sides are iVi and N2l which can be as large as the total number of nuclei involved on each side.

4.2.

Example

In Fig. 5 we show results from a numerical calculation of the evolution equations for resonantly coupled Dicke systems. In this calculation, we have assumed that there are 10 times more receiver side nuclei in the ground state than there are D2 molecules in the upper state. In addition, we have set the relaxation time to be matched to the coherent transfer rate. If we use a much slower relaxation time, then we observe population returning from the receiver side. If we use a much faster relaxation time, then we observe a slower net transfer of excitation. The problem in this case is that if the receiver-side nuclei decay rapidly, then there are relatively few around to provide a (receiver-side) Dicke enhancement of the acceleration. In essence, the fastest net energy generation rate is obtained when we match the excitation transfer rate with the receiver-side loss.

450

10

30

20 12

_G

(2A/1A/2) ' V e f / h b a r Figure 5. Calculation of normalized populations x(t) = ni(t)/Ni function of normalized time for conditions in which N2 = 10N±.

and y(t) = ri2(t)/N\

as a

5. Avoidance of Loss We have noted previously that the probability amplitude tends to avoid regions of high loss. A very much simplified version of this argument can be given. Consider the situation of two states that are coupled, one loss free and the other with high loss: d ih—co(t)

= flocoW + V&icift), .fill

Hi

ci(t) + Vi0co(t).

(11) (12)

We initialize the system such that c0(0) = 1, and ask what happens later on. The exact solution is more complicated than what we are interested in here; however, a useful simplification is allowed if we assume that the level 1 loss is very strong. In this case, CQ decays slowly as we will find, and we may assume that the a(t) probability amplitude is determined in the steady state by Cl (t)

E-

Hx+ih-a/2

VLO

c0(t)

(13)

with E approximately H0. The resulting evolution of level 0 is then

^

( t )

= W )

+

F&^

(14)

451

The effective loss seen by level 0 is then =

[Vbil2

'

n

,.

Increasing the level 1 loss 71 to ever larger values has the perhaps unexpected effect of decreasing the level 0 loss. In essence, the probability amplitude tends to avoid level 1 as it gets increasingly lossy. Alternatively, one can view this result as indicated that the maximum loss from level 0 is obtained when the loss is matched to the coherent transition rate.

6. Nuclear Models We have made progress on the other half of the problem which involves the calculation of the nuclear response in the presence of phonon-mediated excitation transfer. The calculation of phonon exchange matrix elements requires the inclusion of the nuclear center of mass coordinates as phonon operators. Results relevant to such calculations for the four-body problem is discussed in another paper submitted to this proceedings.6 We have in addition developed a new strategy for the calculation of the nuclear response which may be worth discussing briefly. The lattice generalization of the resonating group method that we have developed allows us to include phonon exchange explicitly in calculating nuclear interaction matrix elements. It seems that the most relevant and perhaps cleanest calculation which is needed is a second-order process in which an initial nuclear system receives energy via excitation transfer in a first phonon mediated strong force interaction, then evolves as a daughter plus neutral, and after a while makes a transition to a final state nuclear system. The basic interaction matrix element can be represented as

Mfl(E)

J2(^f(^f(^'---^A)\VN\^>mt[E-Hmt}-1

= int

x{*int\VN\MZu---,U)*i{
(16)

In the initial state, we see an internal nuclear wavefunction <&i(£i,..., £A), with £j as relative nucleon coordinates, embedded in a lattice (or condensed matter system) described by \Pj(q). Transitions are mediated by the strong force, described here by the nuclear potential Vjv- The intermediate internal nuclear wavefunctions for the different possible intermediate configurations are int • The lattice wavefunction in the intermediate state is implied through the specific bra and ket arrangements, but since there is a neutral involved in the intermediate state, the phonon modes of the lattice wavefunction are rotated through a Duschinsky transform (leading to intermediate wavefunctions of the form *i n t (A • q). Finally, the neutral and daughter come back together through the second potential interaction, producing

452

Y ; (q)0, &,...&)

/

\

Wf(q)Of

&,...,&

\

Yint(A-q, rn)Ointfe,...,y Figure 6. states.

Feynman-type diagram for matrix element involving intermediate lattice plus neutral

final state nuclear $ f ( £ i , . . . , £A) a n d lattice wavefunctions \&f (q). In this case, the phonon basis for the initial and final state lattice wavefunctions are locally the same, since there is no net mass change. There could be rearrangements in either the initial or final state systems, such as would occur if D2 or HT molecular systems are involved. However, when the nuclei are close enough to interact, the lattice will simply see four nucleons and two charges. This basic calculation is involved both in phonon-mediated transitions of the form D 2 —> n+ 3 He —> 4 He on the D 2 side, as well as AZ —> n m + A _ m Z —> A Z transitions on the receiver side. The matrix element can be represented by a Feynman-like diagram that is illustrated in Fig. 6. Implicit in the expression for the matrix element and also in the diagram is the point of view that the lattice (or condensed matter system) separates from a neutral (in association with an excitation transfer event), evolves as a daughter lattice plus neutral in the intermediate state, and then comes back together to form the final state lattice. Instead of a vacuum language that focuses on nuclei and nucleons, in the formulation under discussion, the interaction is with a nuclei which is part of a lattice, and it is helpful to think of it as a neutral plus lattice separation. Such a view makes plain what the calculation involves at the outset, and makes clear that it is in fact a fundamentally different calculation than what is involved in related vacuum calculations. 7. Summary We are moving toward viewing relevant models as involving the hindered coupling between a Dicke system for the D2/ 4 He side and a hybrid quantum system on the receiver side composed of one or more Dicke systems strongly coupled to one or more highly excited oscillators. In previous work, we have discussed the possibility that loss can break the symmetry of the coupled oscillator and Dicke Hamiltonian in order to allow the conversion of nuclear energy to phonon energy. Here we have shown that

453 the n a t u r a l boundaries associated with the Dicke system can accomplish the same basic function in a relevant strong coupling limit. Energy transfer between the Dicke system and the oscillator can occur naturally on timescales of the oscillator and two-level system generally in coupled Dicke oscillator systems. In strongly coupled systems in which the coupling strength between nearly degenerate eigenfunctions exceeds the oscillator energy, free energy exchange is expected. This corresponds to the situation we expect in the case of coupling between receiver nuclei and a highly excited acoustical phonon mode. It also is closely related to the coupling mechanism we discussed in the I C C F l l proceeding for a closely related model of two Dicke systems coupled to an oscillator with different coupling strengths in the classical limit. We presented the results of an Ehrenfest analysis of coupled resonant Dicke systems, augmented with loss to take into account energy coupling with the lattice in an empirical way. T h e resulting evolution equations should be relevant to the dynamics of fusion reactions under conditions where the D2 source is not replenished. Progress on the nuclear calculations was discussed briefly as well.

References 1. M. Fleischmann, S. Pons and M. Hawkins, J. Electroanal Chem. 201, 301 (1989); Errata, 263, 187 (1990). See also M. Fleischmann, S. Pons, M.W. Anderson, L.J. Li and M. Hawkins, J. Electroanal. Chem. 287, 293 (1990). 2. S.E. Jones, E.P. Palmer, J.B. Czirr, D.L. Decker, G.L. Jensen, J.M. Thorne, S.F. Taylor and J. Rafelski, "Observation of cold nuclear fusion in condensed matter," Nature 338 737 (1989). 3. P.L. Hagelstein, Proceedings of the Ninth International Conference on Cold Fusion, May 2002, Beijing, China, in: X.Z. Li (ed.), p. 121. 4. P.L. Hagelstein Proceedings of the Tenth International Conference on Cold Fusion, Aug. 2003, Cambridge, MA, in: P.L. Hagelstein and S.R. Chubb (eds), p. 837. 5. P.L. Hagelstein Proceedings of the Eleventh International Conference on Cold Fusion, Nov. 2004 Marseilles, France, in: J.P. Biberian (ed.), (in press). 6. I. Chaudhary and P.L. Hagelstein, this proceedings.

T I M E - D E P E N D E N T E Q P E T ANALYSIS OF TSC

AKITO TAKAHASHI1 Osaka

University,

Yarnadaoka 2-1, Suita, Osaka 565-0871, e-mail: [email protected]

Japan

Time-dependent fusion rates for 2D and 4D reactions are calculated for squeezing of tetrahedral symmetric condensate (TSC) from about 100 pm size to its minimum size (about 10 fm), within about 75 fs squeezing motion. Life time of the minimum TSC state is yet to be studied. Time-averaged fusion rates are given by assuming the life time of minimum TSC state is negligible. Time-averaged 2D fusion rate was given as 2 . 9 x l 0 ~ 2 6 f/s/pair, and time-averaged 4D fusion rate was 5 . 5 x l 0 - 8 f/s/cl. These values are compared with 1.0xl0~ 2 0 f/s/pair for 2D and 1.0 X 1 0 - 9 f/s/cl for 4D, respectively, of previously estimated values by electronic quasi-particle expansion theory/TSC m o d e l s . 1 _ 3 Effective fusion time by the TSC squeezing motion was estimated as 0.04 fs: namely fusions may happen in very short time interval.

1. Introduction For a consistent theoretical model of various condensed matter nuclear effects, namely clean 4 He producing fusion and cold transmutation, electronic quasi-particle expansion theory (EQPET)/tetrahedral symmetric condensate (TSC) models have been developed by the author. 1_4 Transient motion of TSC by four deuterons plus four electrons has been treated with a primitive approximation using the linear combination (EQPET) of wave-functions for pseudo-molecular states of d-d pairs with normal electrons and quasi-particle-electron states e*(2,2) and e*(4,4) as steadystate solutions for narrow time-window. This was a model for "bosonized condensate" of squeezed mode, which can be treated as a kind of steady state in very narrow time-window of squeezed motion. Since the barrier factor changes drastically with astrophysical orders according to the assumed pseudo-molecular states, numerical studies based on time-dependent treatment are expected to know more accurate values of fusion rates of multi-body deuteron interactions in the transient process. This work reports a trial study of time-dependent EQPET analysis for TSC squeezing motion to estimate time-averaged fusion rates of 4D/TSC.

tSubmitted to ICCF12, November 2005. 454

455

2. E Q P E T Model Starting with the formation of TSC state (t = 0) with six-wings wave function which is composed of six dde* molecular wave functions with six orthogonal single spin wave functions, time-dependent screening potentials are adiabatically approximated with pseudo-molecular potentials for ddee, dde* (2,2) and dde*(4,4) according to the change of mean d-d distance i?dd- Semi-classical treatment is done for the timedependent reduction of mean d-d distance. Using this algorithm, a computer code is made.

4re = 4x2.8 fm

(2) Minimum TSC

(1) TSC forms Electron

r~\

<8>

<$>

> 4

4

He

He

Deutron 15fm

(3) 8 Be* formation Figure 1.

(4)

Break U

P

Four steps for TSC squeezing motion and 4D fusion.

The semi-classical feature of TSC squeezing motion is illustrated as four steps in Fig. 1. In Fig. 1, TSC will form in the near surface region of condensed matter by the mechanism (A) or mechanism (B) as discussed in Refs. 2 and 3, with certain probability depending on methods of experiments and near-surface physics of condensed matter. Step 1 (TSC forms). Then TSC starts Newtonian squeezing motion to decrease linearly its size from about 100 pm radius size to much smaller size and reaches at the minimum size state. Step 2 (minimum TSC). Classical squeezing motion ends when four deuterons get into the strong force range (5fm) and/or when four electrons get to the Pauli's limit (about 5.6fm for e-e distance). Here for

456

the Pauli's limit, we used the classical electron radius of 2.8 fm. In Step 3, mutual charged-pion exchange between four deuterons forms 8 Be* intermediate compound state with much smaller radius and the charge neutrality in average of 4D/TSC is broken simultaneously to kick out four electrons. In Step 4, 8 Be* which is collectively deformed with two alpha-clusters promptly breaks up to two 4 He particles. The initial state TSC wave function, when TSC is just formed at t = 0, can be written using combination of six wings of D2 molecule wave functions on six surfaces of the TSC cube, as illustrated in Fig. 2. Here, the wave function of D2 molecule is written with combination of two 1 S wave functions \&ioo of hydrogen atom, as also illustrated in Fig. 2. This feature is obtained by assuming the TSC wave function to be the following Eq. (1) and using the three-dimensional symmetric constraint of TSC squeezing motion in applying the quantum mechanical variational principle of minimizing system energy. The new aspect of the problem is that we are treating "bosonized condensate" of TSC under the environment of ordered dynamic motion (in other words, symmetrically constrained squeezing motion) in the lattice of PdDx condensed matter. *4D ~ ai[^ r 100(''Al)*100(''B2) + *10o(r - A2)*10o(r 1 Bl)]^"s(5'l, 5 2 ) + a2[*100(^Al)*100(^D4) + *10o(rA4)*10o(n3l)]-Xs(£i,S4) + a3[*100(»,A2)*100(»,C4) + *100(jA4) , I'l00(7C2)]^s(S , 2, S4) + a 4 [*100(»'Bl)*100(rD3) + *100(?~B3)*100(>'Dl)]^s(<Sl,S'3)

+ a5[*ioo(^B2)*ioo(»'C3) + ^ioo(rB3)^ioo(rG2)]Xs(S2, + a 6 [*ioo(rc3)*ioo(r D 4) + ^wo{rc4)^wo(rD3)}Xs(S3,Si)

S3) (1)

and the 1-s electron wave function for deuterium atom is given by, *ioo(r) = ( l A ) 1 / 2 ( l / a B ) 3 / 2 e x p ( - r / a B ) .

(2)

Here subscripts A-D denote positions of deuterons at vertexes of cube. And subscripts 1-4 denote positions of four electrons. XS(S{, Sj) is singlet spin wave function for bosonized (anti-parallel spins) pair of electrons. Bohr radius ae is 52.9 pm. Coefficients a\-a% are vectors on six surfaces of the cube, and are usually determined by the variational method to minimize system energy as, <S{<*4D|ff|*4D>/<*4D|tf4D>} = 0.

(3)

Since the solution of Eq. (3), with partial derivatives for coefficients a\-a§, gives sixth order (18th order in exact, taking three-dimensional components of vector aj) secular equation which cannot be solved uniquely. However, the requirement of ordered squeezing, namely the three-dimensionally symmetric constraint of TSC motion in PdDx lattice, gives constraints as,

Kl = Kl = M = M = \a5\ = \a6\ = a0 with a0 = 1/(6(1 + A)) 1 / 2 .

(4)

457

Feature of QM electron cloud Electron center; <e> = (et + ie)/2

RB = 53 pm

• Bohr orbit of D (H)

Deutron

(a) D atom (stable) Bosonized electron center torus for (et + 4e)

y - i^m. *^ y

v_y

Orbit of bosonized electron coupling for (et + ie)

/

(c) 4D/TSC (life time about 60 fs) 73 pm (b) D2 molecule (stable): V 2 D = (2+2Ar 1/2 [ Vl00 (r A1 ) ¥ioo(%z) + Vioot'Aa) ¥IOO('BI)]^S(SI. S2) Figure 2. Features of QM electron clouds for (a) D atom, (b) D2 molecule, and (c) 4D/TSC at t = 0. Bosonized electron center torus of D 2 molecule is a unit of bond for orbits of bosonized electron coupling of TSC (t = 0).

And we have orthogonal conditions between a4 for i = 1-6. aiaj=%.

(5)

We can say that the platonic polyhedral symmetry in constraint motion gives special solution for the variational analysis of so-many-body problem. Thus the TSC wave function at t = 0 has six symmetric wings of modified D 2 wave functions as illustrated in (c) of Fig. 2. D 2 wave function has a torus of electron higher density for singlet (anti-parallel) spin pairs of electrons. Superposition of "wings" at vertexes of the cube make four balls of high density electron clouds at tetrahedral four vertexes of cube as illustrated in Fig. 2c. An electron ball at vertex can be therefore treated as an effective electron center for (e) = ( e | + e|)/2. In Fig. 1, we have drawn effective electron center as classical electron particle with spin. 3. Time-Dependent E Q P E T Analysis The basic equation of time-dependent EQPET is written as *4D(r, t)at = a i ( t ) * ( l , l)(r, t) + o 2 (t)*(2,2)(r, t) + a 4 (t)¥(4,4)(r, t),

(6)

(r(t)) = - (v)t,

(7)

458

M*)} = <*:DM)M*4DM)>,

(8)

(r(0)) = (3 1 / 2 /2)a B = 45.8 pm.

(9)

Here we assumed that the time-dependent 4D/TSC wave function ^4u(r,t) can be expanded with the linear combination of time-dependent wave functions * ( l , l ) ( r , £ ) , #(2,2)(r,t), and *(4,4)(r,i) of EQPET molecules1-4 dde(l, l)e(l, 1), dde*(2,2) and dde*(4,4), respectively. Eq. (7) assumes classical Newtonian motion treatment for averaged particle position with strong constraint of same velocity due to keeping charge neutrality (system Coulomb energy to be minimum) in TSC squeezing motion. Modal fusion rate 5 for 4D cluster is given as A„d(*) = ai(t) 2 A„ d (l, l)(t) + a 2 (i) 2 A„ d (2,2)(t) + a 4 (t) 2 A„ d (4,4)(i).

(10)

Here we take n = 2-4 for 4D/TSC cluster fusion rates. Fusion rates for an EQPET molecule are given by Xnd{m,Z)(t)

= (vSnd/Ed)Pnd(Ed,t).

(11)

Here v is the relative deuteron velocity, Snd the astrophysical S-value (intrinsic cross-section term for strong interaction) for multi-body fusion and Ed the relative deuteron energy, respectively. Also we define the time-dependent barrier penetration probability Pnd(Ed,t) as follows: Pnd(Ed,t)=exp(~nr{t)),

(12)

T{t) = 0.218 / y/Vs(Rdd) - Ed dRdd (in MeV and fm unit). (13) Jr0 Here Rdd is the inter-nuclear distance between two deuterons. For evaluating the time-dependent Gamow integral Eq. (13), we employed the adiabatic approximation for time-dependent potentials for EQPET molecules using three steady-state potentials 6 Vs(Rdd) for (1,1), (2,2), and (4,4) state-electron couplings. Major parameters of EQPET molecule potentials are shown in Table 1. The algorithm of adiabatic treatment is as follows: b{t) = Rdd(t) = bo(m,Z)

forVs-Ed>0 forVs-~Ed<0.

(14) (15)

Constraints are: &min = &o(2,2)=4pm forZ = 14, 6min = fro(4,4) = 0.36 pm

for Z = 2.

(16) (17)

Constraints Eqs. (16) and (17) mean that we switched EQPET potential from V s (l,l) to T4(2,2) at bmin = 4pm, and from Vs(2,2) to Vs(4,4) at 6 min = 0.36pm. So, this step-wise treatment of time-dependent potentials is a primitive adiabatic approximation.

459 Table 1. Major parameters for E Q P E T molecule potentials; Here VSmin is the depth of trapping potential well, bo is the d-d distance value at which potential crosses over zero-value and .Rdd(gs) the d-d distance for ground state dde* molecule, respectively Parameters of dde* potentials e*(m, Z)

Vsmin (eV)

bo(pm)

(1,1) (1,1) x 2 ; D 2 (2,2) (4,4)

-15.4 -37.8 -259.0 -2,460

40 20 4 0.36

Trapping depth

-Rdd(gs) (pm) 101 73 33.8 15.1 Ground state

4. Results and Discussions A computer code was programmed based on the above procedure, and numerical calculations were done to obtain cluster fusion rates for EQPET molecules. To estimate modal fusion rate, we assumed in this work that (Zj-values are constants as: ai(t)2 = a i ( 0 ) 2 =0.782, a2{tf = a 2 (0) 2 = 0.187, a 4 (t) 2 = a 4 (0) 2 = 0.031. Here, combination probabilities 6 for parallel and anti-parallel spins of pairing electrons are only taken into consideration, in this work. Here we assumed (v) = 1 x 105 cm/s corresponding to E& = 0.22 eV which is the highest phonon energy of D-harmonic oscillator6 in PdDx Bloch potentials. As shown in Fig. 3, 2D fusion rate increases from 1 x 1 0 - 6 0 f/s/pair at t = 0, the value of which is the same fusion rate of D2 molecule, to enhanced one of 1 x 10~ 42 f/s/pair at turning point. 2D fusion rate further increases to 1 x 10~ 22 f/s/pair at the turning point to the (4,4) quasi-electron coupling state, by transition to the e*(2,2) state, Cooper pair, formation of electron pairs of antiparallel spins. 4D fusion rate at final stage reaches to the order of 1 x 10~ 4 f/s/cl. Minimum-size state with about 10 fm diameter of TSC is attained in 73 fs. So, this is very rapid squeezing motion. 4D fusion rate at TSC-minimum-size is given as 2.3 x 10~ 4 f/s/cl. We do not accurately know the life time of TSC-minimum-size. We need further study taking into account of quantum mechanical fluctuation of TSC squeezing motion to get information on the life time. Here we can only argue that maximum life time of TSC-minimum-size is about 72min (so long!) if nuclear strong interaction (4D fusion) is the only cause to break charge neutrality of TSCminimum-size according to the fusion rate of 2.3 x 1 0 - 4 f/s/cl as calculated. This 4D fusion rate is very large as 2 x 10 18 f/s/cc (about 20MW/cm 3 of PdDx) if TSC density of 1 x 1022 cl/cm 3 were realized in experiment. Time-averaged fusion rates are shown in Table 2. In our previous study, 1_6 we have given 2D fusion rate as 1 x 10~ 20 f/s/pair ands 4D fusion rate as 1 x 10~ 9 f/s/cl, by the treatment of steady squeezed mode.

460

Time-dependent EQPET calculation forTSC: comparison of X 2d (1,1) (f), X 2d (2,2) (f), and X 4d (4,4) (f)

?

60 50 -o E

40

CO

-Ram da2d (1,1)

- Ram da2d (2,2)

CC

ra

30

_o

«d^^

I

20

•^s^aS^ass -

Ram da4d (4,4)

10 0 0.01

1

(RM (/)> (pm) Time (fs) 72.98

Figure 3.

72.9

Calculated time-dependent cluster fusion rates for TSC squeezing motion.

We found time-averaged 2D fusion rate 2.9 x 10~ 25 f/s/pair is about five orders of magnitude smaller than the steady squeezed mode analysis, but time-averaged 4D-fusion rate 5.5 x 10" 8 f/s/cl is rather closer value. Of course we should prefer values by the present time-dependent analysis. 5. Conclusions 1. Simplified trial of time-dependent analysis on TSC was made. 2. TDEQPET (time-dependent code) gave several orders of magnitude different fusion rates from those by EQPET (Squeezed Mode Model). 3. 4D fusion takes place in 0.04 fs effective reaction time: It is very impulsive. 4. TSC as bosonized condensate has been proposed as SEED of Condensed Matter Nuclear Effects to induce clean 4D fusion. Table 2. Time-averaged modal fusion rates and initial fusion rates for 4D/TSC squeezing motion, calculated by T D E Q P E T code T D E Q P E T calculation for E Q P E T molecules

e*(m,Z)

(A2d) (f/s/cl.)

(A4d) (f/s/cl.)

A2d(0) (f/s/cl.)

A4d(0) (f/s/cl.)

(1,1) (2,2) (4,4)

4.3 x 1 0 " 4 4 2.9 x 1 0 " 2 5 (2.1 x lO" 17 ) 1 "

7.8 x l O - 6 3 2.5 x 1 0 - 2 4 5.5 x 1 0 " 8

1.9 x 1 0 - 6 0 2.4 x 1 0 - 3 7 (5.5 x l O - 2 2 ) !

7.3 x 1 0 ~ 9 3 1.1 x 1 0 " 5 0 5.9 x l O " 2 0

t Virtual value.

461

References 1. A. Takahashi, Deuteron cluster fusion and related nuclear reactions in metaldeuterium/hydrogen systems, Recent Research Developments in Physics, Transworld Research Network, India, 6, 1-28 (2005), ISBN = 81-7895-171-1. 2. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Siena Workshop on Anomalies in D/H loaded metals, Siena, Italy, 13-16 May (2005), http://www.iscmns.org/. 3. A. Takahashi, A theoretical summary of condensed matter nuclear effects, ibid. 4. A. Takahashi, Condensed Matter Nuclear Effects, Proc. IMFP2005, Int. Meet. Frontiers Physics, 25-29 July (2005), Kuala Lumpur, Malays. J. Phys., to be published. 5. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Condensed Matter Nuclear Science, Proc. ICCF10, World Scientific Publ. Co., pp. 809-818 (2006), http://www.lenr-canr.org/. 6. A. Takahashi, Drastic enhancement of deuteron cluster fusion by transient electronic quasi-particle screening, Proc. JCF4, pp. 74-78, A. Takahashi, Deuteron cluster fusion and ash, Proc. Asti Workshop (2004) http://www.iscmns.org/.

U N I F Y I N G T H E O R Y OF L O W - E N E R G Y N U C L E A R R E A C T I O N A N D T R A N S M U T A T I O N PROCESSES IN D E U T E R A T E D / H Y D R O G E N A T E D METALS, ACOUSTIC CAVITATION, GLOW DISCHARGE, A N D D E U T E R O N BEAM EXPERIMENTS Y E O N G E. K I M A N D A L E X A N D E R L. Z U B A R E V Department E-mail:

of Physics, Purdue University, 525 Northwestern Avenue, West Lafayette, IN 47907, USA [email protected]; [email protected]

The most basic theoretical challenge for understanding low-energy nuclear reaction (LENR) and transmutation reaction (LETR) in condensed matters is to find mechanisms by which the large Coulomb barrier between fusing nuclei can be overcome. A unifying theory of LENR and LETR has been developed to provide possible mechanisms for the LENR and LETR processes in matters based on high-density nano-scale and micro-scale quantum plasmas. It is shown that recently developed theoretical models based on Bose-Einstein Fusion (BEF) mechanism and Quantum Plasma Nuclear Fusion (QPNF) mechanism are applicable to the results of many different types of LENR and LETR experiments.

1. Introduction There have been many reports of experimental evidences for low-energy nuclear reaction (LENR) processes in condensed matters as documented in a recent document submitted for a DOE review1 and as reported in Proceedings of ICCF-10. 2 However, most of experimental results cannot be reproduced on demand. This situation has prevented us from development of a coherent theoretical understanding or working theoretical model of the phenomenon which can be used to guide us in designing and carrying out new experimental tests to sort out essential parameters and controls needed to achieve reproducibility on demand (ROD). In this paper, it is shown that recently developed theoretical model based on Bose-Einstein Fusion (BEF) mechanism and Quantum Plasma Nuclear Fusion (QPNF) mechanism are applicable to the results of many different types of LENR and transmutation experiments. Both the BEF and the QPNF mechanisms are based on a same physical model, which assumes that deuterium/hydrogen is in a plasma* state and is mobile in a deuterated/hydrogenated metal as deuteron/proton ion.t *In this paper, we use a general definition of "plasma" as given in the report: National Research Council, "Plasma Science", National Academic Press, Washington DC (1995), p. 1, "Plasma science is the study of the ionized states of matter". * Experimental evidences for the ionization and mobility of deuteron/proton in metal are given in Refs. 14-16. 462

463

Theoretical studies of BEF mechanism have been carried out using an approximate solution to the many-body Schroedinger equation for a system of N identical charged, integer-spin nuclei ("Bose" nuclei) confined in micro- and nano-scale cavities. 3-6 The ground-state (superfluidity state) solution is used to obtain theoretical formulae for estimating the probabilities and rates of nuclear fusion for N identical Bose nuclei confined in a ion trap or an atomic cluster. Most recently, we have investigated the effect of a generalized particle momentum distribution derived by Galitskii and Yakimets (GY) 7 on nuclear reaction rates in plasma. 8 ' 9 We have derived an approximate semi-analytical formula for nuclear fusion reaction rate between nuclei in a plasma. The formula is applied to calculate deuteron-deuteron fusion rate in a plasma, and the results are compared with the calculated results of the conventional Maxwell-Boltzmann (MB) velocity distribution. As an application, we investigate the deuteron-deuteron fusion rate for mobile deuterons in a deuterated metal/alloy. The calculated deuteron-deuteron fusion rates at low energies are enormously enhanced due to the modified tail of the GY's generalized momentum distribution. Our preliminary estimates indicate also that the deuteron-lithium (D + Li) fusion rate, the proton-boron (p+B) fusion rate, and the proton-lithium (p + Li) fusion rate in a metal/alloy at ambient temperatures are also substantially enhanced due to this QPNF mechanism. Implications of our results and other potential applications are discussed. 2. Bose-Einstein Fusion (BEF) Theoretical studies of the BEF mechanism are described in publications 3-6. One of the main predictions is that the Coulomb interaction between two charged bosons may be suppressed for the large N case and hence the conventional Gamow factor may be absent. The theory has been used to analyze LENR experiments involving both atomic clusters (Pd black powders 10 ) and acoustic cavitations. 11 Recently, the one-specie LENR theory of the BEF mechanism 3-6 used for reactions such as (D+D) has been generalized to the two-species case and applied to (D + Li) reactions. 12 The only unknown parameter of the theory is the probability of the BE groundstate occupation, ft. Since, ft is expected to increase as the effective temperature of the BE state (superfluidity state) decreases, the nuclear reaction rates for the BEF mechanism are expected to increase at lower temperatures. 3. Quantum Plasma Nuclear Fusion As shown by Galitskii and Yakimets (GY), 7 the quantum energy indeterminacy due to interactions between particles in a plasma leads to a generalized momentum distribution which has a high-energy momentum distribution tail diminishing as an inverse eighth power of the momentum, instead of the conventional MB distribution tail decaying exponentially. GY's generalized momentum distribution has been used by Coraddu et al.13 in an analysis of anomalous cross-sections for D(d,p) 3 H observed from the low-energy deuteron beam experiments.

464

In this section, we describe a QPNF mechanism, which includes the effect of GY's generalized momentum distribution on the nuclear fusion rates in a plasma. 8 ' 9 The calculated results based on the QPNF mechanism for deuteron-deuteron fusion rates are compared with the results of the conventional calculation with MB distribution. As applications of the QPNF mechanism, we investigate other nuclear fusion rates for (D + Li), (p + Li), and (p + B) reactions in metals/alloys. 3.1. Reaction

Rates for Quantum

Plasma

Nuclear

Fusion

To formulate the QPNF mechanism we start with GY's generalized distribution function given by f(E,p)=n(E)S1(E-ep),

(1)

where n(E) is MB, Fermi-Dirac (FD), or Bose-Einstein (BE) distribution, modified by the quantum broadening of the momentum-energy dispersion relation, 57(E — e p ), due to particle interactions. 51(E — ep) is given by

^

£p)

{Z)

-irl(E-Sp-A(E,p)y+1i(E,p)Y

where e p = p2/2/x is the kinetic energy in the center of mass coordinate of an interacting pair of particles, u is the reduced mass, A(E,p) is the energy shift due to the interaction (screening energy, etc.), and j(E,p) is the line width of the momentum-energy dispersion due to collision. ^{E^p) RJ hpcac^2E/n, where pc is ( 2 2 2 the number density of Coulomb scattering centers (nuclei), ac = Tr(ZfZ je ) /s is the Coulomb scattering cross section, and Zfe is an effective charge which depends on e p . For small values of e p , Zf is expected to be much smaller than Z*, Zf 0 and 7 ->• 0, S1(E-ep)

= S(E-sp).

(3)

The nuclear fusion rate for two nuclei is given by (
depvTel(j{Ecm)f(p),

(4)

where / ( p ) » / dEn(E)67(E-ep), Jo and the normalization N is given by

NJd£pf(p)

(5)

= l.

(6)

For a high-energy region, e p 3> kT, 7 and A we obtain approximately /(fl«l

fn(E)1(E,p)dE

= rJ81^Pc{Z!Zle2)2 7T^ '

j

£4

ocl, po

(7)

465

as shown by GY. 7 This is to be compared with the other conventional cases, f(p) oc e~ £p / fcT . We now derive an approximate analytical formula for obtaining order-ofmagnitude estimate for the nuclear fusion rate. The total nuclear fusion rate, R^, per unit volume (cm - 3 ) and per unit time (s _ 1 ) is obtained from an expansion of Eq. (2) in which the first term is S(E — e p ). R^ is approximately given by Rij « Rtj + Rtj,

(8)

where i?£ is the conventional fusion rate calculated with the MB distribution and i O is the contribution from the second term of the expansion of Eq. (2) and is given by

Gr

where EQ is the Gamow energy, EQ = (2-KaZiZj)2/j,c2/2, p± is the number density of nuclei, and S'ij(O) is the S'-factor at zero energy for a fusion reaction between i and j nuclei. We note that the spectral function 5-y{E — ep) (Eq. 2) introduced by GY 7 needs to be modified to satisfy the following energy weighted sum rule (for fermions),

jMES^E-eJ-^-JW^M,

(10)

where f(p) is the distribution function, given by Eq. (5). Since the integral on the left-hand side of Eq. (10) is a divergent integral, the GY parameterization of ~f(E,p) in 81(E — ep) needed to be corrected for large £ >fcTto satisfy the above sum rule. However, Eqs. (4-9) are still valid since our results for the distribution function f(p) do not depend on j(E,p) in the region where E 3> kT due to the presence of n(E) oc e~E/kT in Eq. (5). 3.2. (D + D) Reactions

in a Plasma

The importance of Eq. (9) is that it distinguishes high density/low temperature plasmas in condensed matter systems from low density/high temperature plasmas produced in magnetic confinement plasma fusion or inertial confinement laser fusion by breaking the contribution of fusion reactions into the MB and the QPNF processes. To access the importance of each, it is useful to investigate the cross section times the velocity averaged over the velocity distribution or fusion reactivity (av), given by Eq. (9), as a function temperature. In Fig. 1, the calculated fusion reactivities, (o~v), are plotted as a function of temperature kT. There are two density regions of interest; the hydrides in metals shown as the solid line in the figure and the tokamak break-even density shown as the dotted line in the figure. The fusion reactivity of a MB distribution is independent of density and is shown in the figure as a dashed line. The intersections of the dashed curve and the solid or dotted curves provide values of critical temperature T cr ,

466

10- 27

—

-'—

-—v.-f

_

Condensed matter p QPNF-theory

10-29

/ / I I I i

b

icr 33

•S co

10-35

c

1(T

Tokamak p-goal QPNF-theory

?

' j

/

I

, * m <* *

^T

^ J^ Ja » w * "*

10 4 1 10"

43

' 0.01

i

* * * * * * *

-**** Maxwell-Boltzmann ' theory ^ ' p-independent ..... I 0.1 1 10 _ j. « « » ™

X;

100

Temperature (eV) Figure 1. Fusion reactivity, (crv), of D(d,p) 3 H reaction in units of c m 3 / s as a function of temperature kT in units of eV. The dashed line, the solid line, and the dotted line corresponds the results calculated using the MB distribution, the GY distribution with p = 10 c m - 3 , and the GY distribution with p = 10 1 5 c m - 3 , respectively.

when the fusion rate is equal for MB and the QPNF processes. This comparison shows that quantum effects are important at low temperatures even for the DebyeHiickel plasma, p
Plasma

Plasmas created in glow discharge experiments are known to have temperatures ranging from 104 to 5 x 105 K (kT ~ 0.8-40 eV) with densities p « 10 7 -10 14 cm" 3 . As can be seen from Fig. 1, if the density of glow discharge plasmas can be increased to p > 1014 cm~ 3 , glow discharge experiments can become ideal testing and probing grounds for the QPNF mechanism.

467

4. Nuclear Reactions in Metals/Alloys One of the other potential applications of the QPNF is the nuclear fusion rates in metals. Hydrogen (or deuterium) molecules in Palladium are known to be dissociated into atoms and ionized to bare nuclei.14 The mobility of protons and deuterons in Pd and other metals has been experimentally demonstrated. 15 ' 16 However, other heavier nuclei (Li, B, etc.) are most likely to have much less mobility and most of them are stationary in metal/alloy lattices. Because of the deuteron mobility in metals, (D + D) fusion rates in metals were investigated using the MB velocity distribution for deuterons with a hope that the high-energy tail of the MB distribution may increase the (D + D) fusion rates in metals. 17~19 However, the calculated results for the (D + D) fusion rates with the MB distribution were found to be extremely small at ambient temperatures. 17~19 given by Eq. (9) covers three different cases: (a) Nuclei i and j are the same specie and mobile in a plasma with a GY velocity distribution (For example i and j are both deuterons yielding the (D + D) fusion reaction rate). (b) Nuclei i and j are two different species and both mobile in a mixed twospecies plasma with velocity distributions (For example i is for protons and j is for deuterons yielding the (p + D) fusion reaction). (c) Nucleus i is mobile and from a single-specie plasma with a velocity distribution, but nucleus j is stationary and imbedded in a metal/alloy matrix. Nuclei i and j are the same specie (For example i and j are both protons or both deuterons or nuclei i and j are two different species yielding (D + Li), (p + Li), and (p + B) fusion reactions). 4.1. Deuteron

Beam Experiments

with Deuterated

Metal

Targets

Recent results of cross-section measurements from deuteron beam experiments with metal targets by Kasagi et al.20 and Rolf et al.21 indicate that the QPNF mechanism may be occurring. Recently, Rolf et al.21 have investigated the electron screening effect in the D(d,p) 3 H reaction with a low energy (center-of-mass energies between ~ 4 and ~ 15 keV) deuteron beam on deuterated targets (32 metals, three insulators, three semiconductors, three groups 3 and 4 elements, 13 lanthanides). They have found that all deuterated metals yield large extracted values of the screening energy Ue ranging from Ue = 180 ± 40 eV (Be) to Ue = 800± 90 eV (Pd), while all deuterated non-metal targets yield smaller values of Ue < 80 eV. If we interpret the anomalous values of Ue for metal targets in terms of the QPNF mechanism, wide variations of 32 different values of Ue ranging from Ue = 180± 40 eV (Be) to Ue = 800± 90 eV (Pd) may be correlated with the number density of mobile deuterons in metal targets which in turn may be related to deuteron loading ratios, deuteron diffusion coefficients in metals, external stimulations, etc., such as applied electromagnetic fields.

468

4.2. (D + D) and (D + Li) Reactions Metals/Alloys

at Ambient

Temperatures

in

For the case of (D + D) fusion reaction, order-of-magnitude estimates for i?rj D are shown as a function of the mobile deuteron density p in Table 1 calculated from Eq. (9) with Sij{0) = 110 keV-barn for both D(d,p) 3 H and D(d,n) 3 He reactions combined. The mobile deuteron density of p = 6 x 1022 cm~ 3 is probably an upper limit of the maximum density achievable in deuterated metals/alloys. To grasp the significance of the results for R^v m Table 1, they need to be compared to the DD fusion rate, -R§ D , calculated utilizing the MB distribution. 17-19 The calculated values 17-19 for i?§ D depend on both p and the electron screening energy. Taking p = 6 x 1022 c m - 3 the results yield i?§ D ~ 10~ 73 cm" 3 s" 1 when a conventional electron screening energy of Es = e2/ao ~ 27 eV (ao is the Bohr radius) is used. These results improve to i?§ D ~ 10~ 31 c m - 3 s _ 1 if Es = 4e 2 /a 0 « 109 eV is used, which is at the extreme limit o.f what an acceptable for Es might be. Both estimates should be compared with R^B « 0.4 x 10 15 c m - 3 s _ 1 given in Table 1. Table 1. Order-of-magnitude estimates for DD fusion rate, i?jj D , in units of c m - 3 s - 1 . The particle (mobile deuterons) number density, p is in units of 6 X 10 22 c m - 3 . Zf = Zj = 1, Ze- = Zj = 1, pc = pi = Pj = p, and kT = 0.02 eV are assumed P (6 x 10 22 c m " 3 )

i?§D (cm"3 s-1)

10"4 HT3 10"2 10"1 1

0.19 0.33 0.39 0.42 0.43

x x x x x

10 3 10 6 10 9 10 1 2 10 1 5

Power ( W / c m 3 ) 0.1 x 1 0 " 9 0.20 x 10~ 6 0.23 x 10~ 3 0.25 0.25 x 10 3

Our results of surprisingly large fusion rates for the DD fusion reaction in a deuterated metal/alloy at ambient temperatures may offer a sound, conventional theoretical explanation for most of the nuclear emissions results reported from the previous LENR experiments. 22 Given similar conditions as for the DD fusion, the fusion rate for the D 6 Li fusion reaction is estimated to be ~10% of the DD fusion rate, R^6Li ~ 0.1i?j5D. 5. Aneutronic and Non-Radioactive Nuclear Fusions The DD fusion reactions create neutrons and radioactive tritium. Candidate aneutronic and non-radioactive nuclear fusion reactions are 6 Li(p, 3 He) 4 He with Q = 4.02 MeV and n B(p,a)2 4 He with Q = 8.69 MeV. Given the same conditions as for the DD fusion, the fusion rate for the p 6 Li fusion is estimated to be ~ 30% of the DD fusion rate, R^6U ~ 0.3i?^ D , while the p n B fusion rate is estimated to be ~ 85% of the DD fusion rate, -fCiiB ~ 0.85i?j5D. The other aneutronic and non-radioactive reaction, 7 Li(p, 4 He) 4 He, has a much lower fusion rate, R 7U ~ 0.5 x 10" 2 i?p D .

469

For two cases, (p + Li) and (p + B), the fusion reaction rate has been estimated and is shown in Table 2 as a function of the fraction of hydrogen that is mobile within the lattice. In the calculation £jj(0) = 4.5 MeV-barn and 197 MeV-barn are used for 6 Li(p,a) 3 He (Q = 4.02 MeV) and u B(p,a)2 4 He (Q = 8.69 MeV), respectively. Table 2. Order-of-magnitude estimates for fusion rate, R®, in units of c m - 3 s _ 1 and power denisty, P, in untis of W c m - 3 . The particle (mobile protons) number density, p is in units of 6 x l 0 2 2 c m " 3 . Zf = Zit ZJ = Zjt pc = Pi = pj = p, and kT = 0.02 eV are assumed p(6 x 10 22 c m - 3 )

RQ6u

10"4

0.57 0.10 0.12 0.13 0.13

io~ 3 io- 2 10"1 1

(cm"3 x x x x x

s-1)/P(W/cm3)

10 2 /0.37 x I O " 1 0 10 6 /0.64 x 10~ 7 10 9 /0.75 x 10~ 4 10 1 2 /0.81 x 1 0 " 1 10 1 5 /0.83 x 10 2

KpiiB(cm-3 s-^/PCW/cm3) 0.16 0.28 0.33 0.36 0.37

X 10 3 /0.22 x 10~ 9 x 10 6 /0.39 x 1 0 " 6 x 10 9 /0.46 x 1 0 " 3 x 10 1 2 /0.50 x 10 1 5 /0.51 x 10 3

Based on the calculated results of fusion rates with the QPNF mechanism shown in Table 2, we see that nuclear fusion rates for (p+ 6 Li) and (p+ 11 B) LENR processes in hydrogenated metals/alloys are sufficiently high for practical energy generation. If we could achieve sufficiently high fusion rates for 6 Li(p, 3 He) 4 He and 11 B(p, a)2 4 He fusion reactions with the LENR processes in hydrogenated metals/alloys, they could become attractive alternative methods for generating clean nuclear fusion energy. 6. Other Potential Applications Finally, it would be of interest to consider other potential applications: 6.1. Glow Discharge

Experiments

As described in Section 3.3, glow discharge experiments are ideal probing and testing grounds for the QPNF mechanism. Recently, there have been many glow discharge experiments reporting anomalous effects.23_30 We plan to investigate the role of the QPNF mechanism in the glow discharge plasmas. 6.2. Acoustic

Nuclear Fusion

Reactions

Earlier, acoustic cavitation experiments (ACE) were carried out by Stringham. 31 In Stringham's experiments, 31 transient cavitation bubbles (TCB) were created in heavy water without the use of a neutron generator and were driven to impact on target metal foils as jet plasma. It has been reported 31 that these TCB jet plasma impacts produce excess heat and nuclear products (4He and tritium) suggesting a plasma impact fusion. In 1990, Lipson et al. reported observation of a very low level of neutron production in TCB type experiment. 32 Recently, Taleyarkhan et alzi

470

reported the observation of tritium and neutron production during their ACE using deuterated acetone and a pulsed neutron generator. Most recently, the temperature measurement of a single bubble acousitic cavitation has been made. 34 We plan to investigate the role of the QPNF mechanism in the ACE in our future work. 6.3. Geophysics

and

Astrophysics

The electron screening effect, in conjunction with a particle velocity distribution, has been shown to enhance the cross sections and reaction rates for protondeuteron (pD) fusion at extremely low kinetic energies. 35 The pD fusion reaction is shown to dominate other fusion reactions involving hydrogen isotopes for kinetic energies E < 8 eV in the center-of-mass frame. This indicates that pD fusion may serve as an important source of internal energy for planetary bodies. It was suggested 36 that the well-established high 3 He/ 4 He ratio in volcanic emissions 37-39 may be attributable to the reaction D (p,7) 3 He (Q = 4.50 MeV) occurring in the mantle of the earth, which has temperatures of 1200-3000° K (kT « 0.1-0.25 eV). The conventional calculation yields values of the pD fusion rate which are astronomically small. The QPNF mechanism enhancement of the fusion rate for the reaction D (p,7) 3 He may therefore explain the high 3 He/ 4 He ratio, and also provide a theoretical support for the view that a major source of mantle heating in the earth is due to reaction D(p, 7) 3 He. The effect of the QPNF mechanism on pD fusion may also provide a balance to the excess heat radiation from the gas giant planets (Jupiter, 40 Saturn, 41 Uranus, 42 and Neptune 4 2 ' 4 3 ). It will be interesting to see whether pD fusion based on the QPNF mechanism is a possible source for the excess heat emitted by Jupiter. We plan to explore these problems in terms of the QPNF mechanism in our future work. 7. Summary and Conclusions Both the BEF and the QPNF mechanisms are based on the same physical model, which assumes that deuterium/hydrogen is in a plasma state and is mobile in a deuterated/hydrogenated metal as deuteron/proton ion. , Based on the QPNF mechanism, we have investigated the quantum corrections to the equilibrium rate of nuclear fusion rate in a plasma. Using a generalized particle momentum distribution given by Galitskii and Yakimets, 7 we have constructed an approximate semi-analytical formula for the nuclear fusion reaction rate between nuclei in a plasma. The calculated results show that the QPNF mechanism leads to a dramatic increase of the fusion rate for mobile deuterons in deuterated metal/alloy at ambient temperatures. Our preliminary estimates indicate also that the deuteron-lithium (D + Li) fusion rate, the proton-lithium (p + Li) fusion rate, and the (p + B) fusion rate in a metal/alloy at ambient temperatures are also substantially enhanced due to the QPNF mechanism.

471 B o t h the B E F mechanism and the Q P N F mechanism are applicable to nearly all of the reported results of the L E N R and t r a n s m u t a t i o n experiments: (1) electrolysis experiments, (2) gas experiments, (3) nuclear emission experiments, (4) transient ACE, (5) ACE, (6) deuteron beam experiments, (7) glow discharge experiments, and (8) t r a n s m u t a t i o n experiments. References 1. P.L. Hagelstein et at, "New Physical Effects in Metal Deuterides", submitted to DOE for a review, July 2004, and references therein. This report was posted December 1, 2004 at the DOE website: http://www.sc.doe.gov. Published in the Proceedings of 11th International Conference on Cold Fusion ICCF-11 (Marseille, France, 2004; Condensed Matter Nuclear Science, pp. 23-59, World Scientific Publishing Co. Singapore, 2006). 2. See experimental papers in the Proceedings of the 10th International Conference on Cold Fusion ICCF-10 (Cambridge, MA, USA, 2003; Condensed Matter Nuclear Science, World Scientific Publishing Co. Singapore, 2006). 3. Y.E. Kim and A.L. Zubarev, Fusion Technol. 37, 151 (2000). . .. 4. Y.E. Kim and A.L. Zubarev, Italian Physical Society Proceedings 70, 375 (2000). 5. Y.E. Kim and A.L. Zubarev, Phys. Rev. A64, 013603 (2001). 6. Y.E. Kim, Progress of Theoretical Physics (Supplement) 154, 379 (2004). 7. V.M. Galitskii and V.V. Yakimets, J. Exp. Theor. Phys. (USSR) 51, 957 (1966). 8. Y.E. Kim and A.L. Zubarev, Quantum plasma nuclear fusion, Purdue Nuclear and Many-Body Nuclear Theory Group (PNMBTG), Preprint PNMBTG-4-05 (November 2005). 9. Y.E. Kim and A.L. Zubarev, Effect of a generalized particle momentum distribution on plasma nuclear fusion rates, PNMBTG-5-05 (December, 2005), to be published in Japanese Journal of Applied Physics, Vol. 45, No. 22, L552-L554 (June 2, 2006). 10. Y.E. Kim, D.S. Koltick, R. Pringer, J. Myers, and R. Koltick, in Proceedings of ICCF10 (Cambridge, MA, USA, 2003), pp. 789-799. 11. Y.E. Kim, D.S. Koltick, and A.L. Zubarev, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003), pp. 779-787. 12. YE. Kim and A.L. Zubarev, Mixture of charged bosons confined in harmonic traps and Bose-Einstein condensation mechanism for low energy nuclear reactions and transmutation processes in condensed matters, in Proceedings of the ICCF-11 (Marseille, France, 2004), pp. 711-717. 13. Coraddu et al., Physica A 340, 490 (2004); 496 (2004) and references therein. 14. F.A. Lewis, Platinum Metals Reviews 26, 20, 70, 121, (1982). 15. Q.M. Barer, Diffusion in and through Solids (Cambridge University Press, New York, 1941). 16. Y. Fukai, The Metal-Hydrogen System, 2nd edn. (Springer, Berlin, Heidelberg, New York, 2005). 17. R.A. Rice, G.S. Chulick, and Y.E. Kim, The effect of velocity distribution and electron screening on cold fusion, Proceedings of the First International Conference on Cold Fusion, pp. 185-193, March 1990, Salt Lake City, Utah, edited by F. Will. 18. R.A. Rice, G.S. Chulick, Y.E. Kim, and J.-H. Yoon, The role of velocity distribution in cold deuterium-deuterium fusion, Fusion Technol. 18, 147 (1990). 19. Y.E. Kim, R. S. Rice, and G. S. Chulick, The effect of Coulomb screening and velocity distribution on fusion cross-sections and rates in physical processes, Mod. Phys. Lett. A 6, 926 (1991).

472

20. J. Kasagi, Progress of Theoretical Physics Supplement No. 154, 365 (2004); Kasagi et al, J. Phys. Soc. Jpn. 73, 608 (2004). 21. C. Rolfs et al, Enhanced electron screening in d(d,p)t for deuterated metals, Prog. Theor. Phys. Supp., No. 154, 373 (2004); F. Raiola et al, Eur. Phys. J. A19, 283 (2004). 22. References 32, 33, 86-111 quoted in Hagelstein et al. (1). 23. T. Mizuno, T. Ohmori, and T. Akimoto, in the Proceedings of the ICCF-7 (Vancouver, Canada, 1998), pp. 247, 253; T. Ohmori and T. Mizuno, pp. 279-284. 24. T. Mizuno, T. Ohmori, T. Akimoto, and A. Takahashi, Production of heat during plasma electrolysis in liquid, Jpn. J. Appl. Phys. 39, 6055 (2000). 25. H. Conrads, R. Mills, and Th. Wrubel, Emmision in the deep vacuum ultraviolet from a plasma formed by incandescently heating hydrogen gas with trace amounts of potassium carbonate, Plasma Sources Sci. T. 12, 389 (2003). 26. Mizuno et al, Hydrogen evolution by plasma electrolysis in aqueous solution, Jpn. J. Appl. Phys. 44(1 A), 396 (2005). 27. T. Mizuno, T. Ohmori, and T. Akimoto, Generation of heat and products during plasma electrolysis, Condensed Matter Nuclear Science: Proceedings of ICCF-10, 73 (2006), World Scientific Publishing Co., Singapore. 28. T. Mizuno, Y. Aoki, D.Y. Chung, and F. Sesftel, Generation of heat and products during plasma electrolysis, Condensed Matter Nuclear Science: Proceedings of ICCF-11, 161 (2006), World Scientific Publishing Co., Singapore; T.B. Benson and T.O. Passell, ibid. pp. 147-160; A.B. Karabut, ibid. pp. 178-193. 29. T. Mizuno and Y. Toriyabe, Anomalous energy generation during conventional electrolysis, in Condensed Matter Nuclear Science: Proceedings of ICCF-12 (Yokohama, Japan, November 28-December 2, 2005), to be published. 30. J.-F. Fauvarque, P.P. Clauzon, and G.J.-M. Lalleve, Abnormal excess heat observed during Mizuno-type experiments, in Condensed Matter Nuclear Science: Proceedings of ICCF-12 (Yokohama, Japan, November 28-December 2, 2005), to be published. 31. R.S. Stringham, in Proceedings of the IEEE Ultras. Intern. Symp. (Sendai, Japan, Vol. 2, 1107, 1998); Proceedings of the Seventh International Conference on Cold Fusion (ICCF-7), Vancouver, BC, Canada (1998); Proceedings of IDDF-8, Villa Marigola, LaSpezia, Italy, May 21-26 (2000); Proceedings of IDDF-9, 323 (2002); Proceedings of ICCF-10 (2003). 32. A.G. Lipson, V.A. Klyuev, B.V. Deryaguin et aL, Observation of neutrons accompanying cavitation in deuterium-containing media, Sov. Tech. Phys. Lett. (Pisma v Zhurnal Teknicheskoi Fiziki), 61, (10), 763 (1990). 33. R.P. Taleyarkhan et al, Science 295, 1898 (2002); Phys. Rev. E 69, 36109-1 (2004). 34. D. Flannigan and K. Suslick, Nature 424, 52 (2005). 35. Y.E. Kim, R.A. Rice, and G.S. Chulick, The role of the low-energy proton-deuteron fusion cross-section in physical processes, Fusion Technol. 19, 74 (1991). 36. S.E. Jones et al, Nature 338, 737 (1989). 37. H. Craig et al, Geophys. Res. Lett. 5, 897 (1978). 38. J.E. Lupton and H. Craig et al, Science 214, 13 (1981). 39. B.A. Mamyrin and L.N. Tolstikhin, Helium Isotopes in Nature (Elsevier, Amsterdam, 1984). 40. R.A. Hanel et al, J. Geophys. Res. 86, 8705 (1981). 41. R.A. Hanel et al, Icarus 53, 262 (1983). 42. J.B. Pollack et al, Icarus 65, 442 (1986). 43. B. Conrath et al, Science 246, 1454 (1989).

CATALYTIC F U S I O N A N D T H E INTERFACE B E T W E E N INSULATORS A N D T R A N S I T I O N METALS

TALBOT A. CHUBB Greenwich Corp., 5023 N. 38th St., Arlington, VA 22207, USA E-mail: [email protected] Cold fusion uses a catalyzed configuration change to replace plasma fusion's need for high-energy particle collisions. 1 In radiationless cold fusion, the configuration change is a coherent partitioning of deuterons into fractional pieces within a set of potential wells provided by a hosting lattice. 2 The coherently partitioned matter distribution is a Bloch wave function. Alpha addition transmutations 3 require active deuterium in the form of Bloch function deuterons with 2-dimensional periodic symmetry. 4 , s The configuration change to Bloch form has been modeled as occurring in the interface volume between a salt and Pd metal. In Arata and Zhang radiationless cold fusion 6 - 8 reactive deuterons are modeled by Bloch ions with 3-dimensional periodic symmetry hosted in metallic nano crystals. 5 The nano crystals are isolated by salt-metal interfaces. In both cases, the fusion process is modeled as a Li—Feshbach resonance transition to an excited nucleus state, with subsequent energy transfer to a metal lattice by phonon cascade. 5 The lattice structure of the deuterons is preserved in the product nucleus until the energy transfer is completed. For the 2-dimensional symmetry case, the intermediate nucleus or many-body nuclear system can sometimes be observed in "flake" lattice form, providing insight about the process. 5 Research on salt-metal interfaces could facilitate cold fusion technology.

1. Introduction This paper builds on modeling published in the Proceedings of ICCF10 and ICCF11 and in the ANS meeting held in Washington in November 2005. Research results presented at ICCF12 clarify the picture of the cold fusion process, causing some revisions to the thinking presented in the ICCF11 Proceedings. New results influencing this paper are gas loading studies by Arata and Zhang, 8 and observations of abnormal nuclear products presented by Lipson et al.,9 Roussetski et al.10 and Savatimova.11 The paper discusses the following topics: the catalytic nature of radiationless cold fusion;1 the proposed role of insulator-metal interfaces in promoting the coherent partitioning of deuterons in Iwamura's alpha addition transmutations; 4 the proposed role of insulator-metal interfaces in heat-generating Zr02,Pd nano crystal powder; 7,8 a discussion of Oriani-Fisher energetic showers and their relation to observations by Lipson,9 Roussetski, 10 and Savvatimova;11 and a preferred picture of cold fusion reactions by Li-Feshbach resonance reactions involving excited product nuclei in lattice-geometry states. 5 473

474

2. Types of Deuteron—Deuteron Fusion There seem to be three different processes by which deuterons can be made to fuse so as to release nuclear energy. The conventional approach is thermonuclear fusion, which uses collisions between energized deuterons to create a transient He nucleus that decays by energetic particle emission. Deuteron-deuteron (dd) fusion is modeled by scattering theory. Quantum wave mechanics uses wave functions to describe the colliding particles as plane waves. The waves are treated as if arriving from infinity, and as going away to infinity after scattering or reaction. Gamow factors calculating the probability of transmission through the dd Coulomb barrier are used in calculating fusion rates. The other two dd fusion processes are catalytic processes. Catalysis substitutes configuration change for kinetic impact in promoting reaction. Catalytic processes usually use surface and interface science to reduce the temperature at which reactions can take place. The one catalytic process that is generally accepted as leading to dd fusion is based on creating an anomalously high-deuteron density. This high density is achieved in a D j molecule by replacing the ion's electron by a negative muon. The process is called muon-catalyzed fusion.12 The mass of the muon is 200 times the mass of the electron and creates a 200 times smaller molecule. The effective density is increased by a factor ~10 7 . At this density, quantum mechanics tunneling through the Coulomb barrier separating the two deuterons leads to a significant wave function overlap and fusion reaction rate. The nuclear products are the normal products of thermal plasma fusion. The process is not practical in a commercial heat source because of the short-lifetime of the negative muon against decay. The other catalytic method uses the reverse strategy. It works at normal density and uses a catalyzed configuration change to reduce dd Coulomb repulsion in a metal deuteride. The configuration change is called coherent partitioning, and the wave function describing the altered configuration is called a Bloch function.3 When the Bloch function configuration applies to deuterons hosted in a metal crystal, energyminimizing quantum mechanics replaces a 2-body wave function with Coulomb barrier by a 2-body wave function with anti-correlation. The anti-correlation factor reduces, but does not prevent wave function overlap and the associated possibility of fusion. The change in wave function configuration occurs when partitioning exceeds a critical value, namely, the point at which the quantum mechanics kinetic energy density associated with the dd repulsion singularity becomes greater than the potential energy density. When the anti-correlation wave function configuration applies, wave function overlap occurs and coordinate exchange symmetry becomes established. The strong force nuclear interaction is then no longer blocked, and deuteron pairs can fuse to produce a helium nucleus of the same Bloch array configuration. The Bloch dd <-> helium transition remains a reversible fluctuation unless energy can be transferred out of the product nucleus. The normal energetic particle and gamma ray modes of energy transfer are blocked by the array geometry. Energetic

475

particles and gamma rays cannot match onto the multiple-maximum array density structure of the Bloch ion. On the other hand, because Bloch deuterons and Bloch helium products have an array structure, they are small crystals that can store energy in their lattice degrees of freedom. Energy is stored in the form of excitations of lattice vibrations and in phonon excitations. If the product nucleus is produced in an excited nucleus state, some of the energy contained in the nuclear phonon modes can be resonantly transferred to the metal lattice provided that the difference between a pair of nuclear excitation levels matches the energy of a metal phonon mode, or multiple thereof. Phonon energy transfer appears to be the most likely mode of energy transfer that occurs in radiationless cold fusion. 3. Role of Insulator—Metal Interfaces The work of Iwamura et al.3 and a subsequent theory 4 ' 5 suggest that it is possible for a process to occur involving nuclear transmutation, in which the equivalent of two alpha particles is added to a Cs or Sr nucleus. In the theory, the alpha addition transmutation process has been modeled as a 4-step process in which the first step is a Fleischmann-Pons (F-P) fusion of Bloch deuterium into Bloch helium.2 This exothermic fusion step is postulated to take place inside the volume that constitutes an interface layer between a salt-like CaO crystallite and the transition metal Pd. The mechanism postulates the presence of deuterium in a 2-dimensional symmetry D + Bloch state. Conditions favoring this D + Bloch state may be provided by the CaO, which as an isolated crystal has a very negative free energy, and the transition metal Pd, which serves as a source of interface electrons. When the CaO makes contact with the Pd, the CaO serves as a lattice template and the more malleable sputtered Pd metal provides interface electrons that can neutralize the Dg loch charge. The thickness of the interface can expand to accommodate ion-dressing Bloch electrons without impairing 2-dimensional periodic order. The process may be aided by deuterium fluxing through the CaO, Pd composite volume. Further evidence for the possible role of insulator-metal interfaces in promoting F - P cold fusion is provided by the DS-cathode work of Arata and Zhang. 7 ' 8 The authors have shown that oxidization of Zr, Pd alloys produces powder that, when deuterided, generates multi-watt levels of excess heat. These powders presumably contain Zr02, Pd interfaces. Arata and Zhang have persistently taught the need for deuterons to have high-surface mobility throughout the powder beds inside their DScathodes, using the term "spillover deuterium" to describe this property. 6 They have used the absorption rate and the quantity of hydrogen absorbed at subatmospheric pressure to quantify this property and identify potentially useful materials. In their newest work,8 they have substituted elevated temperature gas loading for previously used electrolysis. The new work8 is considered exploratory, and though not calorimetric, appears consistent with production of significant excess heat. If the presented observations using Zr02, Pd nano crystals are confirmed, they may be a prelude to practical heating devices.

476

These observations suggest the need for a program to study and more fully understand the properties of insulator-metal interfaces and their applicability to the development of cold fusion heaters. Experiments are needed to more fully define the Iwamura and Arata type processes. There is need to study insulator-metal interfaces, and to determine whether or not a fully loaded deuterium interface is needed for configuring deuterium into active Bloch form. Recent condensed matter physics studies by Ichitsubo et al.13 and Barcaro et al.14 illustrate two types of interface study that could be helpful. The Barcaro et al. paper points out that metal-metal bonding competes with surface adhesion during the formation of a saltmetal interface. Also, it is of interest to know whether a thin coating of adsorbed water on Pd powder can preserve the 2-dimensional periodic geometry of a "flake" nucleus that had previously been formed inside the periodic environment of the ZrC>2, Pd interface volume. Adsorbed water was measured in a post-run study of an Arata-type cathode containing Pd-black. 15 4. Flake Nuclei An important characteristic of dd fusion reactions occurring in accord with imposed Bloch geometry is that both initial state and final state wave functions preserve the coherent partitioning of ions described by Bloch functions. The geometry is that of a Bravais lattice. This geometry is imposed on weakly trapped deuterons by the electron lattice within which the deuterons are embedded or in contact. When 2-dimensional Bloch symmetry applies, the product nucleus has a Bloch symmetry form that resembles a 2-dimensional crystal, e.g., the geometry of a 1-atom thick flake of graphite. 16 However, unlike a 1-atom thick crystal, the Bloch geometry nucleus contains only a 1/Nwe\\ fraction of a deuteron centered on each potential well position, instead of a full deuteron. Here, potential well means the localized volume containing a local minimum in the lattice potential as it attracts dressed-deuteron matter. Under normal circumstances, the flakes are viewed as being planar and embedded within the interstitial volume of a salt-metal interface. Under abnormal conditions, the flake is viewed as being able to move from its creation site within its hosting interface lattice, and to expand or migrate to another location in or on the metal. In extreme CclSGS, El flake nucleus is thought to be able to dissolve into a polarizable solvent like water, and subsequently become air-borne without losing its lattice form, i.e. without collapsing to the "point" form of a normal nucleus.5 At ICCF12, Savvatimova11 reported on a post-run metal surface showing a parallel-to-the-surface etched structure that looked much like the cast of a metalstrip coil, with the axis of the coil parallel to the metal surface. In another case she showed a linear series of etch pits arranged in a straight line and spaced with a strictly periodic order, such as an almost-buried cylindrical coil might cause if it were to periodically touch the metal surface. Neither of these types of structures had ever been seen under conditions not associated with processes designed to induce cold fusion. To me, the observations suggest a flake-like piece of nuclear matter with the geometry of a metal strip coil, such as is sometimes produced during machining of metal on a lathe. The flat strip geometry seems consistent with the

477

idea of a rectangularly extended "flake" nucleus with a "many micron" ^-dimension, a "micron" y-dimension, and an "Angstrom" z-dimension, formed into a cylindrical coil. At ICCF12, Lipson et al.9 and Roussetski et a/.10 discussed "hot zones" in studies of deuterided and hydrided Pd, PdO plates. These hot zones seemed to be sources of nuclear active material which subsequently decayed, producing ~15 MeV alpha particles. Tracks corresponding to alphas of ~15MeV incident energy were recorded in CR-39 plastic plate particle-track detectors. After exposure to the hydrided Pd, PdO plates, the CR-39 plates were etched to reveal the damage trails created by the incident alpha particles (CR-39 can also record energetic protons, but with different track characteristics). To explain the ~15MeV alpha particles produced by Pd, PdO loaded with light hydrogen, I propose the nuclear reaction 2 - 1 H + 1 8 0 -> 4 He + 1 6 0 . Here 2 - XH stands for a spin-paired spin-0 double proton. In its nuclear form the partitioned double proton is designated 2Heg[+ch. Synthesis of 2 Heg^ c h is endothermic when non-partitioned, but is expected to be exothermic when the double proton is coherently partitioned at large Nwe\\, as described in Ref. 5. To explain the ~15MeV alpha particles produced by Pd, PdO plates loaded with deuterium, I propose an incomplete fusion reaction of the form 2 — 2 D (pn, pn symmetry) + M —> 4 He (pp + nn symmetry) + M. Here 2 — 2 D is a Bloch-geometry spin-zero dd pair and M is an overlapped or colliding target nucleus subject to a transient transmutation analogous to the stable exothermic transmutations described by Iwamura et al. Note that the interacting nucleus M serves as a catalyst and is not changed by the reaction. In its nuclear form the partitioned double deuteron is designated 4Hegj+ch. The two forms of baryon symmetry designating different baryon pairings inside the 4Hegj£ h nucleus are shown in Fig. 2 of Ref. 5. The D + + D + symmetry used in the figure is the same as the pn, pn symmetry used here. A consideration of these possibilities, in combination with the Li-Feshbach resonance picture described in ICCF12 and in the next section, suggests that the Oriani-Fisher showers17 may occur by decay of a many-body piece of nuclear material that is produced and preserved in a vibrationally excited nuclear condition. The new picture differs from that presented in ICCF11. The ICCF11 picture was that showers originated in a cluster of individual ground-state nucleus "flakes" tangled up with each other and subsequently energized by collisions.5 In the new picture, the flakes that produce the alpha particles are viewed as being in long-lifetime metastable states, as described in the next section. The many-body nuclear material is envisioned as not having fully transitioned to a Bloch ground state. The nuclear fusion reaction energy has not been fully dissipated and is available to provide the energy that appears when shower-producing disturbances convert the large flake Bloch system into a sum of nuclei in point nucleus form. In other words, when the phonon energy cascade process is blocked by the nuclear flake material being separated from its initial hosting metal lattice, its nuclear reaction energy

478

still remains to energize the alpha particle emissions. In the new picture, there is no need for a "Maxwell demon" energization process, as suggested in Ref. 5. In the revised picture, the physically large nuclear flake structures causing major shower events could be of the same type as those causing the surface anomalies observed by Savvatimova. 5. Cold Fusion by Li—Feshbach Resonance Reaction One of the reasons that most physicists reject the possibility of radiationless cold fusion is the difference in time scale for point-particle nuclear interactions as compared with the time-scale for lattice energy transfer processes mediated by electromagnetic interactions. However, this discrepancy does not always exist even in classical nuclear physics. In particular, it does not seem to exist for 0+ to 0+ nuclear transitions in normal impact nuclear physics, when there are no intermediate non-0+ states between the adjacent 0+ states. Ranken et al. have studied the 19 F ( p , a o ) 1 6 0 and 19 F(p, a7r) 16 0 reaction cross-sections vs. proton energy.18 These two transitions involve the branched alpha-emission decay of 20 Ne to the ground and first excited states of 1 6 0 , both of which are 0+ states. The 7r in the second reaction stands for emission of an electron-positron pair in the transition between the excited state and ground state 0+ states of 1 6 0 . Ranken et al. write, "The excited states of Ne 20 formed by proton bombardment show a high probability of decay by alpha emission to states of O 1 6 . Alpha decay to ground and first excited states of O 16 is of particular interest in that, although the states are widely separated in energy, they are identical in spin and parity (0+) and hence a comparison of the total cross sections for these two processes should yield information concerning the energy dependence of the alpha decay transition probabilities for states of Ne 20 . In addition, the half-life of the pair-emitting state is sufficiently long, 5 x I 0 _ 1 1 s , for the O 16 nucleus to come to rest before the emission takes place". This lifetime is compatible with the Planck time for phonon energy transfers within a metal lattice. One wonders how much longer the lifetime of the metastable state would have been if its energy relative to the ground state had been less than the energy required to create an electron-positron pair. One also wonders what the lifetime would have been if the excited state had been a Bloch state. For 0+ Bloch states, creation of an electron-positron pair is forbidden by lattice geometry regardless of the energy separation between the 0+ states, for the following reason, The Bloch state, with its multiple energy density maxima, cannot provide a sufficiently high-energy density within any selected potential well of the set of occupied potential wells to create an electron-positron pair. The geometry mismatch prevents energetic particle emission. When the reactants and product nucleus are both in coherently partitioned form, both their point-particle and gamma-ray emission decay modes are blocked. This constraint applies to radiationless catalytic cold fusion. This impediment to fast decay leads to the possibility that a Bloch fusion product nucleus can remain in an internally excited nuclear state for an extended period of time if its coupling to

479

the hosting lattice is lost. However, if the nucleus product remains closely coupled to the hosting lattice by being part of a many-body Bloch system that is electrostatically coupled to the lattice, a cascade of energy transfer events can occur by acoustic phonon transfers from the Bloch nucleus with its lattice-geometry to the much more dense continuous spectrum of phonon states characterizing the host lattice. A first energy transfer to the host lattice changes an otherwise reversible fluctuation (a coalescence fluctuation) into an irreversible reaction. Subsequent cascading energy transfers lower the energy of an initially produced excited nucleus to its ground state energy.5 Mossbauer transitions can, in principle, directly transfer momentum and energy from a Bloch subsystem to a hosting lattice during a fusion reaction. However, there is indirect way by which fusion energy can be transferred to the lattice without producing a direct fusion product. One can produce a transient excited Bloch nucleus and subsequently consume it in a transmutation reaction, as seemingly occurs in Iwamura et al. It is not yet clear how prevalent consumption of the direct fusion product is. It might be occurring in Arata-Zhang experiments. Post-run 4 He has been proven to be present in post-run residual gas of an Arata-Zhang DS-cathode, but only at ~0.05% of that necessary to explain the generated heat. 19 However, I am inclined to think that the anomalously low-helium content in the sampled ullage gas is an experiment problem caused by helium loss through microcracks in the stressed wall of the DS-cathodes. 20 Further experiment is required to resolve this issue. The primary dd fusion reaction is considered to be enabled by a Li-Feshbach resonance. This means that the reaction takes place with near-zero energy dissipation. Li models this low-energy dissipation by adding an imaginary component to the strong force interaction potential. 21 The resonating initial and final nucleus states, though nearly identical in energy, are different in either their internal nuclear configuration and/or in their internal nucleus vibration plus phonon excitation profile. Any configuration or excitation change occurring during a Li-Feshbach transition allows additional time for the irreversible transfer of a small quantum of energy to the hosting environment. Alternatively, an energy transfer may occur during the initial coalescence fluctuation. With dd fusion, the strong force reaction occurs within a many-body subsystem 22 with Bloch geometry, and involves a spin-zero coordinate-exchanged dd coupling within the many-body system. Sometimes, a many-body system might contain only two Bloch deuterons within a nano-crystal of Pd. The 2-body case is the case modeled in Refs. 2 and 5. The nuclear transition is a 0+ to 0+ transition. No orbital angular momentum is introduced by the coalescence process. Much of the above is discussed as involving deuterons with 2-dimensional Bloch symmetry, patterned after a modeling of the Iwamura et al. process. However, because of the much higher, multi-Watt powers generated by Arata and Zhang, I continue to believe that their heat generation is based on 3-dimensional Bloch symmetry. Bloch deuterons are envisioned as being partitioned into a communicating

480 network of shallow-well sites, consisting of two tetrahedral sites plus one peripheral, already-occupied octahedral site per unit cell.

References 1. T.A. Chubb, Three types of dd fusion, ANS Transactions 93, 895 (2005). 2. T.A. Chubb, I. Bloch Ions, Proc. ICCF11, 665 (2006). 3. Y.Iwamura. M. -, and T. Itoh, Elemental analysis of Pd complexes: effects of D2 gas permeation, Jpn. J. Appl. Phys. 4 1 , 4642 (2002). 4. T.A. Chubb, II. Inhibited diffusion and surface transmutations, Proc. ICCF11, 678 (2006). 5. T.A. Chubb, III. Bloch Nuclides, Iwamura Transmutations, and Oriani Showers, Proc. ICCF11, 685 (2006). 6. Y. Arata and Y.-C Zhang, A new energy caused by spillover-deuterium, Proc. Jpn. Acad. 70B, 107 (1994). 7. Y. Arata and Y.-C Zhang, Formation of condensed metallic deuterium lattice and nuclear fusion, Proc. Jpn. Acad. 78B, 57 (2002). 8. Y. Arata and Y.-C Zhang, Development of 'DS-Reactor' as the practical reactor of 'Cold Fusion' based on the 'DS-cell' with 'DS-Cathode', ICCF12 Abstracts. 9. A.G. Lipson, A.S. Roussetski, G.H. Miley, B.F. Lyakhov, and E.I. Saunin, Reproducible nuclear emissions from Pd/PdO:D K heterostructure during controlled exothermic deuterium desorption, ICCF12 Abstracts. 10. A.S. Roussetski, Correct identification of energetic alpha and proton tracks in experiments on CR-39 charged particle detection during hydrogen desorption from P d / P d O : H x heterostructure, ICCF12 Abstracts. 11. I. Savvatimova, Unusual structures on the material surfaces irradiated by low energy ions and in other various process, ICCF12 Abstracts. 12. J.D. Jackson, Catalysis of nuclear reactions between Hydrogen Isotopes by fi~~ Mesons Phys. Rev. 106, 330 (1957). 13. T. Ichitsubo, E. Matsubara, T. Yamamoto, H.S. Chen, N. Nishiyama, J. Saidi, and K. Anazawa, Microstructure of Fragile Metallic Glasses Inferred for UltrasoundAcceletared Crysltallization of Pd-Based Metallic Glasses, Phys. Rev. Lett. 95, 245501 (2005). 14. G. Barcaro, A. Fortunelli, F. Nita, and R. Ferrando, Diffusion of palladium clusters on magnesium oside, Phys Rev. Lett. 95, 246103 (2005). 15. W.B. Clarke, B.M. Oliver, M. McKubre, F.L. Tanzella, and P. Tripodi, Search for He and He in arata-style palladium cathodes II: evidence for tritium production, Fus. Sci. Technolog. 40, 152, (2001). 16. K.S. Novoselov, D. Jiang, F. Schedin, T.J. Booth, V.V. Khotkevich, S.V. Morozov, and A.K. Geim, Two-dimensional atomic crystals, PNAS 103, 10451 (2005). 17. R.A. Oriani and J.C. Fisher, Energetic charge particles produced in the gas phase by electrolysis, Proc. ICCF10, 567 (2006). 18. W.A. Ranken, T.W. Bonner, and J.H. McCrary. Energy dependence of F 1 9 + p reactions, Phys. Rev. 109, 1646 (1958). 19. Y. Arata and Y.-C Zhang, Anomalous production of gaseous He at the inside of 'DS-cathode' during D 2 0-electrolysis Proc. Jpn. Acad. 75B, 281 (1999). 20. T.A. Chubb, Modeling the He concentration in a clarke et al. gas sample from an arata-style cathode, Proc. ICCF9, 67 (2002). 21. X.Z. Li, M.Y. Mei, J. Tian, D.X. Cao, and C.X. Li, Coherence in cold and hot fusion, ICCF8, Conference Proceedings. Vol. 70 in: F. Scaramuzzi (ed.), SIF, Bologna, (2000) p. 357; X. Z. Li.

481 22. LP. Chernov, Y.P. Cherndantzev, A.M. Lider, and G.V. Garanin, Excess heat released upon Hydrogen isotopes electrolytical saturation into Metals covered by porous film, Proc. 8th Russian Conf. Cold Nuclear Transmutation of Chemical Elements, 133 (2001).

MULTIPLE SCATTERING OF D E U T E R I U M WAVE F U N C T I O N N E A R SURFACE OF PALLADIUM LATTICE

X I N G Z. LI, Q I N G M. W E I , BIN LIU A N D N A O N. C A I Department

of Physics, Tsinghua University, Beijing E-mail: [email protected]

100084,

China

SHU X. Z H E N G A N D D O N G X. C A O Department

of Engineering

Physics,

Tsinghua

University,

Beijing

100084,

China

The wave property of deuterons and the periodicity of the lattice introduce the coherences in various aspects of the interaction between the deuterons and the lattice. Multiple scattering of deuterium wave function inside a super-lattice would manifest itself through an example where the coefficients of the reflection, penetration, and absorption are calculated while a deuterium flux permeates through a palladium foil coated with alternative layers of titanium carbide and palladium. When the resonance condition is satisfied, the maximized total absorption coefficient might be greater than 50%, even if the absorption coefficient of each single layer is only less than 1%.

1. Introduction Coherence has been an important issue to explain the abnormal phenomena in the palladium deuteride since 1989. However, the word of "Coherence" was used in a variety of situations such as "Q.E.D. Coherence in Matter", 1 "Ion Band State", 2 "Swimming Electron Layer Model" , 3 "Selective Resonant Tunneling" , 4 etc. If we dug into the essence of "Coherence", we might find two important factors: the periodicity of the lattice and the wave nature of the deuteron. These will be the starting points of this paper. 2. Wave Nature of the Deuterons Inside the Palladium Lattice Hydrogen gas is able to permeate through the palladium foil. This property was discovered more than 100 years ago, and it was believed that hydrogen molecule would be dissociated into hydrogen atoms first, and would be further ionized into proton and electron inside the palladium metal. 5 The proton was supposed to diffuse through the palladium foil as if proton was a granular particle. Its wave nature was usually ignored, because the diffusion model described the permeation quite well in most of the cases. Nevertheless, when the thickness of the palladium foil is less than a few microns, the permeation process is affected by the surface condition. 6 Even if the thickness is more than a few microns, the time necessary to establish 482

483

the equilibrium between the hydrogen inside and outside palladium is still sensitive to the surface condition of the palladium. 7 It was familiar that a coating layer of palladium black would work like a catalyst to speed this equilibrium, but the mechanism of these anomalies are not clear. The only thing we know is that these anomalies are not explainable in terms of diffusion model. Since the discovery of the correlation between deuterium flux and heat flow in the gas-loading phase, 8 ' 9 we studied the dependence of the deuterium flux on the number of coating layers, and its dependence on the palladium temperature. 1 0 ' 1 1 Both of these dependences are not explainable in terms of diffusion model either. 2.1. Dependence

on

Temperature

The dependence on temperature would be quite different if different models are assumed for the permeation process. According to the diffusion model, the random walks of the deuterons are constrained by the activation energy inside the palladium lattice. When the temperature increases, more deuterons would have chance to make the random walk; hence, the diffusion coefficient is a monotonic function of the temperature. The higher the temperature, the greater the diffusion coefficient is. Consequently, the deuterium flux permeating through the palladium foil is supposed to increase with the temperature in this diffusion model. However, the experimental observation showed that there was an abnormal deuterium flux, which increased while the temperature was decreasing (Fig. I). This phenomenon appeared even if there was several coating layers on the surface of palladium surface (Fig. 2). Instead of the monotonic feature, a peak-wise feature was shown in the curves of deuterium flux versus temperature. 2.2. Dependence

on the Number

of Coating

Layers

The dependence on the number of the coating layers would be quite different if different models are assumed for permeation process as well. In Fig. 3 the peak value of the deuterium flux permeating through the Pd foil is a function of the number of the coating layers. It shows a peak-wise feature as well. It was unexpected. When the number of the coating layers increases, the deuterons are supposed to permeate a thicker foil. If its behavior is pure diffusive; then, the deuteron flux is supposed to be a monotonic function. It should decrease when the number of layers increases. However, in Fig. 3, the deuterium flux peaked when the number of the layers was equal to three. Moreover, the flux for 3-layer-foil is still higher than that of O-layer-foil (i.e. no coating). This behavior cannot be explained based on the simple diffusion model. 3. Periodicity of Palladium Lattice When periodicity is combined with the wave feature of the deuterons we might expect a lot of new coherent phenomena other than the diffusion. However, the de' Broglie wavelength of the deuteron is very small in comparison with that of

484

45000

50000

55000

60000

50000

55000

60000

100

100 45000

Time (s) Figure 1. The solid line in the upper plot shows the deuterium flux, and the solid line in the lower plot shows the temperature of the D / P d system. Two peaks appear clearly between 150 and 140° C. 25 (f)

PO-

LU

LU)

OJ

:?"

15-

"

T °

10 v i o -

+J

? ~y 0 5= § 0

5" O 20

40

eo

SO

1CO

Temperature

120

140

160

1SO

(°C)

Figure 2. A deuterium flux peak appears near 140° C when the temperature of D / P d system increases. There were three alternative coating layers (Pd-TiC) on the surface of a Pd-foil (thickness 0.1mm).

485

Peak value of deuterium flux versus number of layers 30

E


CM

alu eof

= h « O)

Pea

V

O

20 15

X X 3

10 5 0

0

1

2

3 4 Number of layers

5

6

Figure 3. The peak flux value as a function of the number of the alternative coating layers on the surface of the Pd foil (thickness 0.1 mm).

electrons; hence, one might wonder if the vibration of the lattice might destroy the Coherence. 3.1. Debye-Wallet

Effect

The theory of electron diffraction might be helpful to solve this problem. Early in 1930s, when the electron diffraction by crystal lattice was first proposed, the suspects worried about that the random vibration of the crystal lattice might blur the diffraction peaks. It was found later that this blurring effect was a second-order effect because the diffraction peaks observed are the average result which would make the first-order effect vanished. This second-order effect is proportional to the square of the ratio of amplitude of thermal oscillation to the lattice constant. This is called as Debye-Wallet effect, and has been verified in experiments. 12 The low energy electron diffraction experiments showed that for 100 eV electron beam the diffraction peaks were clearly shown even if the temperature of the crystal lattice approached 400°C. 13 For the deuteron, due to heavier mass we might expect the diffraction and coherent effects for 30 meV deuterons as well, even if the palladium is heated to 140°C. 3.2. Symmetry

of Lattice in Different

Directions

We must notice that the symmetry of interaction between wave and lattice is different for different directions. Periodicity is from the symmetry of the lattice. For a face-center cubic lattice, it seems symmetrical in three directions, but if we consider the gradient of the deuteron density for the gas-loading cases, the perpendicular direction to the surface of the palladium might be different from the directions parallel to the surface of palladium. When we apply the Bloch Theorem for the wave function of the deuterons, we require the periodicity in the surface layer first instead of the symmetry in three directions. The palladium crystal is considered as a combination of many layers: one layer after another layer in the direction perpendicular to

486

the surface. As a result, we have the relation for two components of the momentum in two directions:

k2=kf+k2±.

(1)

Here, k is the total momentum, fcy the component of the momentum of the deuteron moving in the direction lying on the surface of the palladium; k± is the component of the momentum of the deuteron in the direction perpendicular to the surface of palladium. As above mentioned, the periodicity in the surface layer requires that: 2ir fell = k0 H n. " a

(2)

Here, n is an integer, a the lattice constant, and fco is the eigenvector in the first Brillouin region. For the permeation in the k± direction, instead of diffusion coefficient the wave theory would give the reflection, transmission, and absorption coefficients, respectively. 4. Some Qualitative Comparison between Theory and Experiment Before a quantitative comparison available, we may study some of the qualitative feature for any coherence. 4 . 1 . Temperature

Effect

Temperature may change the kinetic energy of the deuteron; hence, the wavelength of deuteron. Thus the wave property should be affected by the temperature. In Eq. (1), the total momentum k is determined by the kinetic energy of the deuteron; hence, k is a function of temperature. It is known that there are several temperature intervals where we have seen the anomalous phenomena in the D/Pd systems. The famous "Heat after Death" phenomenon appears near 100°C;14 the nuclear transmutation experiments were done preferably near 70°C; 15 Arata and Zhang's new Double-Structure experiments were done near 140°C,16 and we discovered the correlation between anomalous deuterium flux and heat flow just near 140-150°C as well. 8,9 These specific temperatures might be the result of some coherence effects between deuteron wave and the periodicity of the lattice. When temperature increases, both the lattice constant and the kinetic energy of the deuteron may increase. However, the effect of kinetic energy dominates. When more specific temperatures are available we may find their relation with some integers just like that of low energy electron diffraction.12 4.2. Surface

Effect

The wave property should be apparent near the surface layer. The reflection of the deuteron wave on the first surface layer may interfere with the wave reflected from

487

the layer next to the surface layer. The destructive interference might greatly reduce the total reflection wave, and enhance the permeation of the deuteron through the palladium foil. A high gradient of deuteron density would appear near the surface to accommodate this enhanced permeation. This high gradient of deuteron density might be a good region to sustain some coherence. Iwamura's nuclear transmutation experiment supported this surface effect.15 4.3. Positive

Correlation

between Deuterium

Flux and Heat

Flow

The positive correlation or negative correlation between absorption and transmission implies different physics on the surface of palladium. If we assume that the absorption in palladium leads to the excess heat (i.e. the heat flow); and the transmission leads to the deuterium flux through the palladium film, then, Fig. 1 shows that both the absorption and the transmission may increase together with the temperature. The positive correlation between deuterium flux and heat flow means that the total intake on the surface of the palladium may increase or decrease with the temperature. In other words, the reflection from the surface may change with temperature when the incident number of the deuterium molecules was about fixed by the deuterium pressure. This may be explained as a result of variation of the wavelength when the kinetic energy of the deuteron is changing. As a consequence, the coherence between deuteron wave and the palladium lattice is changing with temperature. On the contrary, if a negative correlation between absorption and transmission was observed; then, it might imply the total intake on the surface of palladium may be fixed by the deuterium gas pressure. The absorption might vary with the temperature. Any reduction in absorption would result in the increment of the transmission. Hence, the negative correlation might imply that the reflection from palladium surface does not change with temperature. This is a simple diffusion flux through a Pd film as granular particles. In a word, this positive correlation between deuterium flux and heat flow is an additional evidence to show the wave property of the deuterons near the surface of palladium lattice. 5. Numerical Calculation 5.1. New Paradigm

of Theoretical

Description

Reflection, absorption and transmission coefficients are introduced instead of crosssection or life-time here, because we are supposed to set up a model to describe the interaction between the deuteron wave and the periodical lattice well in a steady state. Cross-section is not suitable here, because we are no longer dealing with a beam-target configuration. In the lattice-well-confinement configuration, the reflected wave from the Coulomb barrier may be reflected again by the lattice well. The bouncing back and forth motion happens not only inside the nuclear well, but also inside the lattice well. It is a new kind of resonant interaction between nuclear scale and lattice scale. Hence it is a new paradigm of theoretical description.

We would not use the concept of decay-time of a resonant state here either, because we prefer to study a steady state, i.e., a self-sustaining state maintained by a constant flux. There are three kinds of coherence: the resonance inside the nuclear well; the coherence in multiple scattering of deuteron wave by the symmetric lattice centers; and the coherence between different layers in parallel to the surface layer. In order to simplify the calculation, we start from the simplest configuration, and attempt to answer the most important question: i.e., is it feasible to confine the deuterons inside the lattice well in order to enhance the d + d fusion reaction rate dramatically at low energy in terms of multiple scattering mechanism. 5.2. Multiple

Layer

Model

In this simplest model, only one of the three abovementioned coherences is involved. Only the multiple scattering between different layers is considered. The other two coherences inside each layers has been discussed elsewhere preliminarily.17 A palladium lattice is assumed to be composed by a series of parallel layers in Fig. 4. Each layer has three parameters to describe its intrinsic nature: i.e., the reflection coefficient, R(l), the absorption coefficient, A(l), and the variation of the phase angle, (f>, which gives the phase shift of the wave function after the scattering by this single layer. We have to answer the question: "are we still able to reach a significant absorption coefficient using the coherence of multiple scattering?", even if the absorption coefficient A(l) is very small.

A(N)

T(N)

R(N) R(1),/\(1) Figure 4. Multiple layer model. Coefficient of absorption and reflection (A(N) and R(N)) of multiple layer are function of single layer properties (A(l) and R ( l ) ) .

We have derived a formalism to describe the multiple scattering effect of TVlayers. 18 The reflection coefficient,i?(/V), the absorption coefficient, A(N), for TVlayers may be expressed by R(l), A(l), <j>, and TV as follows: Using quantum mechanics, for a single layer we may write the matrix, M ( l ) , which connects the outgoing wave function, 4 , o u t (l) , and the incoming wave function, Vl/in(l) as: *in(l)=M(l)*out(l).

(3)

489

This matrix is written in the plane-wave representation. For example in the case of outgoing wave only (see right-hand-side of Fig. 4), (4)

*out(l)

then, the incoming wave should be "M(l)u" (5)

*in(l) =

[M(l)21_ In general, the scattering matrix for a single layer may be written as: T(l)

M(l)

fl(l) T(l)

24>

4W)

^^{R{i)

+ T{i))

(6)

Here T(l) = 1 — i?(l) — .4(1) is defined as the transmission coefficient for a single layer based on the conservation of the current of probability. The phase angle, 0, represents the phase change during the scattering in a single layer and during the transition from one single layer to the next layer. The definition of M ( l ) in Eq. (6) guarantees the symmetry of single layer; i.e., the coefficients of reflection and the transmission are same for the left or right incident wave. When M (1) is diagonalized as (7) We have, "M(l)n+M(l)2 a

arccos arccos<

T(1)L

1

A(l)

cos(2c/>) -i

A(l) —^sin(2)

(8)

This a is different from 0, because a is calculated for an incident wave, which is a combination of two plane-waves traveling in both directions. For the case of iV-layers, the scattering matrix equation should be written as * in (JV) = M(iV)* out (7V).

(9)

If we keep the outgoing wave function same as before; then, (10)

WW) We may assume M{N)

M(JV)n

M(N)12

M{N)2l

M(N)22

(11)

490

Hence, 'M(N)u _M{N)21

*in(iV)

(12)

Based on matrix algebra, it can been proved that Wl

^M(1)ll.*iM. sin [a] M(Nhl

(13)

sin[aj * 1 M ( 1 )

s

2

,

(14)

sin[a] The reflection coefficient, penetration coefficient, and the absorption coefficient may be written as the function of the elements of the scattering matrix: |M(1) u , |M(1) ii

fl

(!)=

T

(

1

)

3

|2

•

« '

A(l)sl-i!(l)-r(l). The similar definition is valid for iV-layers _ |M(AQ 21 | 2

(

1 5

)

( 1 6 )

(17)

= WW'

(18)

w = mkrf'

(19)

R{N)

T

A(7V)

EE

1 - R(N) - T(N).

(20)

An important conclusion may be drawn from this very general relationship between M(iV) 2 i and M ( l ) 2 i Eq. (14): when the reflection rate for single cell is not zero; the total reflection rate for N cell might be zero as long as Sin[j

^ = 0. (21) sin[aj In physics, this is the result of destructive interference among all the reflected waves. At the same time R{N) = 0 implies T(N) —> 1 when there is no absorption. It means a constructive interference among all the propagating waves inside A^-layers, which enhances the penetration rate greatly. The conservation of the probability guarantees the eventual penetration after all the reflections and penetrations in layers. Now we may introduce a small absorption coefficient, A(l)
491

abscissa is the phase angle variation for each layer, . It depends on the distance between two adjacent layers also. The ordinate is the three coefficients, A(N), T(N) and R(N). Correlation between absorption (An) and transmission (Tn)

0.2 0.3 Distance between layers (in unit of vt)

0.5

Figure 5. The total absorption coefficient, A(N), transmission coefficient, T(N), coefficient, R(N) for the case of 20-layers with A(l) = 0.01 for a single layer.

and reflection

6. Discussion 6.1. Positive Correlation Transmission

between Total Absorption

and

The solid line, A(N), and the dash-dot line, T(N) reach the peak and valley at the same position. This is just what we expected for a deuteron wave, which is reflected from the surface of the palladium layers. When the reflected wave is minimized [the dotted line, R(N) reaches the valley], the wave entering multiple layers is maximized. Hence, both the total absorption, A(N) and the total transmission, T(N) reach the peak. 6.2. The Maximum

Value of

A(N)

The maximum value of A(N) is more than 0.5 although the absorption for a single layer, A(l), is only 0.01. Since N = 20, this implies that in average the deuteron would pass through each single layer more than 2.5 times. This is what we expected also. The multiple layers play a role of confinement of deuterons, which experience the bouncing back and forth motion inside the palladium before the deuteron flux finally penetrates the multiple layers.

492

6.3.

The Minimum

Value

of

A(N)

T h e minimum value of A(N) is a little bit less t h a n 0.2. It implies t h a t some of deuterons are reflected out before they reach the 20th layer. 6.4. Boundary

for

the Phase

Angle

There is a clear b o u n d a r y for the phase angle, . For (ir/8) < 4> < (3TT/8), the three total coefficients are oscillating, b u t beyond this interval, they are decaying or growing monotonically. This behavior is expected from the coherence as well. T h e phase angle, a in Eq. (8), includes b o t h the information for single layer (A(l)) and the information for multiple layer(0). W h e n A(1) —> 0, cos a in Eq. (7) is mainly a real number. However, a may become a complex number when | c o s a | > 1. It is noticed t h a t even if A ( l ) —> 0, cj> < (TT/8), or (37r/8) < just makes | c o s a | > 1. This makes a an imaginary number, which results the monotonic behavior of A(N), T(N), and R(N). For (n/8) < (f> < (3n/8), \cosa\ < 1; hence, a is mainly a real number with a small imaginary p a r t [A(l)
Remarks

T h e coherence between the deuteron wave and the periodic structure of the multiple layers may explain the positive correlation between the excess heat and the deuterium flux near the surface of the palladium. We may use this coherence to confine the deuteron wave inside the multiple layers in order to enhance the fusion reaction rate in the metal deuterides. Acknowledgments This work is supported by the Natural Science Foundation of China (#10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds). References 1. 2. 3. 4. 5. 6. 7. 8. 9. 10.

G. Preparata, Q.E.D. Coherence in matter. World Scientific, Chapter VIII (1995). T.A. Chubb and S.R. Chubb, Fusion Technol. 20, 93 (1991). H. Hora et al, Phys. Lett. A175, 138 (1993). X.Z. Li et al., Laser Part. Beams 22(4), 469 (2004). A.H. Verbruggen et al, Phys. Rev. Lett. 52, 1625 (1984). X.Z. Ren et al, The Proceedings of ICCF9, in: Xing Z. Li (ed.), Tsinghua University Press (Beijing, China, 2003) 19-24 May (2002) p. 305. G. Alefeld and J. Volkl, Hydrogen in Metal Springer-Verlag, Berlin, Vol. 1 (1978). X.Z. Li, et al, The Proceedings of ICCF9, in: Xing Z. Li (ed.), Tsinghua University Press (Beijing, China, 2003), 19-24 May (2002) p. 197. X.Z. Li et al, J. Phys. D: Appl. Phys. 36, 3095 (2003). X.Z. Li, G. L. Schmidt, and J. Tian, The Proceedings of the 5th Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, Asti, Italy (19-21 March 2004).

493 11. X.Z. Ren, Study on Anomalous Characteristic in Deuterium-Palladium System, Master Thesis at Tsinghua University (2003). 12. C. Kittel, Introduction to Solid State Physics, 5th edn (John Wiley & Sons Inc., New York, 1976), p. 63. 13. J.B. Pendry, Low Energy Electron Diffraction (Academic Press, London and New York, 1974) p. 25 14. M. Fleischmann and S. Pons, Phys. Lett. A 176, 118 (1993) 15. Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642 (2002). 16. M.J.A. Yoshiaki Arata and Y.-C. Zhang, Presented at 12th International Conference on Cold Fusion, Yokohama, Japan, November 27-December 2 (2005). 17. S. Chen and X.Z. Li, Proceedings of ICCF-10, in: P.L. Hagelstein, S.R. Chubb (eds), World Scientific (Singapore 2006) Cambridge, USA, 24-29 August (2003), p. 717. 18. X.Z. Li et al., The Proceedings of ICCF9, in: Xing Z. Li (ed.), Tsinghua University Press (Beijing, China, 2003) 19-24 May (2002) p. 202.

THEORETICAL COMPARISON B E T W E E N SEMI-CLASSICAL A N D Q U A N T U M T U N N E L I N G EFFECT

FULVIO F R I S O N E Department

of Physics,

University of Catania, Via Santa Sofia 64, 95125 Catania, E-mail: [email protected] Tel: +39-095-3785227; Fax: +39-095-3785227

Italy

We compare the trends, at constant temperature, of the probability of tunneling and of the effective quantum and semi-classical potentials, which describe, under these conditions, the interaction between deuterons in pure and impure palladium lattices. It is seen that only the quantum case is characterized by an amplified tunneling effect on increasing the concentration of impurities present in the lattice, as previously observed. Further, it is hypothesized that the phenomenon of fusion is not only conditioned by structural characteristics and the thermodynamic conditions of the system, but also by the concentration of impurities present in the metal, correlated with the deuterium loading within the lattice itself. The analysis will attempt to determine whether, in the case of the three-dimensional isotropy, D2 loading can lead to the formation of micro-cracks in an analogous manner to that suggested for temperature variation. This would constitute an ulterior verification of the hypotheses proposed.

1. Introduction Over the last five years, the theoretical investigation into the phenomenon of cold fusion of deuterons within crystalline lattices with Cubic Face Central symmetry has repeatedly suggested that tunneling, following which fusion should occur, could be significantly influenced by impurities present in the lattice or by variations in the temperature of the system. 1 _ 3 In particular, we have suggested that when these factors act simultaneously they have the effect of reducing the thickness and depth of the attractive part of the effective potential, which describes the interaction between deuterons, both for the pure Coulomb potential and in the case where also the contribution from electronic screening is evaluated. With the aim of further investigating the occurrence of effects of this type, this paper presents an analysis of the behavior of a simplified model of a gas of interacting neutrons, in motion within the Palladium crystalline lattice and free of interactions with lattice ions, in order to exclude possible deformations of the effective potential (due for example to deuteron-plasmon coupling) previously observed.1 The situation proposed is characterized by the presence of ordinary short-range interactions between deuterons, corrected by collective type quantum effects, analogous to the formation of charge density waves (CDW) in metal lattices. The model used is semi-classical, in the sense that it treats atoms as nonimpenetrable, deformable spheres, so as to reproduce, within the limits typical of a 494

495

mechanical model, the effects of tunneling which, it is known, is a typically quantum phenomenon. Further, the model takes account of short-range inter-atomic repulsive forces in several ways, but not long-range attractive forces, using effective potentials analogous to those already employed for the calculation of the probability of tunneling. 2 Finally, the model does not take into account variations in lattice temperature, but only effects due to a greater or lesser concentration of impurities. An overview of the effects linked to variations in temperature is presented in Ref. 2. Before analyzing the semi-classical5 model, we present a brief summary of the quantum results for a three-dimensional model, illustrating 6 the CDW phenomenon in general outline. 2. Three-Dimensional Quantum Model Because of the reduced extension of the phase space, phenomena such as fluctuations, impurities and interactions have considerable effect on the dynamics of systems with few dimensions. For example, almost one-dimensional metals show charge density waves 6 ' 7 and become insulators in correspondence to the phase of transition to CDW state. More precisely, make 8 calculates the probability of the formation of solitonantisoliton pairs due to an electric field using a Lagrange model for the phase variable cp(r,t), which describes the dynamics of a Frohlich CDW condensate. He shows that at sufficiently low temperatures, electrical conductivity is dominated by the quantum tunneling 7 ' 8 effect, and is a strongly non-linear function of the electric field intensity. The probability of the quantum tunneling 8 effect occurring in almost one-dimensional lattice models is given by P(E) = exp(—Eo/E), where EQ = (fkVp)2/ithv-pe* [see Eq. (A12)] and LOP has a small value; e* = em/(m + M-p) is the effective charge of the deuterons, 7 with m the mass of the deuterons and Mp the associated Frohlich mass; E = Eapp\ - Epo\, where i? app i is the electric field applied to the deuterons, given by £ a p p i > 2ET (total energy), while Epoi is the correction introduced by polarization effects, which are however ignored in this case, regarding the motion of deuterons within the lattice. Charge density waves can also be calculated using the Hartree-Fock approximation. The simplest of these CDW states is obtained if it is assumed that all the electrons meet the same potential, independent of spin but periodic concerning their spatial position. This presupposition can be self-consistent and, under certain circumstances, the corresponding CDW state will have lower energy. The Coulomb energy contribution is greater in this case, but this increase is more than compensated for by the decrease in the energy of single particles of electrons just below the Fermi energy. This previous expression for quantum tunneling does not take account of the gradual variation with the distance r of the effective interaction between deuterons, or of the presence of any lattice impurities.

496

The aim of the present analysis is, instead, to study the effect of interaction between deuterons within a crystalline lattice on the process of cold fusion. Further, the lattices available for experimental investigation always contain a certain concentration of impurities, though small. Since one of the characteristic themes of our research has been the elaboration of a model which better reflects "real" processes, these two fundamental characteristics were accounted for by modifying the expression of the probability in order to establish whether they could contribute to the phenomenon by amplifying the tunneling effect, as previous studies 1 , 2 ' 3 indicated. With regard to the influence of impurities, it was found, for example, 3 that the probability of penetrating the Coulomb barrier increases on increasing the concentration of impurities. These appear to be able to concentrate in their vicinity a significant fraction of the deuterons present in the metal. The phenomenon shows characteristics analogous to the formation of a Cottrell 3 atmosphere in metals, known for some time in solid state physics. This essentially consists of a redistribution of the impurities present in the metal around a dislocation of the ions making up the lattice. In this case, the interaction between impurities and dislocations can significantly modify the electrical properties of the material. Further, particular reactions can occur, incorporating the impurities in the core of the dislocations as a result of the different arrangement of atoms with respect to that of the non-perturbed lattice. This type of process has been extensively studied in the literature in the case of high temperature crystalline semiconductors and metals. For the latter, it is demonstrated that the concentration of interstitial impurities around a linear dislocation with point component depends on the temperature according to a law of the type J = JQ exp((3/bkT), where Jo is the concentration of impurities in the zone with null internal pressure, o3 ~ Vi the volume of the ions making up the lattice, while (3 is proportional to the difference v
— - - Ves{r) p J ) d r .

(1)

Co J IT

In Eq. (1), hujp is the vibrational energy of the phonons 8 present in the metal (e.g. palladium), VF is the frequency of the phonon, \i the reduced mass of the deuterons, Ves(r) the effective interaction 9 potential, and J's the concentration of impurities present in the crystalline lattice. Since we require for Vefi(r) an expression which can be used in the case of threedimensional isotropic lattice geometries, and which also takes account of the interaction between deuterons and variations in temperature but not of deuteron-phonon

497

coupling, we can use the following expression: 2,3 fkTR q2 VeS(r) = kc — V{r)u - J^ r Here kc = 1/4TTSQ is the Coulomb constant, q the charge of the deuteron, £ a parameter which depends on structural characteristics of the lattice (number of "d" band electrons), variable between 1.5 x 10" 3 and 2.5 x 10~ 3 , T the absolute temperature, R the nuclear radius and V(r)yi is the intermolecular Morse potential which, introducing appropriate corrections, in this case becomes: 2 ' 3 V(r)M = (JA) exp(-2<^(r - r 0 )) - 2 e x p ( - ^ ( r - r 0 )).

(3)

In Eq. (3), (J/<j) is the depth of the barrier, parameters ^ and

RJ 0.13 Hz, a PS 0.37 A, T(K) = Const) Eta

Pre

140 150 160 170 180 190 200 210 220 230 240 250

10-84 10-81 10-79

io-75 lO"73

io-71 10-70 10-68 10-65 10

-63

10-62 10-60

E is expressed in eV.

Another possible important effect influencing tunneling is that of electronic screening. Already studied by Rabinowitz et al.,4, this effect can be accounted for by using a model in which the negative charge is distributed over a thin shell of internal radius R. Thus, for the interaction potential within the metal, it is possible to write the "shifted" Coulomb potential, given by: "1 1" ri < r < R, (4) V = (kCq2) r ~ ~R where q is the deuteron charge, r\ the nuclear radius, and kc = l/47reo. Then V = 0 for r > R.

498 Table 2. Pure metals palladium ( J ?» 0.28%, u f» 0.13 Hz, a as 0.37 A, T(K) = Const) £f»

P:

140 150 160 170 180 190 200 210 220 230 240 250

10 10 10 10 10 10 10 10 10 10 10 10

E is expressed in eV.

In Ref. 1, the probability of tunneling is compared in impure and pure (J = 0) lattices, using the potentials (2-3) and (4). It was found that a concentration of impurities in the order of 0.75% increases the probability of tunneling by at least 1-3 orders of magnitude with respect to the case of non-deformed lattices, and also reduces the thickness and the height of the Coulomb barrier. This result can be interpreted considering the trend of the curve of potential V(r), which describes the effective interaction between deuterons within the metal. In effect it is shows that in the presence of impurities, the coupling between plasmons and deuterons is able to not only decrease the thickness but also reduce the height of the Coulomb barrier. The reaction of deuteron fusion, catalyzed by the plasmons of a lattice with cubic structure on varying the temperature, was analyzed in Ref. 2. The trend of the probability of fusion in pure and impure palladium lattices suggests that the formation of microcracks in the lattice as the result of deformations 9 induced by variation in temperature, could catalyze the interaction between deuterons, amplifying the tunneling effect and triggering a sort of chain reaction which would favor the fusion process. Also in this case, an examination of the trend of the effective potential describing the effective interaction between deuterons within the metal, confirms a reduction in the thickness K of the Coulomb barrier. The comments regarding electronic screening and its effects, and those referring to the presence of a probable chain reaction in lattices with microcracks, are included here only to summarize the results obtained by the author using the quantum model, but will not be used to determine numerical conclusions, which have already been presented in Refs. 1 and 2.

499

3. Semi-Classical Model The semi-classical probability of tunneling is given by: 5 |T| 2 = e x p ( - 2 7 ) ,

(5)

7 = Ja y/MV(r) - E}^ J dr,

(6)

where E is the total initial energy of the system, mainly thermal in nature, V(r) the potential barrier (which in the semi-classical case substitutes Veg(r)), and V(ri) = E is the condition identifying the semi-classical turning point r\, with a < n < (3. To obtain an expression of the barrier potential V(r), which takes account, in the semi-classical case, of the effects linked to variations in temperature and the presence of impurities, the "shell" potential (4) was modified as follows:

W = (*c« 2 )(J-|^),

n
(7)

where kT is the mean thermal energy, e the vibrational energy, typically in the order of several eV for quantum states. Using Eqs. (5)-(7) for the semi-classical case, some typical values (Tables 3 and 4) were obtained for the probability of tunneling 7 on varying the temperature and concentration of impurities. Table 3. Pure metals palladium ( J * 0.28%, to Ri 0.13 Hz, a RS 0.37 A, T(K) = Const) Ea

T«

140 150 160 170 180 190 200 210 220 230 240 250

10~ 8 9 10-87 10-80

10~ 7 6 10-74

lO"73

io-71 10-69 10-64 10-61 10-58 10~53

E is expressed in eV.

The results shown in the Tables 1 and 2 are obtained using the quantum model while the results in Tables 3 and 4 are obtained with semi-classical model. A comparison of the results obtained shows that the probability of tunneling varies in a similar way to that of the energy and concentration of impurities, although the results differ by several orders of magnitude for equal E and J. This difference is

500 Table 4. Impure metals palladium ( J RS 0.72%, uj ss 0.13 Hz, a. RJ 0.37 A, T(K) = Const)

£«

T ',

140 150 160 170 180 190 200 210 220 230 240 250

io10 10 10 10

ioio10 10 10 10 10

E is expressed in eV.

evidently due to the quantum corrections, considered in only the first two tables and not in the second two. The dependence of the probability of tunneling on the energy and concentration of impurities is mirrored by the trend of the effective potentials, shown in Figs. 1 and 2 for the two cases. 4. Conclusions In Ref. 2, we showed that the thickness of the Coulomb barrier varies according to some parameters such as the concentration of impurities within the lattice, the temperature of the system and the vibrational energy of the deuterons, etc. The present theoretical study has shown that, unlike the quantum case, the semi-classical tunneling effect at constant temperature is not amplified by an increase in the concentration of impurities. The semi-classical potential (7) varies on increasing J in a way that reduces, rather than increases, the tunneling effect. In fact, as shown in Figs. 1 and 2, the thickness and depth of the barrier increase. The amplification of tunneling is seen therefore as an eminently quantum effect, lacking analogies in the semi-classical case. The calculations were performed supposing that the interactions 7 ' 8 between deuterons occur within a Palladium 9 lattice, with a cubic crystalline structure and 10 d-band electrons. An in-depth study of the possible effects associated with the transition of ci-band electrons to higher bands is presently in progress. If the trends obtained here for the potential of interaction within the lattice are compared with previous results, 2,3 it can be seen that in a three-dimensional geometry, temperature effects can induce several important effects. For example, the height of the potential barrier can be reduced for impure metals (J = 0.75%) and the corresponding probability of fusion can vary by 3-4 orders of magnitude, while the barrier remains substantially unchanged for pure metals ( J = 0.25%).

501

150

100

50

>

£ o c o a.

-50 J =0.75%

J =0.25%

-100

-150 0.1

0.2

0.3

0.4

0.5

0.6

0.7

/tA) Figure 1. In this figure a quantum model was used. The trends of the quantum potential (2), which contains the Morse contribution (3), (curve on left) and the modified semi-classical "shell" potential (7) (curve on right), are shown for different values of impurity concentrations. The dotted line (Lei) indicates the lowest energy level; the lower unbroken line indicates the total energy.

An interesting aspect, which merits further investigation, is the application these studies may have in a field completely different from the tunneling effect. Further theoretical and experimental studies are in course to analyze the non-semi-classical tunneling effect on human cells, to detect any mutations, tumor or otherwise, which may be induced. APPENDIX A The charge density in a CDW can be written as follows: (Al)

P = Po+ Pi cos[2fcFir +
the condensate can assume two equivalent ground states, (A2)


<Mx)

COS ( —

| = 7T -


(A3)

502

150

100

50

> j§ c

0

0)

o CL

-50 J =0.75%

J =0.25%

-100

-150 0.1

0.2

0.3

0.4 /(A)

0.5

0.6

0.7

Figure 2. In this figure a semi-classical model was used. The trends of the semi-classical potential (7), left, and quantum potential (2), right, obtained exchanging the values of J with respect to Fig. 1. Tunneling does not appear to be amplified for those metals with a density of impurity J Ri 0.75%. The Morse potential was calculated at T = 295 K. The Coulomb barrier is higher in the case of pure metals ( J sa 0.25%).

which differ only in the sign of the charge, interpretable as arrays of ir solitons of alternating sign, each of which occupy a Lee-Rice domain of length r

1

_

-nCV

x

(A4)

where wp is the bond frequency and

C0 =

/ TO

x

H^

(A5)

is the velocity of the phasons. In a band model, the electron energy is

w;p i n

-Ei 16£ F

(A6)

and Eg = 2A where A represents the energy gap and Ep is the Fermi energy.

(A7)

503 T h e energy gap A assumes a value very close to the energy of the solitons, given by: E

(A8)

T h e probability of tunneling between the states 4>A and B in a Zener model (12) is given by exp(-2Kad),

(A9)

where d is the tunneling distance, such t h a t eEd = 2A.

(A10)

With

rewriting Eq. (A9) in the form P{E) = exp(—E0/E), E0 = ^

.

gives (A12)

References 1. F. Frisone, Deuteron interaction within a microcrack in a lattice at room temperature, Fusion Technol. 39, 260-265 (2001). 2. F. Frisone, Theoretical model of the probability of fusion between deuterons within deformed crystalline lattices with microcracks at room temperature, Fusion Technol. 40, 139-146 (2001). 3. F. Frisone, Can variations in temperature influence deuteron interaction within crystalline lattices? Nuovo Cimento 20(10), 1567-1580 (1998). 4. M. Rabinowitz, High temperature superconductivity and cold fusion, Mod. Phys. Lett. B 4 , 233 (1990). 5. D.M. Brink, Semi-classical methods for nucleus-nucleus scattering, In: P.V. Landshoff, W.H. McCrea, D.W. Sciama, and S. Weinberg (eds) 1985, p. 206. 6. J. Bardeen, Macroscopic quantum tunneling in quasi one-dimensional metals. II. theory, Phys. Rev. Lett. 55(9), (1985). 7. F. Frisone, Study on the probability of interaction between the plasmons of metal and deuterons. Nuovo Cimento 18 (11) 1279-1286 (1996). 8. W. Wonneberger, Effect of viscosity on collective zener tunneling in charge density wave system, Condens. Matter 50, 23-32 (1983). 9. H. Kyeong An, Analysis of deformed palladium cathodes resulting from heavy water electrolysis Fusion Technol. 27, 408 (1995).

N E W COOPERATIVE M E C H A N I S M S OF LOW-ENERGY N U C L E A R R E A C T I O N S U S I N G S U P E R LOW-ENERGY E X T E R N A L FIELD

F . A. G A R E E V A N D I. E. Z H I D K O V A Joint Institute for Nuclear Research, Dubna, E-mail: gareevQthsunl .jinr. ru

Russia

We propose a new mechanism of LENR: cooperative processes in the whole system, nuclei + atoms + condensed matter, can occur at a smaller threshold energies than the corresponding ones on free constituents. The cooperative processes can be induced and enhanced by low-energy external fields. The excess heat is the emission of internal energy and transmutations at LENR are the result of redistribution of inner energy of the whole system.

1. Introduction A review of possible stimulation mechanisms of low-energy nuclear reaction (LENR) is presented in Ref. 1. We have concluded that transmutation of nuclei at low energies and excess heat are possible in the framework of the known fundamental physical laws - the universal resonance synchronization principle, 2 and different enhancement mechanisms of reaction rates based on it are responsible for these processes.1 The super low energy of external fields, the excitation and ionization of atoms may play the role of a trigger for LENR. 3 We argue that the cooperative mechanism can explain how the electron volt domain can influence the nuclear mega electron volt domain. 3 Nuclear physicists are absolutely sure that this is cannot happen. Investigation of this phenomenon requires the knowledge of different branches of science: nuclear and atomic physics, chemistry, and electrochemistry, condensed matter and solid state physics. The puzzle of poor reproducibility is explained by the fact that LENR occurs in open systems and it is extremely sensitive to parameters of external fields and systems. The classical reproducibility principle should be reconsidered for LENR experiments. Poor reproducibility and unexplained results do not mean that the experiment is wrong. Our main conclusion is: LENR may be understood in terms of the known fundamental laws without any violation of the basic physics. The fundamental laws of physics should be the same in micro- and macrosystems. Let us start with the description of the hydrogen atom structure in different models. 504

505

1.1. The Hydrogen

Atom

We will describe very briefly the structure of a hydrogen atom using standard basic physics that is well established, both theoretically and experimentally in micro- and macrosystems. 1.2. The Bohr

Model

At the end of the 19th century it was established that the radiation from hydrogen was emitted at specific quantized frequencies. Niels Bohr developed the model to explain this radiation using four postulates: • An electron in an atom moves in a circular orbit about the nucleus under the influence of the Coulomb attraction between the electron and the nucleus, obeying the laws of classical mechanics. • Instead of the infinity of orbits which would be possible in classical mechanics, it is only possible for an electron to move in an orbit for which its orbital angular momentum L is integral multiple of h: L = nh,

n= 1,2,3,...

(1)

• Despite the fact that it is constantly accelerating, an electron moving in such allowed orbit does not radiate electromagnetic energy. Thus, its total energy E remains constant. Electromagnetic radiation is emitted if an electron, initially moving in an orbit of total energy E\, discontinuously changes its motion so that it moves in an orbit of total energy Ef. The frequency u of the emitted radiation is equal to the quantity E\ - E{ v* = — j — ,

(2)

where h is Planck's constant. The electron is held in a stable circular orbit around a nucleus. The Coulomb force is equal to the centripetal force, according to Newton's second law e2 _ mv2 where r is the radius of the electron orbit and v is the electron speed. The force is central; hence from the quantization condition (1) we have L = |r —>p| =- mvr = nh.

(4)

er solving Eqs. (3) and (4) we have n2h2 e2 n ao. v = —, r= nh me2 Following Eq. (3)-the kinetic energy is equal toi e2

1 Ek= mv2

2

=

Tr>

(5)

(6)

506

and hence the total energy is 2

9

P

9

P

P

E = Ek + V = ^ - - - = ~ . (7) 2r r 2r Having r from Eq. (5) one can write the expression for the energy levels for hydrogen atoms

E==

(8)

-w^>

the same results were further obtained by quantum mechanics. Using the angular momentum quantization condition L = pr = nh/2w and Louis de Broglie's relationship p = h/\ between momentum and wavelength one can get 2irr = nX. (9) This means that the circular Bohr orbit is an integral number of the de Broglie wavelengths. The Bohr model is actually only accurate for a oneelectron system. 1.3. The Hydrogen

Atom

in Classical

Mechanics

Is it possible to understand some properties of a hydrogen atom from classical mechanics? The Hamiltonian for a hydrogen atom is

H = ^p- + ^--j^-r 2

2

\rp-fe\

(10) V

;

All notations are standard. The definition of the center of mass is mprp + mere = 0

(11)

and the relative distance between electron and proton is f=fp-re.

(12)

Equations (10)-(12) lead to the results: me r, re — p mp + me (ur2 2

mp mp + me''

e2 r '

(13)

(14)

where mpme

(15)

77ip + m e

The Hamiltonian (14) coincides with the Hamiltonian for the fictitious material point with reduced mass [i moving in the external field —e2/r. If we know the trajectory of this fictitious particle f = f(t), then we can reconstruct the trajectories of electron and proton using equations (13) r P (t) =

f ^ (t), mp + me

fe(t) =

^—f%t)mp + me

(16)

507

It is evident from (16) that the proton and electron move in the opposite directions synchronously. So the motions of proton, electron, and their relative motion occur with equal frequency (17) over the closed trajectories scaling by the ratio Ve_ _ mp v&_ _ m^ v-n me' v.. mR' xp

,ll,e

U^

llbe

vn

U-p

Vj^ _ mp m„

(18a)

//(.^

Schelaev4 proved that the frequency spectrum of any motion on ellipse contains only one harmonic. We can get from (16) that Pp = P,

Pe = -P,

(18b)

where — P\ = m\r\. All three impulses are equal to each other in absolute value, which means the equality of AD(p) = AD(e) = AD0*) = hAP-

(19)

Conclusion: Therefore, the motions of proton and electron and their relative motion occur with the same Frequency, Impulse (linear momentum) and the de Broglie wavelength. All motions are synchronized and self-sustained. Therefore, the whole system -hydrogen atom is nondecomposable to the independent motions of proton and electron despite the fact that the kinetic energy ratio of electron to proton is small:

# 4 4 = 4-46 xlCT4.

-Ek(p) This means that the nuclear and the corresponding atomic processes must be considered as a unified entirely determined whole process. For example, Weisskopf 5 came to the conclusion that the maximum height H of mountains in terms of the Bohr radius a is equal to -=2.6xl014, a and water wave lengths A on the surface of a lake in terms of the Bohr radius is equal to A 7 - « 2TT x 107. a Let us introduce the quantity / = rv, which is the invariant of motion, according to Kepler's second law, then \iv =

= —, r r and we can rewrite Eq. (14) in the following way: uf2 e2 U=M---. 2r2 r

(20)

(21) '

y

508

We can obtain the minimal value of (21) by taking its first derivative over r and setting it equal to zero. The minimal value occurs at M/

2

9

(22)

'

and the result is " m i n = -C'min =

—

e4 7;

~p^ •

(2o)

The values of invariant of motion vf (in MeV*s) can be calculate from (23) if we require the equality of Em\n to the energy of the ground state of a hydrogen atom fj,f = iivr = 6.582118 x 1(T 22 = h,

(24)

Conclusion: The Bohr quantization conditions were introduced as a hypothesis. We obtain these conditions from a classical Hamiltonian requiring its minimality. It should be strongly stressed that no assumption was formulated about trajectories of proton and electron. We reproduced exactly the Bohr result and modern quantum theory. The Plank constant h is the Erenfest adiabatic invariant for a hydrogen atom: \ivr = H. Let us briefly review our steps: • We used a well-established interaction between proton and electron. • We used a fundamental fact that the total energy = kinetic energy + potential energy. • We used Kepler's second law. • We used usual calculus to determine the minimum values of H. • We required the equality of Em[n to the energy of the ground state of hydrogen atom. Classical Hamiltonian + classical interaction between proton and electron + classical second Kepler law + standard variational calculus, together these well established steps in macrophysics reproduce exactly the results of microphysics; that is, the Bohr model and modern quantum theory (Schrodinger equation). We have not done anything spectacular or appealed to any revolutionary and breakthrough physics. Using the Newton equation with well-established interactions Gryzinski 6 proved that atoms have the quasicrystal structure with definite angles: 90°, 109°, and 120° which are the well-known angles in crystallography. 2. Nuclei and Atoms as Open Systems (1) LENR may be understood in terms of the known fundamental laws without any violation of basic physics. The fundamental laws of physics should be the same in micro- and macrosystems. (2) Weak and electromagnetic interactions may show a strong influence of the surrounding conditions on the nuclear processes.

509

(3) The conservation laws are valid for closed systems. Therefore, the failure of parity in weak interactions means that the corresponding systems are open systems. Periodic variations (24 h, 27, and 365 days in beta-decay rates indicate that the failure of parity in weak interactions has a cosmophysical origin. Modern quantum theory is the theory for closed systems. Therefore, it should be reformulated for open systems. The closed systems are idealization of nature, they do not exist in reality. (4) The universal resonance synchronization principle is a key issue to make a bridge between various scales of interactions and it is responsible for selforganization of hierarchical systems independent of substance, fields, and interactions. We give some arguments in favor of the mechanism - ORDER BASED on ORDER, declared by Schrodinger in Ref. 7, a fundamental problem of contemporary science. (5) The universal resonance synchronization principle became a fruitful interdisciplinary science of general laws of self-organized processes in different branches of physics, because it is the consequence of the energy conservation law and resonance character of any interaction between wave systems. We have proved the homology of the atom, molecule and crystal structures including living cells. Distances of these systems are commensurate with the de Broglie wavelength of an electron in the ground state of a hydrogen atom, it plays the role of the standard distance, for comparison. (6) First of all, the structure of a hydrogen atom should be established. A proton and electron in a hydrogen atom move with the same frequency that creates attractive forces between them; their motions are synchronized. A hydrogen atom represents the radiating and accepting antennas (dipole) interchanging energies with the surrounding substance. The sum of radiate and absorb energy flows by electron and proton in a stable orbit is equal to zero 8 - the secret of success of the Bohr model (nonradiation of the electron in a stable orbit). "The greatness of mountains, the finger sized drop, the shiver of a lake, and the smallness of an atom are all related by simple laws of nature." 5 (7) These flows create standing waves due to the resonance synchronization principle. A constant energy exchange with substances (with universes) create stable auto-oscillation systems in which the frequencies of external fields and all subsystems are commensurate. The relict radiation (the relict isotropic standing waves at T = 2.725 K - the Cosmic Microwave Background Radiation (CMBR)) and many isotropic standing waves in cosmic medium 9 should be results of self-organization of the stable hydrogen atoms, according to the universal resonance synchronization principle, that is a consequence of the fundamental energy conservation law. One of the fundamental predictions of the Hot Big Bang theory for the creation of the Universe is CMBR. (8) The cosmic isotropic standing waves (many of them are not discovered yet) should play the role of a conductor responsible for stability of elementary

510

particles, nuclei, atoms, . . . galaxies ranging in size more than 55 orders of magnitude. (9) The phase velocity of standing microwaves can be extremely high; therefore all objects of the Universe should get information from each other almost immediately using phase velocity. The aim of this paper is to discuss the possibility of inducing and controlling nuclear reactions at low temperatures and pressures by using different low-energy external fields and various physical and chemical processes. The main question is the following: is it possible to enhance LENR rates by using low and extremely low-energy external fields? The review of possible stimulation mechanisms is presented in Refs. 1 and 5. We will discuss new possible ways to enhance LENR rates in condensed matter. 3. LENR in Condensed Matter The modern understanding of the decay of the neutron is n —> p + e~ + ve.

(25)

The energetics of the decay can be analyzed using the concept of binding energy and the masses of particles by their rest mass energies. The energy balance from neutron decay can be calculated from the particle masses. The rest mass difference 0.7823 MeV/c 1 between neutron and (proton + electron) is converted to the kinetic energy of proton, electron and neutrino. The neutron is about 0.2% more massive than a proton, an energy difference is 1.29 MeV. A free neutron will decay with a half-life of about 10.3 min. Neutron in a nucleus will decay if a more stable nucleus results otherwise neutron in a nucleus will be stable. A half-life of neutron in nuclei changes dramatically and depends on the isotopes. The capture of electrons by protons is possible p + e~ —» n + z/e,

(26)

but for free protons and electrons this reaction has never been observed which is the case in nuclear + atomic physics. The capture of electrons by protons in a nucleus will occur if a more stable nucleus results. 3.1. Cooperative

Processes

The processes (25) and (26) in LENR occur with individual nucleons and electrons. In these cases the rest mass difference is equal to 0.7823 MeV/c . In the case of neutron decay the corresponding energy (Q = 0.7823 MeV) is converted to kinetic energies of proton, electron, and antineutrino. In the case of the capture of electrons by protons the quantity Q = 0.7823 MeV is a threshold electron kinetic energy under which the process (26) is forbidden for free proton and electron.

511

We have formulated the following postulate: The processes (25) and (26) in LENR occur in the whole system: cooperative processes including all nucleons in nuclei and electrons in atoms, in condensed matter. In these cases the threshold energy Q can be drastically decreased by internal energy of the whole system or even more - the electron capture by proton can be accompanied by emission of internal binding energy - main source of excess heat phenomenon in LENR. The processes (25) and (26) are weak processes. A weak interaction which is responsible for electron capture and other forms of beta decay is of a very short range. So the rate of electron capture and emission (internal conversion) is proportional to the density of electrons in nuclei. This means we can manage the electron-capture (emission) rate by the change of the total electron density in the nuclei using different low energy external fields. These fields can play the role of triggers for extracting the internal energy of the whole system or subsystems, changing quantum numbers of the initial states in such a way that forbidden transitions become allowed ones. The distances between proton and electron in atoms are of the order 10 ~6 — 10~5 cm and any external field decreasing these distances, even for a small value, can increase the process (26) in nuclei in an exponential way. Therefore, the influence of an external electron flux (discharge in condensed matter: breakdown, spark, and ark) on the velocity's processes (25) and (26) can be of great importance. The role of external electrons is the same as the catalytic role of neutrons in the case of the chain fission reactions in nuclei: neutrons bring to nuclei binding energies (about 8 MeV) which enhance the fission rates by about 30 orders. 4. Predicted Effects and Experimentum Cruices Postulated enhancement mechanism of LENR by external fields can be verified by the Exprimentum Cruices. We 8 predicted that natural geo-transmutation in the atmosphere and earth occur in the regions of a strong change in geo-, bio-, acousticand electromagnetic fields. The various electrodynamic processes at thunderstorms are responsible for different phenomena: electromagnetic pulses, 7-rays, electron fluxes, neutron fluxes, and radioactive nuclei fluxes. 4.1. Neutron

Production

by

Thunderstorms

The authors of Ref. f0 concluded that a neutron burst is associated with lighting. The total number of neutrons produced by one typical lighting discharge was estimated as 2.5 x 10 10 . 4.2. Production

of Radiocarbon

and Failing of Radiocarbon

Dating

The radiocarbon dating is based on the decay rate of radioactive isotope 14 C which is believed to be constant irrespective of the physical and chemical conditions.

512

The half-life of radiocarbon 14 C is 5730 years. A method for historical chronometry assuming was developed that the decay ratio of 14 C and its formation are constant in time. It was postulated that 14 C is formed only by the cosmic ray neutrons 14

N(n,p) 1 4 C.

(27a)

Radiocarbon dating is widely used in archeology, geology, antiquities,... There are over 130 radiocarbon dating laboratories. The radiocarbon method of dating was developed by Willard F. Libby who was awarded the Nobel prize in Chemistry for 1960. The radiocarbon method do is not take into account the following facts which have been established recently: • The neutron production by thunderstorms. 10 • The Production of radiocarbon by lighting bolts. 11 Let us consider the reaction 14

N + e - ^ 1 4 C + ^e,

(27b)

the Tfc(e) = 165.41 keV is the threshold energy which should by compared with 782.3keV for process (26). Production of radiocarbon by lighting bolts was established in Ref. 11. Unfortunately, this means FAILING of RADIOCARBON DATING. 4.3. Production

Radiophosphorus

by

Thunderstorms

The life-times of f§P and f|P are equal to 14.36 and 25.34 days, respectively. They were found in rain-water after thunderstorms. 12 Production of the radiophosphorus by thunderstorms can be understood in the following way: r6S + e-^ltP

+ ve,

(28)

fjjS + e - ^ P

+ i/e,

(29)

thresholds of these processes are equal to 1.710 and 0.240 MeV, respectively. The precipitation of MeV electrons from the inner radiation belt 13 and enhancement of the processes by lighting are possible. 4.4. LENR Stimulated

by Condensed

Matter

Discharge

Let us consider the condensed matter discharge (breakdown, spark, and arc) using the different electrodes. There are the following processes: (1) The electrode is Ni. Orbital or external electron capture iNi(68.27%) + e~ -> lfCo(70.78 days) + i/e.

(30)

The threshold Q\ = 0.37766 keV of this reaction on Ni should be compared with the threshold Qi = 0.7823 energy for electron capture by free protons:

513 Q2/Q1 ~ 2. The velocity of orbital electron capture can be enhanced by the discharge. (2) Orbital or external electron capture pCo(70.78 days) + e" -> ^Fe(0.28%) + ue,

(31)

with emission of energy Q2 = 2.30408 MeV. (3) Double orbital or external electron capture iNi(68.27%) + 2e" -> ^Fe(0.28%) + 2ue,

(32)

with emission of energy Qs = 1.92642 mostly by neutrinos. The proposed cooperative mechanism of LENR in this case can be proved in an extremely simple way: presence of radioactive 27C0 and enriched isotope of |gFe. This mechanism can give possibilities to get a way of controlling the necessary isotopes and excess heat. 4.5. Neutrinoless

Double Beta

Decay

1

As we know, the physical roles of electron and neutrino for LENR in condensed matter has not been investigated in detail up to now despite the fact that weak processes in nuclei are well understood. The double beta decay is the rarest spontaneous nuclear transition, in which the nuclear charge changes by two units while the mass number remains the same. Such a case can occur for the isobaric triplet A(Z,N), A(Z±l,N=fl), A(Z±2,NT%), in which the middle isobar has a greater rest mass than the extreme ones, and the extremes are the nuclei with the even Z and N. The usual beta-decay transferring a given nucleus into another via an intermediate nucleus is energetically forbidden. The double beta decay in nuclei can proceed in different modes: 14 • The two neutrino decay mode 2v(3j3 A(Z,N)

-> A(Z + 2,N-2)

+ 2e~+2ve)

(33)

which is allowed by the Standard Model of particle physics. The total kinetic energy of two emitted electrons present continuous spectra up to £ m a x . • The neutrinoless mode Ov/3/3 A(Z, N) -> A(Z + 2, N - 2) + 2e",

(34)

which requires violation of a lepton number. The total kinetic energy of two emitted electrons is equal to Emax. Two neutrinos in the mode 2v(3/3 carry out almost all emitted energies, which is useless for practical applications; therefore, this mode is not important for us. A fundamental question is: does the neutrinoless double beta decay exist or not (for the review of the history see Ref. 14). The emerged energies in the neutrinoless 0^/3/3 mode are easily detected for practical use but these are the rarest spontaneous nuclear transitions (T « 10 18 - 1030 years). Is it possible to enhance the decay rate?

514

Above and in Refs. 1-3, we have discussed the cooperative and resonance synchronization enhancement mechanisms of LENR. Some of the low energy external fields can be used as triggers for starting and enhancing of exothermic LENR. It is natural to expect that in the case of beta-decay (capture) the external electron flux with high density, or a laser of high intensity, or any suitable external fields should play this role. Any external field shortening distances between protons in nuclei and electrons in atoms should enhance beta-decay (capture) or double-beta decay (capture). There are a great number of experiments in Japan, Italy, Russia, US, India, China, Israel, and Canada in which cold transmutations and excess energy were measured (see http://www.lenr-canr.org). It is very popular to use Ni, Pd, Pt, and W as electrodes in the condensed matter discharge (breakdown, spark, arc, and explosion) experiments. Let us consider the case Pd electrodes. The difference of the rest mass of m Qe°Pd) - m Q|°Cd) = 1.9989 MeV/c 2 , therefore, the external field can open the channel 46°Pd —> 4g°Cd with Q = 1.9989. The experimental data 1 5 seem to confirm such expectations. Therefore, expensive and time-consuming double beta decay experiments can be performed in cheap and short-time experiments by using suitable external fields. This direction of research can open production of new elements (utilization of radioactive waste) and excess heat without of ecological problem. A careful analysis of the double beta decay shows that the 2e~ cluster can be responsible for the double beta decay. The difference between the rest mass 56°Ba and 52°Te, which is equal to 92.55 keV, indicates the possibilities to capture the 4e~ cluster by j ^ B a . It is a full analogy with the Iwamura reactions. 16 The lack of financial support and the ignorance from the whole physical society of LENR lead to catastrophes. The mechanism of shortening the runaway of the reactor at the Chernobyl Nuclear Power Plant and catastrophes induced by the High Frequency Active Auroral Research Program (HAARP) program is based on our postulated cooperative resonance synchronization mechanism. The same mechanism should be responsible for the International Experimental Fusion Reactor (ITER) explosion in future.

5. Conclusion We proposed a new mechanism of LENR: cooperative processes in whole the system - nuclei + atoms + condensed matter can occur at a smaller threshold energies than the corresponding ones on free constituents. The cooperative processes can be induced and enhanced by low energy external fields. The excess heat is the emission of internal energy and transmutations at LENR are the result of redistribution of inner energy of the whole system.

515

References 1. F.A. Gareev, I.E. Zhidkova, and Yu.L. Ratis, Preprint JINR P4-2004-68, Dubna, 2004 (in Russian); in: Proceedings of the 11-th Russian Conference on Cold Nuclear Transmutation of Chemical Elements and Ball Lighting, Dagomys, city Sochi, September 28 - October 5, 2003, Moscow 2004, p. 169. 2. F.A. Gareev, in: FPB-98, Novosibirsk, June 1998, p. 92; F.A. Gareev, G.F. Gareeva, in: Novosibirsk, July 2000, p. 161. 3. F.A Gareev, I.E. Zhidkova, and Yu.L. Ratis, in Program Abstracts on ICCF-11, Marseille: France: 2004, 31 October - 5 November; F.A. Gareev, I.E. Zhidkova, E-print arXiv Nucl-th/0505021 vl 8 May 2005; E-print arXiv nucl-th/0511092, Vol. I, 30 November 2005. 4. LA. Schelaev, FPV-2004 (Novosibirsk, 2004), Vol. II, p. 27. 5. V.F. Weisskopf, Am. J. Phys. 54 (2), 110 (1986). 6. M. Gryzinski, FPV-2004, Vol. I (Novosibirsk, 2004). 7. E. Schrodinger, What is Life? The Physical Aspects of the Living Cell (Cambridge University Press, Cambridge, 1967). 8. F.A. Gareev, I.E. Zhidkova, and Yu.L. Ratis, Appl. Phys. J. N 3 , 25 (2005). http://www.iscmns.org/siena05/program.htm. 9. A.M. Chechelnitsky, E-print arXiv: physics/0105056 (2001). 10. L.S. Bratolyubova-Tsulukidze et al, Adv. Space Res. 34, 1815 (2004). 11. L.M. Libby and H.R. Luken, J. Geophys. Res. 78, 5902 (1973). 12. LP. Selinov, Isotops (Nauka, Moscow, 1970). 13. U.S. Unan et al, Geophys. Res. Lett. 15, 172 (1988). 14. H.V. Klapdor-Kleingrothaus and A. Staudt, Teilchenphysik Ohne Besschleuniger (B.G.Teubner, Stutgart, 1995). 15. LB. Savvatimova and A.D. Senchukov, ICCF6 2, 575 (1996). 16. Y. Iwamura, ICCF11 (2005). 17. O.R. Grogoryan, A.V. Sinyakov, and S.I. Klimov, Adv. Space Res. 20, 389 (1997). 18. L.S. Bratolyubova-Tsulukidze et al., Cosmic Res. 39, 602 (2001).

P O L Y N E U T R O N THEORY OF T R A N S M U T A T I O N

J O H N C. F I S H E R 600 Arbol Verde, Carpinteria, CA 93013, E-mail: [email protected]

USA

Polyneutron theory is applied to nuclear transmutation. Implications of the theory are compared with experiment. Additional more definitive experiments are suggested.

Polyneutron theory postulates that large clusters of neutrons are bound and stable against strong decay and that their interactions with ordinary nuclei are responsible for a new class of low-temperature nuclear phenomena. It is postulated that these clusters, also termed polyneutrons or neutron isotopes, grow to include hundreds of neutrons in chain reactions fueled by isotopes such as 2 H, 1 8 0 , and 7 Li. 1 It is anticipated that an ordinary nucleus AX and a polyneutron B n can bind to form a composite AXBn that subsequently decays by transfers or exchanges of nucleons between its components. The present analysis focuses on composite formation and on the transmutations that result from composite decay. I assume that the neutrons in polyneutrons are paired with the BCS symmetry first described for electrons in superconductors, 2 and that breaking a pair requires so much energy that odd-numbered polyneutrons can be produced only in reaction with deuterium. In the reaction 2An + 2 H —> 2A+1n + 1 H transmutation of H makes available up to 5.847 MeV for adding the odd neutron. If the mass excess of 2A+1n were to exceed that of 2An by (say) 5 MeV, the reaction forming it would be exothermic by 0.847 MeV. On the other hand the reaction 2 A + 1 n + 2 H -> 2A+2n + *H would be exothermic by 10.847 MeV with a much larger cross section, and in a chain reaction where polyneutrons are growing and fissioning in interaction with 2 H, as in the experiments of Iwamura et al.,3~5 the concentration of even polyneutrons is expected to substantially exceed that of odd ones. Hence as a first approximation I consider only even polyneutrons. Transmutations associated with composite formation and decay are expected to occur at differing rates. Formation is expected to be the limiting rate, depending as it does on the very small concentration of polyneutrons. Strong reactions that do not require associated beta decay or electron capture are assumed to be most rapid, and to occur during composite formation. Weak reactions that require associated beta decay or electron capture are assumed to be slower. Weak reactions that require associated double beta decay or double electron capture are assumed to be slower still, followed by reactions that require three or more associated weak 516

517

reactions. With the foregoing assumptions the following procedure determines the sequence of transmutations according to the present status of the theory: Step 1. Consider a starting element G X for which we desire to know the isotopes to which it may be transmuted by interaction with polyneutrons. The first step is formation of a composite ^X B n in a reaction such as ^X + D n —> ^X B n + G+D_yl B ^ n . Such a reaction can only occur in an environment where polyneutrons are continuously being created, as in the active region of an ongoing chain reaction. In a newly formed composite the value of A is that for which the composite is stable against the strong reactions ^X B n —> A+1^.XB~Nn for all positive and negative even values of N. These reactions must be endothermic. The energy they release is EQ = A(-^X) — /S.(A+NZX) + NS, where S represents half the change in polyneutron mass excess associated with adding a pair of neutrons, 5 = (l/2)[A( j 4 + 2 n) —A(' 4 n)]. The reaction is exothermic for EQ > 0. Are any such transfers exothermic? If yes, choose the most exothermic among N = ±2, ±4, ± 6 , . . . , and go to Step 2. If no, go directly to Step 2. Step 2. Represent the output of the previous step by ^X. Is there an isotope zi'i'Y of the element having one more or one less proton than AX that can be reached by exchange or transfer of nucleons within the composite? (Each of these reactions requires an associated beta decay or electron capture.) The energy released is Ei = A(^X) —A( J±(Y) + N5. Are any such transfers exothermic? If yes, choose the most exothermic among z = ± 1 and N = 0, ±2, ± 4 , . . . , and return to Step 2. If no, go to Step 3. Step 3. Represent the output of the previous step by AX. Is there an isotope A ^±2^ of the element having two more or two fewer protons than AX that can be reached by exchange or transfer of nucleons within the composite? (Each of these transfers requires two associated beta decays or electron captures.) The energy released is E^ = A(AX) — A( 0"±2Y) + NS. Are any such transfers exothermic? If yes, choose the most exothermic among z ± 1 and N = 0, ±2, ± 4 , . . . , and go to Step 2. If no, continue with three or more associated weak decays, or stop if transmutations with such decays are neglected. The beta decays in Steps 2 and 3 can be imagined as occurring in the polyneutron in association with transfer of the resulting proton to the ordinary nucleus. For N = 0 each proton so formed exchanges with a neutron from the ordinary nucleus, accelerating the rate of N = 0 beta decays to match that of N ^ 0 decays. Electron captures can be imagined as occurring in association with transfer of a proton from the ordinary nucleus to the polyneutron. For N = 0 each proton so transferred exchanges with a neutron from the polyneutron, accelerating the rate of N = 0 electron captures to match that of N ^ 0 captures. Examples of reactions and their energies are shown here in more detail. No beta decay:

fXBn^A+NzXB~Nn E0 = A(AX)

- A(A+N2X)

+ E0, + N5.

518

Single beta decay:

Single electron capture: ^ n ^ ^ Y ^ n Ex = A(AX)

+ i^,

- A( A z t?Y) + N6.

Double beta decay: *XBn^Az++N2YB-Nn E2 = A(AX)

- A(A\N2Y)

+ E2, + N5.

Double electron capture: ^ X B n ^ A z t ^ Y B " i v n + £;2,

E2 = A{AX) - A ( ^ Y ) + NS. In my calculations, I assume that 5 is independent of A with the value S = 1.143 as tentatively determined from transmutation of 138 Ba to 150 Sm. With this value of 5, and assuming that the binding energy of a composite is independent of the properties of its components, it is possible to calculate the transmutation chain for any starting isotope. (The assumption of constant 5 holds only approximately over a limited range of values of A, and the assumption of a constant binding energy for composites ignores the influence of shell structure of the ordinary nucleus and of the sizes of both components. These questions should be addressed in a more realistic treatment of the theory.) Transmutation chains can be more easily visualized by simplifying the notation. Abbreviate the composite AX n as (^X) where the size of the polyneutron component is understood. Then as an example the transmutation 139 La n —> 141 Ce ~~ n is abbreviated ( 139 La) —> ( 141 Ce). With this notation, and neglecting transmutations with three or more associated weak interactions, the transmutation chain for 139 La is 139

La + An -+ ( 139 La) - ( 141 Ce) -+ ( 141 Pr) -

( 143 Nd).

In addition to these decay channels, each composite has a side channel that frees the ordinary nucleus and substitutes a helium nucleus, typified by 141

CeAn^4HeA~4n +

141

Ce.

In consequence, accompanying the composite decay chain there is in its wake a residual of free isotopes 141 Ce, 141 Pr, 143 Nb whose numbers depend on the relative magnitudes of the side channels. To recapitulate, I assume that formation of the initial composite ( 139 La) is the rate-limiting step. Once a composite has formed, I assume that it decays rapidly through the chain leaving behind a residue of free

519

transmuted isotopes that can be revealed by mass spectrometry. Shortly after composite formation ceases, signals for 139 La, 141 Ce, 141 Pr, and 143 Nb would be revealed; perhaps with the largest signal for 143 Nb if the side reactions are small and most composites survive to the end, or perhaps with the smallest signal if the side reactions are larger and deplete the composites as they pass through successive transmutations. At a later time after composite formation ceases mass spectrometry would detect signals only for 139 La, 141 Pr, and 143 Nb with an enhanced 1 4 1 Pr signal from beta decay of 141 Ce with its 33 day half life. I now consider the transmutations investigated by Iwamura et al.3~5 Transmutation of 138 Ba is reported to lead to 150 Sm. The decay chain predicted by polyneutron theory is 138Ba

+

An _+ ( 1 3 8 B a ) _> ( 1 4 0 C e ) _> ( 1 4 4 N d ) _>

(150gm)

^

(

158Gd)

leaving residual amounts of 140 Ce, 144 Nd, 150 Sm, 158 Gd, and so on. It leaves a residue of free 150 Sm nuclei only for values of S that lie in the narrow range 1.142 < S < 1.144. This is the basis for my assumption that S = 1.143. Transmutation of 88 Sr is reported to lead to 96 Mo. The reaction chain predicted by the theory is 88

Sr + An -+ ( 90 Sr) -> ( 92 Y) -+ ( 96 Zr) ^ ( 96 Nb) ^ ( 100 Mo) -+ ( 102 Tc) ^ • • •

leaving residual amounts of 90 Sr, 92 Y, 96 Zr, 96 Nb, 100 Mo, 102 Tc, and so on. The 96 Nb residue decays to 96 Mo with a half life of 23 h. During composite formation, mass spectrometry will reveal a signal at mass 96 from residual 96 Zr and 96 Nb, along with 96 Mo from decay of 96 Nb. A few days after composite formation has ceased the mass signal will come from 96 Zr and 96 Mo with an enhanced 96 Mo component from decay of 96 Nb. A Mo signal from XPS will be obtained from the 96 Mo and 100 Mo residuals. Transmutation of 133 Cs is reported to lead to 141 Pr, and to as yet unidentified isotopes with intermediate masses between 133 and 141. The theory predicts 133

Cs+A

n - ( 137 Cs) -+ ( 137 Ba) - ( 139 La) - ( 141 Ce) -+ ( 141 Pr) ^ ( 143 Nd)

leaving residual amounts of 137 Cs, 137 Ba, 139 La, 141 Ce, 141 Pr, and 143 Nd. The latter portion of this chain was treated in the example above for transmutation of 139 La, in which a signal for 1 4 1 Pr arose from the 1 4 1 Pr residual plus additional 141 Pr from decay of 141 Ce. Finally transmutation of 137 Ba was reported to lead to a signal at mass 149, tentatively attributed to 149 Sm although no XPS signal for Sm could be detected. Theory predicts the decay chain 137Ba

+

An_^

(137Ba)

^

(139La)

^

(141Ce)

^

(141pr)

^

(

143Nd)

leaving residual amounts of 139 La, 141 Ce, 141 Pr, and 143 Nd as for transmutation of 133 Cs. No signal for Sm is expected. (It may be that the reported mass 149 signal represents 137 Ba 12 C or 1 3 3 Cs 1 6 0 from contamination by carbon or cesium during the transmutation process.)

520 Overall the agreement between theory and the experiments of Iwamura et al. is suggestive but not definitive. Consideration of other t r a n s m u t a t i o n chains identifies experiments t h a t could be more definitive. T h e parameter choice 5 = 1.143 implies t h a t 2 0 7 P b and 2 0 8 P b are absolutely stable, all potential t r a n s m u t a t i o n s involving any number of possible associated weak interactions being endothermic. Looked at another way, these P b isotopes are the final products of t r a n s m u t a t i o n of every starting element, provided only t h a t sufficient time is allowed. Nuclei lighter t h a n lead t r a n s m u t e by b e t a decay alone, as in 205 T 1 +

An^(205T1)^(207pb)>

Nuclei heavier t h a n lead t r a n s m u t e by electron capture alone, as in 209

Bi + ^ n ^ ( 2 0 9 B i ) ^ ( 2 0 7 P b ) .

Lead isotopes 2 0 4 P b and 2 0 6 P b t r a n s m u t e by neutron transfer in association with composite formation, as in 204

Pb+

A

206

Pb+

A

n^ n^

(208Pb), (208Pb).

These transmutations are ideal testing grounds for the theory. T h e y suggest t h a t polyneutrons can induce transmutations where the final nucleus differs from the starting nucleus by addition of a proton and a neutron, by subtraction of a proton and a neutron, or by addition of two or four neutrons. Each of these reactions requires only a single step from composite formation to the final 2 0 7 P b or 2 0 8 P b product. Because the product is stable, one-to-one substitution of 2 0 7 P b for 2 0 5 T1 and for 2 0 9 Bi should be seen, as should substitution of 2 0 8 P b for 2 0 4 P b and 2 0 6 P b . T h e predictions of the theory are definite and clear-cut, although minor corrections can be expected when the analysis is extended to include odd polyneutrons. If the predictions are borne out by experiment the credibility of the theory will be enhanced. If not the theory will face a crisis.

References 1. 2. 3. 4.

J. C. Fisher, Fusion Tech. 34, 66 (1998). J. Bardeen, L. N. Cooper, and J. R. Schrieffer, Phys. Rev. 108, 1175 (1957). Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys., 4 1 , 4642 (2002). Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi, Proc. ICCF 11 (World Scientific Inc., 2006), 339. 5. Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, and T. Ishikawa, Proc. ICCF 12 (World Scientific Inc., 2006), to be published.

T H E T H E R M A L C O N D U C T I O N FROM THE C E N T E R S OF T H E N U C L E A R R E A C T I O N S IN SOLIDS

KEN-ICHI TSUCHIYA Department of Chemical Science and Engineering, Tokyo National College of Technology, 1220-2 Kunugida, Hachioji, Tokyo 193-0997, Japan E-mail: [email protected]

If nuclear reactions happen in solids, heat generated from the reaction center is diffused. In this study, the thermal conduction from the centers of a DD reaction in solids induced by the Bose—Einstein condensation is considered. The voids in solids are assumed as the sites of the reaction centers. The equations of the thermal conduction are solved using Fourier expansion. The calculated results show the rapid temperature relaxation. This means that nuclear reactions in solids do not induce thermal explosions.

1. D D Reaction Rate in Solid In the previous work,1 DD reaction rate in Pd void is calculated applying the equivalent linear two-body (ELTB) method. The rate is determined by the ELTB ground state wave function ^> for N identical charged Bose nuclei as

R=

m¥)—'

(1)

where imaginary part of Fermi pseudopotential V? 2 ' 3 is written as ImV£

Ah = -—Sin-rj).

(2)

The short-range interactions of nuclear forces between two Bose nuclei are introduced by using 6 function. 2 ' 3 The constant A is given by the Bohr radius TB and the S factor of the nuclear reaction between two nuclei as A = 2Sr-e,/-Kh. The ELTB solution also gives the critical temperature Tc of Bose-Einstein condensation (BEC) by well-known formula which is written as h2

(

n

\2/3

where n is the local number density of Bose particles and (,{Z) is the Riemann's zeta function. The probability of the ground-state occupation is given by / ji \

2

/3

f2 = 1 - f - J

forT
(4)

522

If the ground state occupation for T < Tc is taken into account the fusion rate is given by M l When T > Tc, no nuclear reactions happen because fi = 0. The trapped site for a deuteron cluster is shown in Fig. 1. The calculated results for Tc and R are listed in Table 1. When N > 4 with using nonlinear screening, 4,5 Tc is higher than the room temperature. The ELTB solution is plotted in Fig. 2 for the case of the 5-deuteron cluster trapped at VacO.

Figure 1. The structure of VacO in fee lattice. The black and the gray circles mean occupied and unoccupied lattice points, respectively. These defects construct octahedral void, which is called VacO in this paper. Table 1. The nuclear reaction rate R(10 7 s _ 1 ) and the critical temperature T C (K) for the case of N deuterons rapped at VacO in Pd Nonlinear screening

Thomas- Fermi screening TV

Tc

R

Tc

R

3 4 5 6 7

56 66 76 86 95

2.1 3.5 5.0 6.7 8.6

257 329 403 480 558

33.8 66.4 108.6 160.2 221.3

2. Thermal Conduction If nuclear reactions happen in solids, heat generated from the reaction center is diffused. In this study, the thermal conduction from the center of a DD reaction in Pd is estimated. The equation of the thermal conduction in solid is written as dT

~m

fcV2T,

(5)

where T is the deviation of the temperature from the equivalent value and t is the time from a reaction. The constant k is defined as k=

K/Cp,

(6)

where constants K, C, and p mean the thermal conductivity (75.5 J / s m K ) , the specific heat (25 J/mol K) and the density (12.0 g/cm 3 = 12.0 x 10 6 /166.4mol/m 3 ),

523

;

1

! p/x 2

1I

£

i2

i

i

<

M

5 •

-1 -

y

m

---•

1 .--~"' 10

- - Total

,''15

20

" ~ ;~ ~

Figure 2. The ELTB solution for the system including five-deuterons in VacO in fee Pd. Nonlinear screening potential is used as the DD interaction. The nondimensional quantity x is defined as x = ^mujjhp, where to = 0.86 X 1 0 1 4 s _ 1 and p2 = Ejrf. The solid line means the ELTB solution. The dashed lines mean each potential normalized by |e| = | — 409|. (p/x 2 ; component divided from the operators for kinetic energy, qf/x; screened DD repulsion potential. E m ; the lattice summation for the Coulomb potentials by host Pd ions (see Ref. 1))

respectively. The initial condition used for solving Eq. (5) is T = T0 in the dxdxd cube and T = 0 for otherwise. In this condition, the parameter d corresponds to the size of the deuteron cluster and the initial temperature is obtained by To =

E/CMo,

(7)

where constants E and MQ mean the energy generated from a DD reaction (23.8 MeV = 23.8 x 106 x 1.60 x 10" 1 9 J) and the number of moles in the d x d x d cube (4/Avogadro number mol), respectively. The periodic boundary condition used for solving Eq. (5) is written as for 0 <x < ±=4,

0 X(x)

T

l/3

0

for ±=* < x <

^

(8)

for £±4 < x < L,

and X{x) = X(x + L),

(9)

where X(x) is one of the divided components of T which is written as (10)

T(x,y,z,t)=X(x)Y(y)Z(z)U(t). A solution of Eq. (5) using Fourier expansion is written as T

Cnx coa(qxx)e-k'£tCnv

cos(qyy)e-k&Cnz

co^z)^^,

(11)

524

where constants are defined as 2n,'7r and 1/3 -l)n<2T0 • riiiT

(-'n

riiird sin •

(12)

L

The parameter L means distance between two neighboring reaction centers. This parameter is obtained by the well-known formula for the concentration of Shottky defect in solid. It is written as n/N = e~w/k*T,

(13)

where n, N, and w mean the number of defect, the number of total atoms and vacancy formation energy (~1 eV), respectively. Assuming the uniform distribution of the trapped sites, the parameter L is obtained by L

Q iu/3fe B T

(14)

4V3

where a is the lattice constant of fee Pd (3.89 A). As the temperature is increased, the concentration of the vacancy is increased and the mean distance between vacancies is decreased. They are shown in Figs. 3 and 5. The calculated result for the thermal conduction is plotted in Fig. 5. The rapid relaxation can bee seen in Fig. 5.

6 •

100

200

300

400

500

Temperature (K)

Figure 3. The temperature dependence of the vacancy concentration n/N, where n and N mean the number of the vacancy and the number of the total atom, respectively.

3. Conclusions (1) If a DD reaction happens in a void, temperature of the reaction center becomes extremely high. However rapid recovery from the high temperature is seen, because thermal conductivities of metals are high. For the case of Fig. 5, recovering time is smaller than 10~ 10 s. This is smaller than the inverse of the reaction rate 108.6 x 1 0 r s _ 1 (see Table 1).

525

E

0.005

0.000 >

„*_—.=—*».—™„«^™™™»_«^™_™, 250 300 350 400

Temperature (K) Figure 4.

The mean distance between the vacancies as a function of the temperature

(2) If iterative reactions happen, temperature raises slowly. This is shown in Fig. 6. For the case of 5-deuteron cluster trapped at VacO, Tc of BEC is 403 K (see Table 1). Seeing Fig. 6, temperature becomes higher then Tc after the 1.3 x 108 times iterative reactions. After that, local BEC in VacO is broken and DD reactions are stopped. This means that nuclear reactions in solid do not induce thermal explosions.

Figure 5. Thermal conduction from a center of a DD reaction. Position along the line x = y = z is normalized by the size of a deuteron cluster. In this case, d = 2.45 X 10~~ 10 (rn) for 5-deuteron cluster trapped at VacO. This corresponds to the initial temperature To = 3.85 x 10 9 (if).

526

420

400

_,

Tc=403 K

380

for five deuteron cluster trapped at VacO | a) a. E |2

360

340 320

300 0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

Iteration (x108)

Figure 6. The rise in temperature by the iterative DD reactions. In this case, the initial temperature is 300 K. For the case of 5-deuteron cluster trapped at VacO, T c of BEC is 403 K (see Table 1), which is shown by dashed line. After the 1.3 X 10 8 times iterative DD reactions, the temperature becomes higher than T c and BEC is broken.

References 1. K. Tsuchiya, Q u a n t u m s t a t e s of d e u t e r o n s in P d , Int. J. Hydrogen Energy 2 9 , 1513 (2004). 2. Y . E . K i m a n d A.L. Zubarev, Nuclear fusion for Bose nuclei confined in ion t r a p , Fusion Technol. 3 7 , 151 (2000). 3. Y . E . K i m a n d A.L. Zubalev, Equivalent linear t w o - b o d y m e t h o d for m a n y - b o d y p r o b lems. J. Phys. B: Atomic, Molecular and Optical Physics 3 3 , 3905 (2000). 4. H. H o h e n b e r g a n d W . K o h n , I n h o m o g e n e o u s electron gas, Phys. Rev. 1 3 6 , B864 (1964). 5. W . K o h n a n d L.J. S h a m , Self-consistent e q u a t i o n s including exchange a n d correlation effects, Phys. Rev. 1 4 0 , A1133 (1965).

F O U R - B O D Y RST G E N E R A L N U C L E A R W A V E F U N C T I O N S A N D MATRIX ELEMENTS

I R F A N C H A U D H A R Y A N D P E T E R L. H A G E L S T E I N Research

Laboratory

of Electronics, E-mail:

Massachusetts Institute of Technology, MA 02139, USA [email protected], [email protected]

Cambridge,

The inclusion of phonon exchange in a nuclear reaction is accomplished most easily when the associated matrix elements are written explicitly as a function of the nucleon spatial co-ordinates. We report on the wavefunctions and matrix elements for the special case of a T = 0 4-body deuteron—deuteron fusion reaction.

1. Introduction Physicists have long assumed that the dynamics of nuclear reactions in condensed matter proceeds fast enough that successful approximations can be obtained using a vacuum approximation. Such an approach has been widely successful for many decades in the case of nuclei that have been accelerated. The many experimental claims for anomalous effects in metal deuterides, such as excess heat, helium, low-level fusion, and fast alpha emission, suggest that the use of the vacuum approximation may not be universally applicable. We have been interested in the development of models in which the vacuum approximation is not made, and in which the nuclear system interacts with the local condensed matter environment. Our focus in recent years has been on models in which we propose that phonon exchange takes place during a nuclear reaction that occurs in a lattice. If exchange happens in the case of a highly excited phonon mode, quantum coupling may occur with other processes that exchange phonons with the same phonon mode. In the case of deuteron-deuteron (d-d) fusion reactions, the resonating group approximation was used for many years as the primary theoretical tool with which to understand reactions, and to predict reaction cross-sections. We have been interested in the generalization of the resonating group method to include lattice effects. A possible generalization is one in which the channel separation factors of the resonating group method, which describe the center-of-mass dynamics, is replaced by a more general channel separation factor, which describes the center-of-mass dynamics of the reacting nuclei on the same footing with other nuclei in the lattice. We have termed this a "lattice resonating group method". To make detailed calculations with this approach, we need to be able to compute matrix elements and interaction potentials in the presence of phonon exchange. To implement such calculations, one approach is to simply include phonon operators in 527

528

the basic description of a nucleon (i.e. proton or neutron) co-ordinate. For example, if nucleon j were bound to a nucleus, we would be perfectly content in a vacuum calculation thinking of the position of the nucleon as being determined relative to the nuclear center-of-mass co-ordinate. One often finds this notion expressed as Tj = R a + Xj,

(1)

where Vj is the (absolute) position of nucleon j , where R a is the center-of-mass coordinate of nucleus a containing nucleon j , and where Xj is the position of nucleon j relative to the nuclear center of mass. In the generalized problem in which the lattice is made part of the problem, the nuclear center-of-mass co-ordinate is a phonon operator. In this case, we would write instead Yj = R a + Xj,

(2)

with the associated interpretation that the nucleon co-ordinate Vj itself depends on the lattice through the position of the nuclear center-of-mass co-ordinate R 0 , which is an explicit phonon operator. To compute nuclear matrix elements including phonon exchange, we need simply to express the nuclear wavefunctions as explicit functions of the spatial co-ordinates, and then perform integrations as required. Since the wavefunctions and the nuclear interaction have spin and isospin degrees of freedom, this task very quickly becomes much less simple. One encounters an additional difficulty. To implement this program, we are interested in working with general correlated wavefunctions, focusing on the spatial dependence to implement phonon operators. Nuclear physicists instead usually generally make use of Racah algebra for interaction matrix element calculations, which is based on an independent nucleon (protons or neutrons) approximation. There does not exist much in the literature, which is helpful in implementing phonon exchange more fundamentally in the case of general wavefunctions. Consequently, we have undertaken a program in which the wavefunctions are written explicitly as functions of space, spin and isospin; and in which matrix elements are reduced to sums of spatial integrals. In this paper, we focus on the four-nucleon problem. 2. Four-nucleon Wavefunctions Group theory and the Pauli exclusion principle place rigid constraints on the form of the wavefunction. The exclusion principle dictates that the total wavefunction must be totally antisymmetric. Each wavefunction can be characterized by a total spin and isospin. However, by the Schur-Weyl duality, the spin (and isospin) determines the irreducible representation of the symmetric group that the spin (and isospin) wavefunction can belong to. The Clebsch-Gordan series of the symmetric group

529

then constrains the possible symmetries of the spatial wavefunctions. In general, such wavefunctions can be constructed in the form

* = YlCMAS\AT\j,

(3)

3

where [R]j, [S]j, and [T]j are the space, spin and isospin parts, respectively, and the Cj are the products of the Clebsch-Gordan coefficients of the symmetric group, 5(4). In this paper, we focus on the T = 0 case only. This is the simplest case, and contains the important example of d-d fusion reactions (in an approximation in which the neutron and proton channels are equivalent). The generalization to other isospins is conceptually and computationally completely straightforward. However, the number of terms increases significantly. At this level of discussion, we neglect the Coulomb potential, which does not conserve isospin. 2.1. Basis

Vector

Labels

The labeling of the basis vectors (in our case, it would be the space, spin or isospin wavefunctions) of any representation of the symmetric group can be done via the Yamanouchi symbols. 1 These symbols determine how the wavefunction (basis vector) transforms under the groups 5(2) C 5(3) C 5(4). The index scheme, we use for the Yamanouchi symbols, is defined in Table 1. Table 1. Definition of indicies for the Yamanouchi symbols

2.2. The Isospin-zero

Yamanouchi symbol

Index

4321 3211 3121 1321 2211 2121 2111 1211 1121 1111

1 2 3 4 5 6 7 8 9 10

Ladder

Wavefunctions

Below, we explicitly write down the T = 0 wavefunctions, which corresponds to a ladder type of coupling scheme. Please note, that the subscripts on the left-hand side of the equations are merely ways of enumerating the possible wavefunctions, where as the subscripts on the right-hand side are the indicies for the Yamanouchi symbols (see Table 1).

530

S = 0

S = 1 * 4 = —7^7 [S8*6 - Sgt5] + 7-/5^8 [V2s 7 t 6 + S 8 t 6 + S 9 i 5 J + ^ - ^ 9 [-%/2s 7 t5 + S 8 ts - Sgt6J * 5 = ITT^l

[ v ^ ^ - S8*6 - sgt 5 j - -Z~l=^3 [^87*5 + s 8 i 5 - Sg£6J + ^ " 0 4 [ss*5 + Sgt6] •

S = 2 * 6 = -?= [^5S10^6 - 1p6SWt5] •

3. T h e Nuclear Potential We will use t h e H a m a d a - J o h n s t o n (HJ) potential 2 as our model nuclear potential in t h e discussion t h a t follows. It is one of t h e simplest isospin-preserving nuclear potentials t o give reasonable results. T h e H J potential can be written as HHJ

= Vc + VTS12

+ VLSL.S

+ VLLL12,

where t h e individual potentials are denned as

Vc

= (n.T2)

(5I.CT 2 ) yc{r 12),

VT = (Ti.f 2 )y T (r 1 2 ), c, ASi.r^) (a2.ru) A12 = o

VLS =

-. a a

2 r 12

l- li

yLS(ri2)(L.S),

VLL = VLL(ri2), -2 1 VLL = {Si-S2)L - -(ai.L)(a2.L)

1 -

-(a2.L)(ai.L).

The spatial functions are given by + acY{x)

+

bcY2{x)},

y%{x) = 0.08|z(a;){l + aTY(x)

+

bTY2(x)},

yc(x)

yts{x) ytL(x)

= 0.08^Y(x){l

= liGLSY2{x){l 2

= vGLLx- Z(x){l

+

bLSY{x)}, + aLLY(x)

+

bLLY2(x)},

(4)

531

where \x is the pion mass, a stands for singlet-odd, singlet-even, triplet-odd or triplet-even. The functions Y(x) and Z(x) have the definitions Y{x)

= —,

Z(x)

1 + - + -I 1 Y(x) X1

X

4. Matrix Element Calculation Given the discussion above, the basic calculation of a matrix element is straightforward. We begin with initial and final RST states defined as

* = Y.C^\i\SW\i,

*' = ^Cfc[i?']fc[S']fc[T']fc.

3

k

We can then formally calculate the matrix element to be

= (J2CMAS]ATli

(*\HHj\*')

/ , Cj jk

HHJ Y,C'k[R']k[S']k[T'

C

(5)

'k {[R]j l-ffscalari [R']k) ,

where

H scalar

([S\An3\HHj\[S']k[T']k)

The significance of this result is that the matrix element is now expressed as a sum of spatial integrals, with the spin and isospin algebra evaluated to contribute to the expansion coefficients.

4.1. Specific

Result

We have calculated a complete set of such RST matrix elements for the T = 0 case. There are too many cases to be presented here. We therefore focus on a specific example by calculating the tensor force matrix element of Wi(M s = 0) and *e(M 5 = 1).

{*I(0)\VT\W))

3 ^ 3 (a; 12 + M/12) «12 VT (r 12)

no

where ipio = V'IOC^IJ • • • >^i) ordinates alone.

ip5 d TV

•d 3 r 4 ,

(6)

12 an

d ^5

=

V'sC^ii • • •

I^A)

are

functions of spatial co-

532

5. T r a n s i t i o n M a t r i x E l e m e n t for a T — 0 F u s i o n R e a c t i o n We can now formally calculate the reaction matrix elements for the d - d fusion reactions including phonon coupling. Since we are focusing on isospin-preserving T = 0 matrix elements, this calculation applies to isospin-preserving reaction models. T h e relevant states are: • One 4 + 0 state of 4 He in a spin singlet ground state (mostly spatially symmetric). • One 2 + 2 state of two deuterons in a quintet spin 2 state. a • Two 3 + 1 states (since these can be singlets or triplets). These are a linear superpositions of the H + p and He + n states.

5 . 1 . Physical

Wavefunctions

T h e wavefunctions discussed above are formal R S T objects, which are very general. We need to focus on specific wavefunctions for the different mass 4 (T = 0) channels in order to proceed. For example, the wavefunction for the ground state 4 He nucleus can be taken to be just \l/i with a spatial p a r t t h a t is completely symmetric. Hence #4,0

=

1plO—f=[s5t6-S6t5].

(7)

For simplicity, we adopt a wavefunction for two deuterons t h a t are in a quintet (spin 2) state. In this case, we can use #2,2 = A{^(12;34:)swt6}.

(8)

Here, A is an antisymmetrizer, and ^ ( 1 2 ; 34) is the spatial part of the deuteron wavefunctions. This wavefunction can be taken to be of the form V(12; 34) = Mr2

- r i ) 0 d ( r 4 - ?3) F ( j

1

^ ,

^ ± ^ j

.

(9)

There are two kinds of 3 + 1 wavefunctions, including singlet and triplet states. T h e singlet S = 0 states can be written a s b #3,1 = ^ J V ( 1 2 3 ; 4 ) | ( s 5 t i 2 i ( m T = l / 2 ) U -s&t211(mT

• ^ ( 1 2 3 ; 4 ) i ( s 5 i i 2 i ( m T = - l / 2 ) U -s6t211{mT

= l/2)

U)

=-1/2)

|4) } . (10)

a

We should, in general, consider the deuterons to be in a singlet or triplet as well. However, we are only doing an example here. In this enumeration of states, we are ignoring the various Mg values. The subscripts 211, 121, and 111 are the Yamanouchi symbols for the 3-body wavefunctions

533

The 3+1 triplet S = 1 states can be written as %A = X | 0 ( 1 2 3 ; 4 ) i ( s 8 t i 2 1 ( m T = 1/2) U ~sQt2ll{mT

= l/2) j 4 )

-V(123;4)^(s 8 ti2i(mT = - l / 2 ) T 4 - S 9 t 2 i i ( m T = - l / 2 ) T 4 ) ] . (11) We used the notation | 4 or J.4 to refer to the isospin of the fourth particle. The spatial part of ^ i and ^'3 1 is of the form ^(123; 4) = 0 3 (ri, r2, r 3 ) F> (Vl

+

^

+

^ , r4) ,

(12)

where 03 only depends on the two co-ordinate differences such as f\ —ri and r^ — r^. 5.2. Physical

Wavej"unctions

in Terms of Ladder Basis

States

To compute the matrix element, we need to change basis and describe our physical wavefunctions in terms of our ladder basis. This change of basis can be accomplished either using induction coefficients of the symmetric group or by brute force calculations. The results are c •4{*4,o} = * i ,

-4{* 2 , 2 } = * 6 -

(13)

The definition of the ladder basis i state involves the fully symmetric tpio spatial wavefunction, which is well defined for the 4 He nucleus. In the case of two deuteron states, the ladder basis \&6 is expressed in terms of mixed symmetry spatial wavefunctions %p5 and -06- For the physical state we used, these mixed symmetry spatial wavefunctions can be written as 0 5 = - L [2^(12; 34) + 2^(34; 21) - 0(23; 14) - ^(14; 23) - 0>(13; 24) - (24; 13)], V 12

4>s = \ [-^(23; 14) - ^(14; 23) + 0,(13; 24) + 0(24; 13)]. In the case of the singlet 3+1 channel, the antisymmetrizer acts to produce a single ladder basis state *4{*3,i} = * i ,

(14)

where the associated fully symmetric spatial part -0io can be expressed as a symmetric combination of the physical 3+1 states as ^10 = \ [0(123; 4) + 0(124; 3) +^(134; 2) +0,(234;!)]. c

(15)

T h e results will only involve * i , \&4, and \&6- These wavefunctions and no others are involved because of group theoretical considerations and our assumptions that the spatial part of the deuteron, triton, and helium wavefunctions are symmetric under the exchange of any two particles.

534

In the case of the triplet 3+1 channel, the antisymmetrizer acts to produce a single ladder basis state A{*'3il}

= *4)

(16)

where the associated mixed symmetry spatial parts I^T, ip$, and xpg are V>7 = ^ L [3^(123; 4) - ^(124; 3) - ^(134; 2) - V(234; 1)],

(17)

V 12

^ 8 = - ^ [4^(124; 3) - V(134; 2) - ^(234; 1)],

(18)

V9 = - ^ ( 1 3 4 ; 2 ) - V ( 2 3 4 ; l ) ] .

(19)

The computation of the relevant matrix elements is made simpler because we have a complete set of results for the matrix elements available in terms of the ladder basis. 6. Matrix Elements We focus here on one specific example: ( ^ { * 3 , i ( M s = 0 ) } | y T | ^ { * 2 , 2 ( M s = l)}) =

(*i(M 8 =0)|V r |*6(M 1 , = l)).

(20)

The rest of the matrix elements can be calculated similarly. From our previous example we know that <*I(0)|VT|*6(1)>

=

/

/'

^1*0

3 ^ (a 12 + iyu) Z12 ypjrn) r 12

^ d

f\ • • • d

?4.

We can use this with the appropriate definitions of the spatial wavefunctions for the different channels: •05 = ~4= [2^(12; 34) + 2V>(34; 21) - ^(23; 14) - ^(14; 23) - V(13; 24) - ip(24; 13)] , V 12

(21) V-io = \ [V>(123; 4) + V(124; 3) + ^(134; 2) + ^(234; 1)].

(22)

7. Conclusions To include phonon exchange in a description of nuclear reactions, we require a description explicitly in terms of spatial wavefunctions. We have developed a complete set of such nuclear wavefunctions for the 2-body, 3-body, and 4-body problems using a ladder basis. Results for the 4-body case is presented above. A complete set of matrix elements for the HJ potential has been developed in terms of explicit spatial integrals. Antisymmetric wavefunctions that are appropriate for d-d fusion calculations in the T = 0 approximation have been developed, and we have presented a specific example in this paper.

535

Acknowledgments Support for I. C h a u d h a r y was provided by the Kimmel Fund, Bose Foundation, and from a D a r p a subcontract.

References 1. M. Hamermesh, Group Theory and its Applications to Physical Problems (AddisonWesley, New York, 1962). 2. T. Hamada and I.D. Johnston, Nucl. Phys. A34, 382 (1962).

S T U D Y ON FORMATION OF T E T R A H E D R A L OR OCTAHEDRAL S Y M M E T R I C C O N D E N S A T I O N B Y H O P P I N G OF ALKALI OR ALKALINE-EARTH METAL ION

HIDEMI MIURA 1-27-6 Tsurugaoka, Izumi-ku, Sendai 981-3109, E-mail: miubrewer@h9. dion. ne.jp

Japan

Formation of tetrahedral or octahedral condensation related to the experiments on electrolysis or deuterium permeation was studied. We obtained the scenario about the formation that alkali or alkaline-earth metal ions infiltrating into the host metal made cavities there when they hopped onto the other sites of the crystal lattice of it, then through squeezing of H + / D + ions in the cavity tetrahedral or octahedral condensation of protons/deuterons is caused.

1. Introduction Much research on nuclear fusion and nuclear transmutation in condensed matter is currently in progress. Recently, experiments with deuterium permeation through Pd complex by Iwamura et al. have indicated that nuclear transmutations occur with alternating CaO and Pd layers, but no nuclear reaction is observed when this material is replacing it with MgO. 1 On the theoretical side, we have directed our attention to Tetrahedral Symmetric Condensate/Octahedral Symmetric Condensate (TSC/OSC) model of protons/deuterons by Takahashi, which can explain consistently the major experimental results. 2 " 4 We have examined the role of the alkali and alkaline-earth metal ions in the crystal lattice of the host metal when TSC/OSC is formed. As a result, we have obtained a very consistent and simple scenario as one of hypotheses about the formation of TSC/OSC that the alkali or alkaline-earth metal ions infiltrating into the host metal make cavities there, when they hop onto the other sites of the crystal lattice, then through squeezing of H+/D+ ions in the cavity the protons or deuterons undergo TSC/OSC. 2. Scenario of Formation of T S C / O S C Experiments on nuclear fusion and nuclear transmutation in condensed matter are performed, for example, by the electrolysis of LiOH/LiOD or K2CO electrolytic solution using Ni or Pd cathode, and by the deuterium permeation through alternating CaO and Pd layers, respectively. The scenario about the formation of TSC/OSC is constructed from following five processes that would proceed in the face-centered cubic (fee) lattice of the hydride-forming metals. This scenario would be as simple as possible with the role of the alkali or alkaline-earth metal ions. 536

537

2.1. Permeation

of H+/D+

Ions

Figure 1 shows the permeation of H+/D+ ions and typical infiltration of alkali or alkaline-earth metal ions in the case of electrolysis of water and in a deuterium permeation experiment. Electrolysys

Deuterium permeation

Tetrahedron

Octahedron

Q:Ni/Pd

Figure 1. (typical).

D:Tsite

O : 0 site

Permeation of H + / D + ions and Infiltration of alkali or alkaline-earth metal ions

H+/D+ ions permeate into the fee crystal lattice of the host metal such as Ni and Pd by electrolytic voltage and D2 gas pressure, and they are located mostly at the O sites. Although H+/D+ ions move corresponding to the permeation rates, they are confined at the O sites of the crystal lattice of the host metal for a short while. 2.2. Infiltration

of Alkali or Alkaline-earth +

Metal

Ions

Alkali metal ions such as Li and K and alkaline-earth metal ions such as Ca 2 + infiltrate into the fee crystal lattice of it, and they come to the T sites, O sites, and the lattice voids or defects. In the case of electrolysis, alkali metal ions accumulating on the surface of the host metal infiltrate into the near surface layers due to the surface vibration and the electrolytic current, and then mostly stay at the T sites of the crystal lattice for a long while. Each of the alkali metal ions at the T sites vibrating thermally interacts with four H + / D + ions at the vertexes of the tetrahedron surrounding it and vibrates them widely. In the case of deuterium permeation, alkaline-earth metal ions staying in contact with the surface of the host metal also infiltrate into it due to the surface vibration and the deuterium flow, and then mostly stay at the lattice voids or defects for a long while. Each of the alkaline-earth metal ions at the lattice void or defect vibrating thermally also interacts with six H+/D+ ions at the vertexes of the octahedron surrounding it and vibrates them widely. 2.3. Hopping

+

of Alkali or Alkaline-earth

Metal

Ions

Figure 2 shows typical case of hopping of alkali or alkaline-earth metal ions, squeezing of H + / D + ions, recoil and condensation of protons/deuterons. The alkali metal

538

ions hop onto the other sites of the crystal lattice of the host metal due to the thermal vibration, electrolytic voltage and most probably some electromagnetic impulses, and then make cavities at the former positions. The alkaline-earth metal ions also hop due to thermal vibration, deuterium flux, and electromagnetic impulses, also making cavities.

Impulse

fi#o " 4p/TSC, 4dfTSC

V Condensed and recoiled * S • i f / K+ V ^ Tetrahedron 4^:Ca + O^Ni/Pd

D:Tsite

V Condensed and recoiled 6d/0SC Octahedron O : o site

Figure 2. Hopping of alkali or alkaline-earth metal ions, Squeezing of H + / D ions, Recoil and Condensation of protons/deuterons (typical).

2.4. Squeezing

of H+/D+

Ions and Recoil

The hopping of the alkali or alkaline-earth metal ion causes the cooling down of the cavity and the recoil of cluster H + / D + ions around it. The cluster H + / D + ions, namely protons/deuterons at the vertexes of the tetrahedron or octahedron that make up the surface of the cavity, are squeezed in the center of each polyhedron due to the reaction of hopping-out of the alkali or alkaline-earth metal ion. A heavy alkali or alkaline-earth metal ion causes the strong recoil of even heavy cluster H + / D + ions, while a light alkali or alkaline-earth metal ion causes the weak recoil of only light cluster H + / D + ions. 2.5. Condensation Transmutation

of Protons/Deuterons or Fusion

and

Nuclear

In the combination of strong recoil of squeezed cluster H + / D + ions, after the condensation of protons/deuterons, condensed 4p/TSC, 4d/TSC or 6d/OSC would collide against the atomic nucleus of the crystal lattice of the host metal or other one to cause the nuclear absorption and transmutation according to the Takahashi's TSC/OSC nuclear absorption theory 2 ~ 4 . In the case of 4p/TSC by Li or K in the T site of Ni: 4p/TSC + M(A, Z) -»• M*(A + 4, Z + 4), others.

(1)

In the case of 4d/TSC by K or Ca in the T site of Pd: 4d/TSC + M(A, Z) -> M*{A + 8, Z + 4), others.

(2)

539

In the case of 6d/OSC by Ca in the lattice defect or void of Pd: 6d/OSC + M(A, Z) -> M*(A + 12, Z + 6), others.

(3)

On the other hand, in the combination of weak recoil of squeezed cluster H+/D+ ions, after the condensation of protons/deuterons, condensed 4d/TSC unite together tightly to cause the cluster nuclear fusion according to the Takahashi's TSC nuclear fusion theory without collision against the atomic nucleus of the crystal lattice of the host metal or other one. 2 - 4 In the case of 4d/TSC by Li in the T site of Ni or Pd: 4d/TSC -» Be* -s- 2a + 47.6 MeV

(4)

Specially, the production of M* (A+8, Z + 4) by the reaction (2) and M* (A+12, Z + 6) by the reaction (3) can explain nuclear transmutations like 133 Cs into 1 4 1 Pr and 137 Ba into 149 Sm, respectively, which is indicated in the deuterium permeation experiments through alternating CaO and Pd layers by Iwamura et al.1 Moreover, consistent with his reports, replacing Ca with Mg in his experiments would occur with no nuclear absorption and nuclear transmutation of TSC/OSC because of being too light for Mg 2 + ion to recoil and collide 4d/TSC or 6d/OSC against the other nucleus, and no nuclear fusion because there would be too many valence (+2) and influential Mg 2 + ions to keep the symmetry of each polyhedron. This scenario about the formation of TSC/OSC can explain some of the experimental results of the electrolysis or deuterium permeation qualitatively, but it is based on many assumptions that must be proved experimentally or theoretically. And the hopping of the alkali or alkaline-earth metal ions and the recoil of H + / D + ions must be considered not only on the mass difference of each other but also on the other qualities. 3. Properties Derived from the Scenario Some properties are derived from the above scenario. Some of the major ones are as follows. 3.1. Three Kinds Flux

of Electrolytic

Current

Density

or

Deuterium

There are three kinds of electrolytic current density i or deuterium flux / , which have the minimum and maximum, respectively: (a) For permeation of H+/D+ ions: i h / d or f^. (b) For infiltration of alkali or alkaline-earth metal ions: iaik or /aik(c) For hopping of alkali or alkaline-earth metal ions: ihop or /hopGenerally, it may be that: 0 ~ (c) i ho p < (a) h/d < (b) iaik or 0 - (c) / h o p < (a) / h / d < (b) /aik-

(5)

540

However, these values might depend on the settings of experimental apparatus. Therefore, it might be necessary to control the value of the electrolytic current density or deuterium flux properly in experiments, for example in the high range for the preparation process of the permeation of H+/D+ ions and infiltration of the alkali or alkaline-earth metal ions first for a while, and then in the low range for the response process of the hopping of the alkali or alkaline-earth metal ions, condensation of protons/deuterons and nuclear reactions lastly. 3.2. Local Cooling Down due to Hopping Alkaline-earth Metal Ion

of Alkali

or

When the hopping of the alkali or alkaline-earth metal ion makes a cavity in the crystal lattice of the host metal, four H+/D+ ions at the vertexes of the tetrahedron or six H + / D + ions at those of the octahedron remain there constructing the surface of the cavity. In the analysis of the model of surface phonons, when one of the springs composing an infinite long one-dimensional diatomic lattice is cut off, the frequency of the lowest optical mode decreases to the Wallis mode. This explained using the Rayleigh's theorem described by the following equation: When the number m oscillator of infinite long one-dimensional lattice composed by f oscillators changes it's mass and spring constant, the motion of this one-dimensional lattice is described by the proper equation as follows.5

l/(au2-p)

/

+ J2^i/(MJu;2-CJ)=0

(6)

.7 = 1

a: change of mass (3: change of spring constant to: frequency, My. mass of the number j oscillator, Cy. spring constant of the number j oscillator, 5rnj-. Kronecker's delta. By replacing z = u2 and Zj = w|, the equation F(z) = F\(z) — F2{z) = 0 transformed from Eq. (6) gives solutions which are indicated by intersections of Fi(z) = F2(z) on the graph, where / F1(z) = ^mj/(MjZ •? =

- Cj)F2(z) = - l / ( a z - /?).

(7)

!

If the mass and spring constant of number m oscillator change to become a = ~Mm < 0 and (3 = —Cm < 0 which means disappearance of them, respectively, the lowest frequency decreases and the highest one increases. Applying this relationship to the diatomic lattice system consisting of light H+/D+ ions and alkali or alkaline-earth metal ion and heavy host metal ions, it might be expected that the frequency of some mode of lighter H + / D + ions on the surface of the cavity decreased and the cavity was cooled down while the alkali or alkaline-earth metal ion hopped out by increasing of frequency. If the coherent

541

phonon of the crystal lattice of the host metal is caused by electromagnetic impulse simultaneously with or after the hopping-out of the alkali or alkaline-earth metal ion, and the coherent oscillation of phonon is just in the decreased mode, it might be possible to cool down the local region effectively, although the frequencies of only a few modes decrease almost 10 meV at the most.

4.

Conclusion

In this study we revealed the formation of T S C / O S C explained clearly by the processes by which alkali or alkaline-earth metal ions infiltrate into the host metal and hop onto the other sites of the crystal lattice of the host metal. T h e hoppingout of the alkali or alkaline-earth metal ion recoil the condensed protons/deuterons strongly, causing nuclear transmutation, or weakly, causing nuclear fusion. And we showed, the important roles of the alkali or alkaline-earth metal ions is to make the cavity in the crystal lattice of the host metal by hopping, which squeezes H + / D + ions and cools down the cavity to cause the condensation of protons/deuterons.

Acknowledgements T h e author wishes to t h a n k Professor Takahashi of Osaka University for valuable information and advice.

References 1. Y. Iwamura, T. Ithoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasadi, Low energy nuclear transmutation in condensed matter induced by D2 gas permeation through Pd complexes, Proc. ICCF11 (in press) http://www.lenrcanr.org/ 2. A. Takahashi, Deuteron cluster fusion and related nuclear reaction in metaldeuterium/hydrogen systems, Recent Res. Devel. Phys. 6, 1-28 (2005). 3. A. Takahashi: 3 He/ 4 He PRODUCTION RATIOS BY TETRAHEDRAL SYMMTERIC CONDENSATION, Proc. ICCF11 (in press) http://www.lenr-canr.org/ 4. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Proc. ICCFIO (in press) http://www.lenr-canr.org/ 5. T. Ohshima and Y. Ohtsuki (eds.), Surface Phonons, Front of Physics Vol. 30 (Kyoritsu, 1992) (in Japanese).

CALCULATIONS OF N U C L E A R R E A C T I O N S P R O B A B I L I T Y IN A CRYSTAL LATTICE OF L A N T H A N U M D E U T E R I D E

V . A . K I R K I N S K I I A N D Y U . A. N O V I K O V Institute of Mineralogy and Petrography, Siberian Branch of the Russian Academy of Sciences, Prospect Academy Koptyuga 3, Novosibirsk 630090, Russia E-mail: [email protected]

The dynamic model of electron orbitals deformation was previously devised for palladium deuteride. It has now been applied to calculate the probability of nuclear reactions of hydrogen isotopes in the crystal lattice of lanthanum deuteride. In a series of computer simulations, the probability of D—D approach for random initial conditions was calculated, when the initial energies of the approaching deuterons were set in the range of 0.001-9.0 eV. For each experimental value of D—D approach the reaction rate was calculated on the shifted Coulomb potential with the shift energy, which equals to the energy of screening. The mean distance of D - D approach on the whole series equals 0.19 A. More than 54% of all experimental values show an approach of deuterons at a distance smaller than 0.1 A. The average reaction rate for the given set of the initial conditions is 10 3 , 2 8 s _ 1 per DD pair. This is three orders of magnitude less than the analogous rate calculated earlier for palladium deuteride. Allowing for the higher D content and the higher number of adjacent tetrahedral sites in LaD3 as compared with PdDo, 6, an overall nuclear fusion rate in lanthanum deuteride will be only slightly lower than in palladium deuteride, that is, 1 0 ~ 1 2 - 1 0 - 1 4 s _ 1 per DD pair.

To achieve a more sophisticated understanding of the mechanism and peculiar features of nuclear reactions in condensed matter, it is very important to expand a circle of substances that have been investigated. However, direct experimental research of new materials involves considerable difficulties, as the observable effects only slightly exceed the sensitivity of instrumentation, or the background level. In this connection, a random search of all substances to find which ones can catalyze cold nuclear fusion would be labor consuming and ineffective, especially taking into account the variations of their physical state and impurity content. Although most research on nuclear reactions in metal have been done with palladium, the high price and limited quantities of this material hinder the practical use of it. From the foregoing, the importance of theoretical calculation for search of materials is clear - a search to find which materials can be activated to produce nuclear fusion at low energies. We conducted a simulation of nuclear reactions of deuterium in palladium crystal lattice based on a dynamic model of electron orbital deformation in which hydrogen atoms are located in octahedral sites of closely packed metal atoms. 1_4 The calculation results correspond within an order of magnitude to the experimental 542

543

measurements of excess energy output (see, e.g. Ref. 5 and reviews in Refs. 1 and 6). Later, using the same model, the rate of a nuclear reaction was calculated in a titanium deuteride, where deuterium atoms are situated in tetrahedral sites of a crystal lattice, and the limiting content corresponds to TiD2 crystal structure. 4 In the present paper, we calculate the probability of a nuclear interaction in lanthanum deuteride, in which deuterium atoms can reside both in octahedral and tetrahedral sites of closely packed lanthanum atoms forming the LaD3 crystal lattice. The high content of deuterium in lattice should be favorable for implementing a nuclear interaction. Studies of lanthanum deuteride are also valuable because based on them we can draw conclusions about analogous compounds of lanthanide elements and yttrium, which have a similar lattice with slightly diminished crystal lattice parameters. For calculations of probability of nuclear reactions of hydrogen isotopes in the crystal lattice of lanthanum deuteride the dynamic model of electron orbitals deformation (EODD) offered earlier for palladium deuteride was used. 1-3 The hydrogen isotopes predominantly occupy tetrahedral sites in the face-centered cubic lattice of lanthanum hydride. Symmetrical positions of deuterium atoms with respect to the edge connecting two adjacent tetrahedral sites in lanthanum were selected as initial conditions for numerical tests. The initial trajectory of lanthanum 6s-electron was set as an ellipse, in one of its focal points a nucleus of lanthanum atom with an effective charge Z\,& is located. The effective charge Z\,a is calculated from the potential of ionization and the maximum radial density of La 6s-orbital wave-function.7 The electron can be found also on ellipse-like trajectories, which are distinct from the most probable ones, at different electron distances from La atom nucleus at the apogee. The calculations were carried out also for such trajectories using different initial outer electron orbital radii (see below). In a series of computer simulations, the probability of D-D approach for random initial conditions was calculated in the initial energy range of 0.001-9.0eV of approaching deuterons (the potential barrier for diffusion of deuterium atoms in lanthanum is about 0.43 eV). The most favorable conditions of two deuterons approaching one another were determined by preliminary computer modeling1 within the framework of the described model to reduce the calculation time. For each experimental value of D-D approach the reaction rate was calculated on the shifted Coulomb potential with the shift energy, which is equal to the energy of screening. The series consists of 40,000 experimental values. The mean distance of D-D approach on the whole series equals 0.19 A, however, more than 54% of all experimental values show an approach of deuterons for a distance smaller than 0.1 A. If one considers the reaction rate at each case of approach, and then averages as a whole on the entire sample, the general reaction rate for the given set of the initial conditions will make 10 3 2 8 s _ 1 per DD pair. It is three orders of magnitude less than the analogous rate calculated earlier for palladium deuteride, 1_3 but more than 10 times higher than the rate calculated for titanium deuteride. 4

544

Results of these calculations show that probability of fusion reactions depends not only on initial distances between deuterons but also on the character of electron orbitals of metal atoms. In order to investigate the influence of the initial outer electron orbital radius on an efficiency of deuteron approaching, another set of simulations was carried out. In the second series the range of outer orbital radii (a - 0.4) ± 0.05 A was used instead of (a —0.2)±0.05 A in the fist series (were a is a half of distances between lanthanum atoms located at the vertex of tetrahedral sites). The results of the second series essentially differ from the first series ones. The mean distance of D-D approach on the series equals 0.25 A (Fig. 1).

0.0

1.0

2.0

3.0

4.0

5.0

6.0

7.0

8.0

9.0

Energy (eV)

Figure 1. Distribution of minimal distances of D—D approach during their counter motions on the boundary of the neighbor tetrahedral sites in lanthanum deuteride vs their initial kinetic energy.

More than 33% of all experimental values show an approach of deuterons at a distance smaller than 0.1 A. If one considers the reaction rate at each case of approach, and then one averages as a whole over the entire sample, the average reaction rate for the given set of the initial conditions will be 10 1,41 s _ 1 per DD pair. Comparing Figs. 2 and 3, one can see that at the energy < l e V the reaction rates in both cases are nearly equal, but at higher energy the dependence character differ. The D-D reaction rate in lanthanum deuteride has a reverse dependence on energy in comparison with palladium deuteride (see, Refs. 1-3). To optimize calculations the most favorable initial conditions were selected. To obtain the true results, calculated values should also be multiplied by a correction factor,1 which allows for the probability of the occurrence of these favorable conditions. When calculating this factor it is necessary to take into consideration the fact that the content of deuterium in lanthanum deuteride is six times higher than in palladium deuteride and the number of deuterium atoms in adjacent tetrahedral

545 4.5-1

3.5-

o CD

H ••R

2.54

24

1.5-

0.5-I 0

1

2

3

4

5

6

7

8

9

Energy range (eV)

Figure 2. Energy dependence of D-D reaction rate in lanthanum deuteride according to EODD simulations for the first series.

sites is 32 times higher than in adjacent octahedral sites in PdDo.s- Besides, in LaD3 there are closely spaced adjacent octahedral and tetrahedral sites occupied by deuterium. Thus, if it is possible to provide high mobility of deuterons in LaD3 crystal lattice, the reaction rate will be only slightly lower than the rate calculated earlier 1-3 and experimentally observed in palladium deuteride (see, e.g. Ref. 5 and reviews in Refs. 1 and 6).

4

5

Energy range (eV)

Figure 3. Energy dependence of D-D reaction rate in lanthanum deuteride according to EODD simulations for the second series.

546

Owing to the diminished parameters of crystal lattices of deuterides of other rare earth metals and yttrium, the reaction rate of a nuclear fusion in t h e m can be closely matched to the rate in palladium deuteride, i.e., 1 0 - 1 2 - 1 0 - 1 4 s _ 1 per DD pair. Since the cost of a n a t u r a l mixture of rare e a r t h metals is much lower t h a n the same weight of palladium, and rare earth metals are much more a b u n d a n t in n a t u r e t h a n palladium (and other platinum group metals), they are attractive perspective catalysts for nuclear fusion at low energies.

Acknowledgement This work was supported by the R F B R (Grant No. 05-05-64930).

References 1. V.A. Kirkinskii and Yu. A. Novikov, Theoretical modeling of cold fusion. Novosibirsk, Novosibirsk State University, 105 p. (2002). 2. V.A. Kirkinskii and Yu. A. Novikov, Numerical calculations of cold fusion rates in metal deuterides, in: Condensed Matter Nuclear Science (Xing Z. Li, ed. Proc. ICCF-9), 162 (2003). 3. V.A. Kirkinskii and Yu. A. Novikov, Modelling of dynamic screening effects in solid states, Europhys. Lett. 67, 362 (2004). 4. V.A. Kirkinskii and Yu. A. Novikov, Calculations of nuclear reactions probability in a crystal lattice of titanium deuteride, in Condensed Matter Nuclear Science (P. Hagelstein and S. Chubb eds. Proc. ICCF-10) (2005). 5. V.A. Kirkinskii, V.A. Drebushchak, and A.I. Khmelnikov, Excess heat release during deuterium sorption-desorption by finely powdered palladium deuteride, Europhys. Lett. 58, 462 (2002). 6. P. Hagelstein et al. New Physical Effects in Metal Deuterides (http://www.lenrcanr.org/acrobat/Hagelsteinnewphysica.pdf). 7. J.T. Waber and D.T. Cromer, J. Chem. Phys. 42, 4116-4123.

POSSIBLE C O U P L E D ELECTRON A N D ELECTRON N E U T R I N O IN N U C L E U S A N D ITS PHYSICAL CATALYSIS EFFECT ON D - D COLD F U S I O N INTO HELIUM IN Pd

MIKIO FUKUHARA MR Tohoku University, Sendai, E-mail: [email protected].

Japan ac.jp

We investigate a possibility of coexistence of an electron and an electron neutrino in nucleus, by normalization of electroweak interaction. Provided that the electron of atom takes one's share of both electromagnetic and weak interactions, we obtain 2.07 x 10 — 5 eV as the electron mass for the weak one, from Compton wavelength. This value is close to estimated neutrino mass, 10~ 5 — 10 —6 eV, giving a possible answer for an unexplained problem of the standard model in particle physics. Thus, we can see that one electron and one neutrino exist in proton and neutron, respectively. Physical roles of electron and neutrino for cold fusion of helium in solid lattice were investigated in terms of elemental particle physics. The electron and neutrino in nucleus enhances the fusion reaction, based on weak interaction in 13 decays, as well as a catalytic effect of neutral pions.

1. Introduction An atomic nucleus is composed of neutrons and protons, but we cannot find electrons and neutrinos in the nucleus at the first glance. However, it has been recognized that these light particles, which are lepton with isospin 1/2, do not contain originally in nucleus, but generates certainly in nuclear transmutation processes such as /3 decay and helium formation in sun. Since a composite model, which the nucleus is composed of proton and electrons, was knocked out by discovery of neutron, wide credence has been given to a fixed concept that the electrons cannot exist in nucleus. 1 However, as far as the nucleus is constituent element of the atom, the distribution of the electron in nucleus is not perfectly zero without violation of uncertainty principle in spite of its extremely small volume. On the other hand, generation process for neutrino has not been entirely resolved. We have another look at the generation process. Our first interest lies in studying a possibility of coexistence of electrons and neutrinos in nucleus from a new angle on particle physics with lower energy. Although the neutrinos have three families or three flavor eigenstates (ye,v^ and vT) associated with the three charged leptons: the electron, the muon and the tau, we use the electron neutrino with the lightest mass in this study. As far as we know, no previous research has been done on coexistence of electrons and neutrinos in nucleus, except for nuclear reaction of excited electron and neutrino in solids.2 547

548

Next, we investigate an enhancement effect by the coupled electron and neutrino for nuclear cold fusion, in addition to catalytic effect of neutral pions. showed that the formation of helium nucleus from In the previous paper; two deuterons, i.e., fusion, requires necessarily a direct force due to exchange of two neutral pions which do not actually compose the deuteron nucleus. D 2 + D 2 + 2^° = He 4 .

(1)

The neutral pion is provided by two photons, which are produced by emission of excited collective electrons derived from the palladium atoms. The introduction of the pions makes possible to reduce remarkably an internuclear distance, enhancing fusion rate for helium formation. For a significant role for nuclear fusion by neutral pion, we explained that the pion could easily enter within effective nuclear force field of deuteron pairs at close proximity, because the neutral pion does not experience a Coulomb barrier. 4 Then we investigated necessary and sufficient conditions for cold fusion of helium in solid lattice in terms of elementary particle physics, using the Heisenberg uncertainty relation is given by the Yukawa formula: L < cAtzi

h/mpc,

(2)

5

where c is the velocity of light and t is time. The interaction for deuterium atom pairs is schematically shown in Fig. 1, along with charge pion-mediated pn interaction in deuteron. P

(3)

Figure 1. Schematic representation of electromagnetic interaction, p + e <-> p + e , mediated by photon 7 for two deuterium atoms, D2, where p and n are proton and neutron, respectively.

The Pd lattice for confinement of deuteron pairs plays the same role as magnetic field confinement in hot nuclear fusion, because the attractive interaction between deuterium atom and electron is mediated by massive photon with 5.2 keV.

549

On the other hand, nitrogen in the earth's atmosphere was interpreted by endothermic nuclear transmutation of carbon and oxygen nuclei confined in carbonate lattice of the mantle, with help of electropionic attraction effect due to the excited electron and plenty of neutrinos. 6 However, it is not necessarily clear physical role of the electron and electron neutrino for nuclear fusion yet. 2. Coupled Electron and Neutrino in Electroweak Interaction For the generation of neutrinos and electrons, the /3-decay is the most familiar physical phenomenon. The following relation of the /3-decay describes a weak interaction between lepton and nucleon;7 n + v <-> p + e~.

(4)

This formula shows that four particles form two groups; (n, v) with neutral charge and (p,e~) with charge. Since p and n have the quark structure uud and ddu, respectively, we can rewrite Eq. (4) as the form: d + v <-> p + e~.

(5)

Equation (5) indicates that four elementary particles form two groups; (d, v) and (u, e~). In this formula, barion and lepton numbers, and charge (—1) are preserved before and after reaction. As far as quarks are permanently confined inside the nucleons, we must consider the interaction in narrow region of the nucleus. However, as a matter of fact, Eq. (5) has been treated in utter disregard of the above-mentioned physical condition. Then we consider conformation of Eq. (5), in terms of standard model in particle physics. Fermi elementary particle interaction between proton and neutron is shown in Fig. 2, using Feynman diagram. For this purpose, we use the lightest deuterium nucleus with one proton and one neutron, as a representative one. In Fig. 2, the weak interaction of Eq. (5), which involves exchange of electric charge, is mediated by charge intermediated vector boson, W between u and d quarks in different nucleon each other. On the other hand, both neutrino and antineutrino v in proton and both electron and antielectron e + in neutron are mediated by neutral intermediate boson, Z°: v + v <-> e~ + e + . ±

(6) 8

Here, since masses of W and Z bosons are extremely large, 80.375 and 91.187 GeV,9 respectively, we can calculate their Compton wavelengths; 2.46 and 2.16 x 10~ 18 m, respectively. Thus, two group particles (u,e~) and (d, v) must bind together by weak force in very narrow region of around (2.2 — 2.5) x 10~ 18 m. For proton, the total positive charge (+1) of three quarks cancels the negative charge (+1) of the electron, while the neutron has positive and negative electrons for a total electric charge of zero. As a result, we can see that one electron and one neutrino exist in proton and neutron, respectively. Furthermore, v and e~ are coupled as an s-wave boson of spin 0, because the electroweak force requires that the spins are

550

Neutron

Proton

Figure 2. Schematic representation of elementary particle interactions, d + v <-> u + e~ and e~ +v ^ e+P, mediated by W and Z° bosons in proton and neutron deuterium atom, respectively, where u and d are up and down quarks, respectively. The reaction, e _ -\-v <-> e~ +v, is eliminated.

opposed to each other due to boson exchange. 10 Since the size of both lepton and quark is less than 1 0 _ 1 8 m and the nucleus size is around 10~ 15 m, we can assume that u and d quarks are surrounded by spherically symmetrical ball of electron and neutrino blurred by a time-exposure of its rapid motion in nucleus, respectively. Furthermore, although the standard model in particle physics does not specify how many quark-lepton pairs constitute the family,11 a limit number exists, as far as we treat natural atomic elements with atomic number up to around 110; three pairs must assign for one proton-neutron pair. In other words, the three kinds of pairs must intrinsically assign for one proton-neutron pair, but this problem has been overlooked in the high-energy particle physics. 3. Electron Distribution in Electroweak Interaction In the previous section, with a view to explaining coexistence of electron and neutrino in nucleus, a necessary role of weak interaction was shown. Notwithstanding the necessary condition, we feel a new question why the existence of electrons in proton does not violate uncertainty principle. Next, we consider a possibility of existence of electron in proton in terms of electroweak interaction. If light particle such as electron exists in nucleus, it cannot be generally confined in the nucleus because of large uncertainty of the momentum. However, the uncertainty determining the position of the electron in nucleus decreases as speed of the electron increases. This means probability of existence for electron in nucleus is not zero. In atom, nucleus and electrons are bound together by electromagnetic force of mediated photon (Fig. 1) for two deuterium atoms, D 2 . In general, the strength of force for boson exchange interaction is in proportional to square of an effective interacting zone of boson or in inverse proportion to square

551

of boson mass. In calculation of the strength for photon, we cannot make use of the latter's relation, because of photon with zero mass. Since Compton wavelength of the electron is 3.86 x 1 0 - 1 3 m, we can use the wavelength as the interacting zone of photon. Similarly, Compton wavelength, i.e., the interacting zone, of the W boson in weak interaction is 2.46 x 10~ 18 m. Thus the zone ratio of the electromagnetic interaction to the weak one is around 4.04 x 1 0 - 1 1 . Here, since one electron corresponds to one proton in atom, we can assume that the electron of atom takes one's share of both electromagnetic and weak interactions in proportional to the effective zone ratio in normalization of electromagnetic and weak interactions in regardless of their coupling constants. In other words, the weak force mediator is lodged with the (u, e~) group for a brief time. From the effective zone ratio, we can obtain 2.07 x 1 0 - 5 eV as the electron mass associated with the weak interaction. This value is close to the electron neutrino mass, 10~ 5 —10 -6 eV, 12 extrapolated from masses of muon and tau neutrinos obtained in Super-Kamiokande collaboration. This indicates that the ratio of the lepton mass is almost equivalent to the ratio of quark ones, giving to a possible answer for an unexplained problem of the standard model in particle physics, which the ratio of lepton mass within the first family is so large compared with the ratio of quark ones. And we can also reply why only the first family is needed to make up the ordinary protons, neutrons and electrons in the universe? The electrons and neutrinos coexist with quarks in "nucleon vessel" of atom which is firmly bound by electromagnetic interaction. On the other hand, the other two families exist only ephemerally after the electrons are completely separated from the nucleus by high-energy collisions. Although nuclear behaviors at low temperature have not aroused researcher's interest, because most nuclei have enormous energy of the order of a few MeV, we cannot ignore the role of the electrons for atoms associated with u and d quarks in particle physics. Further study for this interesting area is called for. 4. Physical Role of Electrons and Electron Neutrino for Nuclear Fusion In the previous section, we reported a possible coexistence of an electron and an electron neutrino in nucleus, based on weak interaction in /3-decay. Provided that the electron of atom takes one's share of both electromagnetic and weak ones according as the zone ratio, we can see that one electron and one neutrino exist in proton and neutron, respectively. When a helium atom is formed two deuterons, quarks, electrons and neutrinos must be mediated by charged and neutral intermediated bosons, W and Z° (Fig. 3), respectively, as a result of mediation of charged and neutral pions. u + e~ <-> d + v,

(7)

+

e + v ^> e~ + u,

(8)

e~ + v <-• e~ + v.

(9)

552

From Fig. 3, an addition of neutral pions is equivalent to the double addition of Eq. (9), i.e., two e~-v pairs. Thus the addition of e~ and v pairs enhances the fusion reaction. Proton

Neutron

U

1

Figure 3. Schematic representation of elementary particle interactions, d + v <-• u + e~, e+S" <-> e~ + v and e~ + v <-» e~ + v, mediated by W and Z° bosons in proton and neutron of deuterium nucleus, respectively, where u and d are up and down quarks, respectively. The black lines are W and Z° mediated interaction between proton and neutron. W and Z° mediated interactions among protons and neutrons are dotted and broad lines, respectively.

5. Creation of Electron and Neutrino Pairs Last, we consider how the pairs create before fusion reaction. When palladium nuclei with even atomic number exist, there is a possibility that double /3-decay, which is the second-order /3-process, occurs. 13 {Z,A)^{Z

+

2,A)+2e~

•2v,

(10)

553

where Z and A are atomic and mass numbers, respectively. Equation (10) is nonequilibrium equation. Since palladium in nature has five isotopes with even atomic number, i.e., 102 Pd, 104 Pd, 106 Pd, 108 Pd, and 1 1 0 Pd of 0.96, 10.97, 27.3, 26.7, and 11.8%, respectively,14 the corresponding element sets for Eq. (10) are i 0 6 p d ^ i 0 6 C d ) i 0 8 p d ^ i 0 8 C d ] a n d n o P d ^ i i o C ( 1 F o r s t a r t i n g elements, 106 Pd, 108

Pd, and 1 1 0 Pd are plausible. As far as we know, no previous research has been done on physical role of electron and neutrino for nuclear reaction, except for nuclear reaction of excited electron and neutrino in solids.6 This interesting area needs for further work. 6. Conclusion In this study, we investigated a possibility of coexistence of coupled electron and electron neutrino in nucleus, using electroweak interaction. In nucleus, the weak interaction is mediated by W ^ boson between u and d quarks in proton and neutron, respectively or neutron and proton, respectively, while neutrino and antineutrino in proton and electron and antielectron in neutron are mediated by Z° boson. From Compton wavelengths of the electron and the W boson, the effective zone ratio of the electromagnetic interaction to the weak one is around 4.04 x 1 0 ~ u . Provided that the electron of atom takes one's share of both electromagnetic and weak ones according as the zone ratio, we obtain 2.07 x 10~ 5 eV as the electron mass for the weak one, closing to estimated neutrino mass, 1 0 - 5 — 10~ 6 eV. This is a possible answer why the ratio of lepton mass within the first family is so large compared with the ratio of quark ones in the standard model. The electron and the neutrino are coupled as s-wave boson in nucleus. From view of particle physics by mediation of charged and neutral pion, the introduction of s-wave coupled electron and neutrino enhances cold fusion. The addition of neutral pions is equivalent to the double addition of Eq. (9), i.e., t w o e - — v pairs. The electron and neutrino pair may come from double /3-decay formation of helium, (Z,A) -^(Z + 2,A)+2e~

+ 2v.

(11)

In this nonequilibrium equation, 106 Pd, 108 Pd, and 1 1 0 Pd are plausible in nature. The sufficient conditions in this interesting area needs further study. References 1. E. Fermi, Nuclear Physics (The University of Chicago Press, Chicago, 1950), p. 97. 2. M. Fukuhara, Proc. 4th Meeting of Japan Cold Fusion Research Society, Tokyo (2005), p. 63. 3. M. Fukuhara, Fus. Sci. 34, 151 (1998). 4. D.F. Measday and G.A. Miller, Am. Rev. Nucl. Phys. 29, 121 (1979). 5. M. Fukuhara, Proc. 6th Meeting of Japan Cold Fusion Research Society, Tokyo (2005), p. 53. 6. M. Fukuhara, Nuovo Cimento C27, 99 (2004).

554 7. W. Greiner and B. MuUer, Gauge Theory of Quark Interactions (Springer-Verlag, Berlin, Heidelberg, 1996), p. 241. 8. Particle Data Group, Euro. Phys. J. C 3 , 224 (1998). 9. Particle Data Group, Phys. Rev. D54, 214 (1996). 10. S.M. Bilenky and J.Hosek, Phys. Rep. 90, 73 (1982). 11. G.J. Feldman and J.Steinberger, Sci. Am. Feb., 26 (1991). 12. Neutrino, KEK Jp. News, June 12 (2002). 13. T.D. Lee and C.S. Wu, Weak Interactions, Ann. Rev. Nucl. Sci. 5, 381 (1965). 14. IUPAC, Element by element review of their atomic weights, Pure Appl. Chem. 56, 695 (1984).

T U N N E L R E S O N A N C E OF ELECTRON WAVE A N D FORCE OF FLUCTUATION

MASANOBU BAN Tokyo Metropolitan

Industrial E-mail:

Technology Research Institute, 3-13-10 Tokyo 115-8586, Japan [email protected]

Nisigaoka

Kitaku,

We propose that cold fusion (CF) is fluctuation of the resonance, which happens to the electron wave. When electricity is discharged, a special crystal is made from free particles by the tunnel phenomenon of the electron wave. If free particles line up in the arrangement of the crystal, and the particle shifts, the line makes a wave. When alignment fluctuates, phase transition occurs in crystal. There is a possibility that the distribution of energy is converted into all the combinations for the phase transition of the crystal. The phenomenon of CF appears variously for that.

1. Introduction It is pointed out that cold fusion (CF) is responsible for the configuration of deuterium atoms in crystal. The CF is connected to three kinds of resonance occurring in electron discharge. The CF is a type of electron resonance, which occurs in the dc circuit. I would like to propose that self-expansion tunnel resonance of the material wave is the primary cause. In the dc circuit, the charge causes the alignment of the free particle. 1 - 5 We found a force that the electric charge assists to form in line for deuterium atoms in crystals. In this study, we investigate a relation between matter wave resonance occurring in dc discharge current and CF in view of variation of the resonance. For dc electric discharge three noises interchange in the same condition 6 (see Figs. 12 and 13 of Ref. 6). The noise, which occurs in power spectral density P(f), fluctuate white, 1 / / square, and 1 / / noises. These noises are exchangeable. We propose that the phenomenon must be a phase transition of the crystal from the investigation. Nanocarbons, nanotubes, and Fullerene are produced at a phase transition by dc discharge circuit. 7 Since phase conversion of crystals awes to dc discharge, we consider phase conversion for CF. We explain the relation for CF, using change of resonance matter wave.8 We describe more an outline. Maeda et al. successfully found that the noise component of 1 / / and 1 / / square was observed at discharge portion in graphite electrode,6 and took out the noise of the electric discharge portion from demodulation controlled by the electric discharge distance 6 (see p. 2141). In this 555

556

case, the two kinds of noise occur alternately in the circuit. Maeda's P(f) can analyze the feature as P ( / ) / i = C or P(f)J2 = C. Therefore, three kinds of phenomena exist in the electrical discharge part together with P(f)fo = C of the white noise. In general, it is well known that the white noise always exists as J. B. Johnson Noise. Indeed, the three kinds of noises occur continuously and alternately at least. This is responsible for tunneling in discharge at part of discharge. Thus the tri-stable of tunneling phenomena occurs alternately. The free electrons in discharge are emitted from metal surface into the air by tunneling. And the electron makes standing waves and traveling waves in the electric discharge. 8 In other words, existence of the standing and traveling waves make assist to form in line for deuterium atoms in crystals, leading to CF. Such phenomena will occur in plasma dust from direct current glow discharge as plasma crystal. 8 Furthermore, since dust makes line up as some crystal, we propose that phase change exists in resonance of the de Broglie wave. 2. Particle Alignment by Tunneling We think that CF occurs because of the tunnel phenomenon of the electron wave, and the reason is announced here. In experiment of Fujita et al, a plasma dust phenomenon occurs in a glow discharge part. 1 The power, which led dust to the plasma crystal, can be considered based on a tunnel phenomenon (see Fig. 1). It is thought that movement draws Lissajous figures of wave motion when dust is led to the formation. The Lissajous figure will be carried out based on the traveling wave and standing wave of a tunnel phenomenon. Fujita's circuit is equal to Maeda's tunnel microscope in the composition and the voltage of the electric circuit. The theory of electricity is never changed because of the distance in the electrical discharge section. The particulate is caught also by STM. The tunnel phenomenon of the electron has occurred together in these electrodes. When the carbon graphite was observed in the experiment on STM by Maeda et al, two kinds of power spectrum densities P(f) were observed from the electrical discharge in the same frequency band region.

A

hi> T7 ff

•fAAM* Figure 1.

Tunneling out from Cathode at discharge.

557

Maeda's P(f) can analyze the feature as P(f)fi = C or P(f)f2 = C. Therefore, three kinds of phenomena exist in the electrical discharge part together with P ( / ) / o = C of the white noise. The feature of a nonlinear phenomenon is found from tri-stable of the power spectrum. Fullerene and a nanotube is actually manufactured from the phase transition by uniting the file of a new crystal from the carbon caught by the electrical discharge. An atom moves because a force is applied in the phase transition. A wave fluctuates and changes for these three sorts at the time of a phase transition, and it is guessed that motion by the force is born to a particle. Therefore, it is important in the research of CF to observe a power spectrum density especially. 3. White Noise and 1 / / Square Noise An expectation of energy can be obtained from a transition probability of quantum mechanics. When analogy of a fluid and the electricity of direct current are used, the formula of electric current can be made from a variable of time. That time it is possible to change the operational order of integral calculus and square root extraction by making use of orthogonality concerning integral calculus for square of momentum. 8 Then, the momentum calculates from the square root of power. Equation (1) is displayed from Eq. (9) of a paper. 8

i(t) = ep^sJ^

r ^ e - ' + ^ W (1) \ m-K Jx UJ The 1 / / square characteristic of a power spectrum density appears in the expression. Because it is a linear algebra, the same power spectrum density as the expression cannot be shown at the same time by other expressions. Therefore, the current of 1 / / square was decided to this expression. However, the electron makes the white noise when generated from the cathode, and the signal of the Poisson distribution becomes Rayleigh distribution. Also, when the signal is 1 / / square characteristic, the following electron in the period should synchronize initial phase 8 (t). Let us pay attention to 1//square noise having been against nature of this Rayleigh distribution. In Rayleigh distribution, amplitude strength R is normal distribution p{R) because of the random probability process. Rayleigh distribution formula is shown in Eqs. (2) and (3). = ^eXp(-R2/n),

(2)

i(t) = C(t) cos {w0t + 9 (t)},

(3)

p(R)

The current of narrowband i(t) is expressed with alternating current and the feature is in a random jump change of initial phase 8 (£) . However, when initial phase 8 (t) of the electron is synchronized for a long period, the quantum resonance makes 1 / /

558

square noise of Eq. (1). Therefore, we conclude that 1//square noise is nature of the quantum resonance. Then there will be many standing waves of the electron wave by the tunnel phenomenon in the discharge. If the initial phase is a steady value for each wave in the period, 1 / / square noise is synthesized from the standing wave that the amplitude is in inverse proportion to frequency /. The frequency versus power spectrum density can be written in Fig. 2, and the envelope curve be shown in both logarithm graph by the straight line proportional to - 2 .

Figure 2.

Power spectrum density

P(f).

The harmonic component from a basic wave of mir radian is synthesized to the electrical discharge, and many electrons are made to exist in the electrode. If amplitude is inversely proportional to order of harmonics, and the wave number is proportionate to the order, a special standing wave is synthesized. If amplitude is proportional to l / / w h e n the number of basic waves in the electrical discharge layer is mn radian, it is made sure that self-organization become caused to a row of electrons. Also it is in 1//square too. If the electron of the electrical discharge organizes the row, the lattice of the crystal is synthesized from existing probability as in Fig. 3. 8 There is a barrier in the electrical discharge region, that barrier shapes a potential well. Electron wave includes wave packet and standing wave in the potential well. From the harmonic that have the quality of 1 / / in amplitude, the wave is synthesized inside the well as Fig. 3. Function sinz/x is used for the harmonic component because it is a nature that the amplitude is in inverse proportion to the frequency at the phase proportional to wave number. It is a condition that there is wave number of mix in a basic wave between the cathode and the anode discharging electricity. Then, the row of the subdivided small well can be

559

+

(V

1

sin mtof \ - 1/

t

•'ham

W

2,,

1

2

3

4

5

6

7

n„

lAAMAl0

5n

Cathode

Figure 3.

ion (rad)

Anode side

Synthesis of harmonic.

made in the bottom of a big well between cathode and anode. The existence probability is set to the electrode side high. When the harmonic component of the standing wave is synthesized on an easy condition, the line of the particle is found from the free particle group. 8 When harmonic of the standing wave are synthesized, the free particle getting together, it lines up. 1 If the electron propagates into the crystal on any condition, Nakamura's calculation of power spectrum density is always 1//square. 10 The crystal was self-organized from the tunnel resonance of the electrical discharge. And the electrode in a carbon-graphitized layer exists in that Maeda's experiment, 6 ' 9 so the amplification of the resonance is promoted. Therefore, the layer of the electrode helps the resonance, and the result also makes the multiple layers in the electrical discharge part. In the row of barrier on potential well, whenever the quantum propagates, 1//square noise must be made. 10 The difference between 1//noise and white noise is caused from the initial phase 9 if) of Eq. (1). If the freedom of the phase is excluded, then 1//square can be considered to be a basic character of the electrical discharge circuit. White noise and 1//square noise have been explained basically. 4. Force of Resonance Alignment appears at Yham in Fig. 3 and the electron wave build the aligned power. Also in our paper, 8 the power of the electron wave was settled in simple Eq. (4).

560

dfc d£

dE dt

dE(k)dk dfc dt

h

ldE(k) dk

This is thought from the relational expression when the electron propagates in the semiconductor. The free particle moved by the force Fmake the row at the position in which Yham is shown in Fig. 3. 8 Therefore, tunnel resonance is made and it becomes the relation of Eq. (I). 1 0 If initial phase of the wave is does not fluctuate, in the discharge circuit, character of power spectral density is inverse proportion to square of the frequency /. For example, if the electrode is the graphite in Maeda's experiment, expansion of resonance furthermore is promoted because of the graphite, and resonance makes the layer of the graphite in the electrode. 6 ' 9 Therefore, the layer of the electrode helps the resonance, and the result also makes the layer by itself. 5.

1//Noise

The 1//noise will be explained next from principle of 1//square noise. 1//noise is explained also on the basis of the column of particles, which shows in Fig. 3 of 1 / / square noise. This row is same as a crystal. Therefore, the row is harmonic oscillators. If wave packets propagate into the harmonic oscillator, the output of signal is integrated because of Virial theorem. The meaning of integration is a low-pass filter if it is explained as working of the electric circuit. As the result, the square of 1 / / becomes 1 / / depending upon operation. However, action does not work always uniformly. There will be such a resonance, and the resonance changes in tri-stable. The structure of a repetition is increasing resonance. Accordingly resonance of electron wave by power of l / / m a y be promoted by surface structure of an electrode. For instance, it can be expected that a graphitized layer structure promote the resonance more. Promoting resonance, it can expect the type of stratified structure of graphite. As an example, if perylene is observed with STS, there is negative resistance. 11 In the experiment there is negative resistance from resonance. 6. Parametric Amplification The crystal is made as a free particle queues up in the electrical discharge. Then, the quantum can propagate under the crystal similarly to a semiconductor as Fig. 4. Then, the soliton u propagates while shaking the lattice. The lattice is made up of Shrodinger equation and the propagation of u is made up of Soliton equation.

L4> = e^

L= -

f|-x

561

Figure 4.

Propagation of Soliton.

There is an answer according to a paper by Kimio Ueno.

dt

[B,L]

.(x,t)

dx

logr(a;,t).

(5)

It is settled to a nonlinear equation (j^r — [B, L\) <j> = 0 that causes the amplitude modulation wave and the parametric amplification. The lattice of the crystal consists of the array of the particle. Each particle vibrates. Then, the amplification arises if the quantum passes many potential barriers by the tunnel phenomenon. When three waves become complete in the condition for the resonance, the wave is amplified in the parametric nonlinearly 13 (Fig. 5). d2x0 , —

2

+01X0

d2£i

=

~pxix2,

- u2x\ = -f3x0x2,

d2X2

- UJ2X2

dt2

=

U)Q = LJ\ +

Figure 5.

~/3x0x2, ljj2.

Harmonic Oscillator.

562

The condition for amplification is quite same as the amplitude modulation composed of carrier wave, signal wave, and modulated wave. If there is resonance, it can calculate conservation of energy in even the wave. 13 The condition of an insufficient quantum in the wave is supplemented because of the parametric amplification. There is a multiplication product of the wave in term mp if the potential of Schrodinger equation is assumed to be a soliton at that time. When the term from multiplication of the wave is explained from theory of communications engineering, it is amplitude modulation. An envelope curve from the signal of amplitude modulation is always seen. Therefore, because it is visible with anytime, one of feature of fluctuation is explained well. 7. Characteristic of Resonance When it is P(f) oc 1 / / , power spectral density P, is in inversely proportional to the frequency / in 1 / / noise. If we display in formula, it becomes P(f) = C/f. The C is constant. By the way, white noise indicates P(f) = C. Also it can rewrite to P(f)fo = C. Also 1/'fz noise is P(f) oc l / / z , it can be written to P{f)fz = C. There is always an equation P(f)fm = C that it looks like the equation P(f)fo — C of the oscillator at Planck's black body radiation. White noise occurs from law of equipartition of energy. Therefore, the feature of P(f)fm = C like law of equipartition of energy is every resonance. 8. Conclusion Free electron is discharged by tunneling at the time of electric discharge to the air by the cathode. Therefore, free particle and matter wave exist in tunneling. Also at least three kinds of resonances exist in electron. When it fluctuates alternately with three interspecific, phase change occurs in "plasma crystal"of the electron wave. In electric discharge of a direct current, the feature of a phase transition is found in many examples. The conduction of heat with a sudden temperature change occurs to the electrical discharge as an example of the phase transition at the electrostatic cooling phenomenon. 14 Graphite in electric discharge is changed into fullerene or nanotube. 7 There is a technology to control single atom when the atom is transported with the tunnel microscope. 15 Similarly, "the plasma crystal" is made from the gravitation of the electron wave. We would like to propose that these features prove phase transition. When free particles are contained in the material placed between the electrodes, the material wave is the same condition even if it is not an electrical discharge. For example, if the tunnel phenomenon has occurred in a solid solution, a semiconductor, electrolysis liquid, and gas, a phenomenon of same class will occur. We would like to propose that CF is fluctuation of the resonance, which happens to the material like a semiconductor.

563 Acknowledgments I would like to t h a n k and appreciate Dr. Hiroo N u m a t a for his help. I would also like to t h a n k J C F to make the paper successful.

References 1. 2. 3. 4. 5. 6.

7. 8.

9.

10.

11.

12. 13.

14. 15.

http://annex.jsap.or.jp/hokkaido/ yokousyuu39th/B-29.pdf (in Japanese). H.M. Thomas and G.E. Morrill, Nature (London) 379, 806 (1996). F. Melandso, Phys. Plasmas 3, 3890 (1996). S.V. Vladimirov and O. Ishihara, Phys. Plasmas 3, 444 (1996). S.V. Vladimirov, P.V. Shevchenko, and N.F. Cramer, Phys. Plasmas 5, 4 (1998). S. Sugita, Y. Mera, and K. Maeda, Origin of low frequency noise and l//fluctuations of tunneling current in scanning tunneling microscopes, J. Appl. Phys. 79(8), 4166-4173 (1996). Y. Hayashi, Dusty plasmas and carbon fine particles, J. Plasma Fusion Res. 78(4), 320-324 (2002) (in Japanese). M. Ban, Composition of 1 / / amplitudes electron wave and a work of one dimension of lattice, Proceedings of the J^th Meeting of Japan CF-Research Society, Morioka, October 17-18, 2002, p. 90-94. K. Maeda, S. Sugita, H. Kurita, M. Uota, S. Uchida, M. Hinomaru, and Y. Mera, Spatial variation of 1//current noise in scanning tunneling microscopes, J. Vac. Sci. Technol. B12(3), 2140-2143 (1994). T. Haga, Y. Takane, and K. Nakamura, I / / 2 law in one-dimensional quantum transport: an example of weak chaos in quantum systems, Chaos Soliton. Fract. 5(7), 1077-1083 (1995). M. Okuda, H. Inaba, H. Naitou, J. Ehara, and T. Takagi, Negative resistance of the organic membrane with STS, IEICE, Technical Report, OME 93-56 (1994-03) (in Japanese). K. Ueno, Suurikagaku, Soritonnga Hakobu Mugennno Sekai 387, 42-47 (1995) (in Japanese). T.Taniuti, K.Nishihara, and Iwanamisyoten, Nonlinear Waves pp.10-11, 88-91, 100127, 1998 (in Japanese), Pitman Advanced Publishing Program, Boston, 1983; Translated from the Japanese edition. K. Kisi and H. Eda, Electrostatic cooling, J. IEIC9/77 60(9), 1044-1046 (1977) (in Japanese). D.M. Eigler and E.K. Schweizer, Positoning single atoms with a scanning tunneling microscope, Nature 344(5), 524-526 (1990).

T Y P E S OF N U C L E A R F U S I O N IN SOLIDS

NORIO YABUUCHI High Scientific

Research Laboratory, 204 Marusen 28-16 Marunouchi, Tsu City, Mie 514-0033, Japan E-mail: [email protected]

Building,

The author has been fortunate enough to encounter both types of nuclear fusions, and so hereby presents a theory regarding these two fusion types. The first phenomenon that may be considered is thermonuclear d-d fusion in a vacuum crack within a solid. When a platinum plate is connected to a positive electrode and a palladium-alloy plate is connected to a negative electrode in deuterium and a 200-V electrolysis current is passed through them, neutrons, helium 3, and 3.27 MeV of heat are obtained. The fact that such a phenomenon is produced despite the low voltage suggests the following: first, a vacuum microcrack is produced within the palladium alloy. Next, a large quantity of Bose-particle deuterium nuclei flow into the crack as impurities due to the Kondo effect. Accordingly, the effect of the Heisenberg uncertainty principle (Ax Ap > h) is exerted, the movementposition range of the deuterium nucleus becomes extremely small ( i - t 0), and the movement amount gradually increases (p(mv) —> oo). Integrating this movement amount yields J mv dv = 1/ 2mv2 + C, and when the movement energy of this 1/2 mv2 exceeds 10 keV, thermonuclear fusion occurs. The second phenomenon is that of the experiment conducted by Iwamura et al. this is elemental transmutation due to nonthermal nuclear fusion in a solid by deuterium permeation. In this case, coating the surface of the palladium alloy facing the deuterium gas with cesium resulted in the creation of praseodymium, and coating the surface with strontium resulted in the creation of molybdenum. Common points in these phenomena are the facts that the atomic number increased by 4 and the atomic mass by 8. In this regard, it appears that the transmutation was the result of nuclear fusion of the cesium or strontium with two compound nuclei of deuterium.

1. Fusion Due to Condensation Within a Vacuum Crack in a Solid The next thought experiment that may be considered is nuclear fusion that occurs due to the condensation of deuterons within a vacuum crack formed in the surface of a solid. When deuterons ionized at 20 eV aggregate in large numbers within a vacuum crack in hydrogen-absorbing metal and are enclosed by the walls of the metal, it is believed that due to the effect of Heisenberg's uncertainty principle, they are excited to 10 keV and quantum tunneling causes the nuclear fusion among the deuterons. This is similar to the phenomenon of hurricanes caused by the aggregation of large amounts of air molecules in locations of relative vacuum in the 564

565

atmosphere; the wind energy of a hurricane caused by the inrush of air into lowpressure areas due to a temperature differential of only 20° C can be tremendous amount, equivalent to 300,000 thermonuclear bombs. The energy of the deuterons that are excited in a vacuum crack can be determined by this equation: h/Ax = 10 keV.

(1)

2. Structure of the Atomic Nucleus The Platonic structure of the atomic nucleus as intuitively understood by the author is as follows. A tetrahedron, indicated by T, has four apices, and a neutron (n) or proton (p) exists at each apex. Similarly, a cube (C) has eight apices, an octahedron (O) has six, an icosahedron (I) has 12, and a dodecahedron (D) has 20, with an n or p at each. Because a Platonic regular polyhedron may be both inscribed and circumscribed on spherical surfaces, spheres having the same center and different radii form shells, with regular polyhedra both inscribed and circumscribed on each, thereby forming superimposed layers. A jHe nucleus has a T-structure, and at its four apices there are two p and two n. Accordingly, 4He[T] = (2n + 2p).

(2)

^ 0 [ T , I] = (2n + 2p, 6n + 6p) = (8n + 8p).

(3)

Next,

Here, the I is circumscribed on the sphere on which the T is inscribed, with two n and two p in the inner shell and six n and six p on the outer shell, for a total of eight n and eight p. Next, toCa[C, I, D] = (4n + 4p, 6n + 6p, lOn + lOp) = (20n + 20p).

(4)

Also, lgNi[C, D][T] [C, D] = (4n + 4p, lOn + 10p)(4n)(4n + 4p, lOn + lOp) = (14n + 14p)(4n)(14n + 14p) = (28n + 28p + 4n).

(5)

This has a [T] sphere interposed between and interlinked with two [C,D] spheres. Next, 1

£gS[T ) C,0,I,D][T 1 C ) 0][T,C ) 0 ) I ) D] = (25n + 25p)(18n)(25n + 25p) = (50n + 50p + 18n).

(6)

566

Next, 208 82 Pb[T,

C, O, I, D] [C] [I, D] [C, D] [I, D] [C] [T, C, O, I, D]

= (25n + 25p)(8n)(16p + 16n)(28n)(16p + 16n)(8n)(25n + 25p) = (126n + 82p).

(7)

Here, the magic numbers 2, 8, 20, 28, 50, 82, and 126 are obtained by fulfilling the structure of regular polyhedra. They yield a nuclear structure that is stable. The correctness of the Yabuuchi model of the atomic nucleus according to the structure of Platonic regular polyhedra is verified by the following explanation of the nuclear-fission ratio of uranium (see Fig. 1). P

23n+23p Figure 1.

n

23n+23p

23n+23p

Structural diagram of | | 8 U atomic nucleus based on Platonic philosophy.

238 92 U[C,

O, I, D] [T] [C, O, I, D] [C, O, I, D] [C, O, I, D] [T] [C, O, I, D] (23n + 23p)(4n)(23n + 23p)(46n)(23n + 23p)(4n)(23n + 23p), 96 T 140 + 2.

(8)

(9)

238

Fission of U atom at an atomic weight of 96:140 is shown by the arrow in Eq. (7). It is believed that two nucleons are split by collision with an incident neutron. This explains why fission of uranium occurs at an atomic-weight ratio of 96:140 (see Fig. 1). 3. Fusion of Nuclei in a Liquid-Crystal State The author obtained the chemical formula shown in Eq. (8) for the nuclear fusion of liquid-crystal ^fCs with 2(2D)-that is, two 2D liquid crystal compound nuclei— rather than with helium, which presents strong proton reaction. Atomic nuclei that have become liquid crystals in nanometer-order space are, respectively, arranged

567

and bonded in blocks that have crystallized into Platonic structures. Because these bonds are between liquid crystals, the attraction between the respective blocks is weakened by the large distance between the blocks. Here, blocks are indicated by square brackets ("[.]"), and the bond between two blocks by a dash ("-"). Because the distance between two bonded blocks is large, the proton reaction can be termed small. At JCF4, the author described how the spherical surface of the shell is externally and internally tangent with the Platonic Yabuuchi structure, yielding the nuclear chemical formula for 1 | | C s shown in Fig. 2. The items have been labeled to aid understanding. 9 *

-7

•

'<•'','

*

rn

;it ft, t

(b)

" ^

(c)

Figure 2.

11 •

>

•.s I

(a)

^ ,

K1

•

•'-''/' - 1 _•

• (I

: »

•

"-'#"2»'-

(d)

(e)

# : Proton o : Neutron

Liquid-crystal nucleus structure of 55 3 Cs.

ilCsfT, C, O, ID] - [T] - [T, C, O, I - 7] - [O] - [T, C, O, I, D] = (25n + 25p)(2n + 2p)(23n)(3n + 3p)(25n + 25p).

(10)

The third term from the left hand side of Eq. (8) represents the outermost shell, which in terms of Platonic structures is an icosahedron, indicated here as an I-polyhedron. As shown here, its configuration has been stripped of seven crystalline nucleons (here neutrons). The state in which the two 2D units in Eq. (8) react is indicated by Eq. (9). ^ 2 ( n + p) + 2(n + p) + 1 ^ C s , = (25n + 25p)(2n + 2n + 2p + 2p)(23n)(2n + 2p + 3n + 3p)(25n + 25p).

(11) (12)

Equation (10) depicts the state in which the 2D units in the second (b) and fourth (d) blocks of the nucleons of the 1 | | C s nucleus have undergone liquid-crystal fusion. Because items (b) and (d) have fewer protons than the other items, proton reaction is small. Item (c) is a crystal composed solely of neutrons and lacking protons, and so because it has no power to attract the neutrons of the liquid-crystal compound nucleus 2(n+p), the 2(n+p) block is the result of reaction between (b) and (d). Its shell structure cannot be explained in terms of Victor Weisskopf's

568

Platonic structures. Further, under the solar-system model of the atomic nucleus, the reaction between (b) and (d) seen here cannot be produced by proton reaction. = (25n + 25p)(4n + 4p)(23n)(2n + 2p + 3n + 3p)(25n + 25p),

(13)

141 P r [ T , C , 0 , I , D ] - [ C M T , C , 0 , I - 7 ] - [ T , O M T , C , 0 , I , D ] . 59

(14)

Equation (11) indicates the change in the numbers of protons and neutrons that occur due to nuclear reaction in the blocks within the atomic nucleus. In the atomic nucleus that has undergone nuclear change to become ^gPr, indicated by Eq. (12), in the second block, (2n+2p) has become (4n+4p), indicating that the T-polyhedron (tetrahedron) has reacted to the C-polyhedron (cube) and changed. Similarly, in the fourth block, (2n+2n) has become (2n+2p+3n+3p), indicating that the O-polyhedron (octahedron) has changed to a T-polyhedral structure in the inner shell and an O-polyhedral structure in the outer shell. This is as shown in Fig. 3.

4 m, • m * * * • • *

: :

i ! .

*++

"

•••

• •

. ! ! . ! :

« *%•

7 . " ' - . ,T

'- • •

'

• • . . . ; •

•

•

•

•"#'-•

. ' . . - . - .

•::

;:


;. ' . . ' / / ' . . .

•

: :

,,«*

v

• ** ' . .

* P

<:

:

**'•,*• *

*

*

_

»

'• - v

•

*•'

• m : Proton :;; : Neutron

Figure 3.

Liquid-crystal nucleus structure of g ^ P r .

The result is as follows: 133Cs ri„ +i 2o • on 2D -v. =>141 ^ P r + AE. (15) 55 The reason why a change in the crystal is produced because of the change in the numbers of neutrons and protons is related to Kepler's theory of space-filling polyhedra and to quantum change in spaces, and like the mystery of crystallization of snowflakes, remains a topic for future study. Nuclear reaction can be explained similarly for g|Sr as well. This is represented first by Fig. 4, followed by the chemical formula. l|Sr[T, C, O, I, D - 12] - [I] - [T, C, O, I, D - 12] = (19n + 19p)(12n)(19n + 19p), ^ l S r + 2(n + p) + 2(n + p),

(16) (17)

569

(b)

(a)

(c) i : Proton :"; : Neutron

Figure 4.

Liquid-crystal nucleus structure of II Sr

2(n + p) + (19n + 19p)(12n)2(n + p) + (19n+ 19p),

(18)

(21n + 21p)(12n)(21n + 21p),

(19)

Mo[T, C, O, I, D - 8] - [I] - [T, C, O, I, D - 8].

(20)

The result is as follows: §|Sr + 2 • 2D =•

HMO

+ AE.

(21)

Figure 5 shows Eq. (18).

Because item (b) in Eq. (14) is composed entirely of neutrons and does not attract protons, the 2D does not react. Accordingly, items (a) and (c) are each lacking six neutrons and protons, for a total of 12, and the 2D reacts ate locations. The riddle of nuclear fusion is thus explained. The bonds described are not formed in a chaotic integral atomic nucleus. Fusion can take place in an atomic nucleus having crystalline blocks with weak bonds.

570

References 1. Y. Iwamura, Detection of anomalous elements, X-ray, and excess heat in D2-Pd system and its interpretation by the electron-induced unclear reaction model, Fusion Technol. 33(4), 387-500 (1998). 2. V.F. Weisskopf and E.P. Rosenbaum, A model of the nucleus, Sci. Am. 193(6), 4-91 (1955). 3. M. Brack, Metal clusters and magic numbers, Sci. Am. (1997). 4. W. Green, Cold Fusion 12, 28, 29, 31 (1995). 5. C. Illert, Cold Fusion 13, 28-29 (1995). 6. N. Yabuuchi, Low-speed nuclear fusion, Cold Fusion 17, 11, 16-19 (1996). 7. S.M. Austin and G.F. Bertsch, Halo Nuclei. Sci. Am. (1995). 8. N. Yabuuchi, Proceedings of the Fourth International Conference on Cold Fusion, Vol. 4; Theory and Special Topics Papers. TR-104188-V4 Proceedings, Lahaina, Maui, Hawaii (July 1994, December 6-9, 1993).

NEUTRINO-DINEUTRON REACTIONS (LOW-ENERGY N U C L E A R R E A C T I O N S I N D U C E D B Y D 2 GAS PERMEATION THROUGH PD COMPLEXES — Y. I W A M U R A EFFECT)

V. M U R O M T S E V A N D V. P L A T O N O V State Scientific

Centre of Russian Federation Karpov Institute Vorontsovo Pole Street, 103064- Moscow,

of Physical Russia

Chemistry,

10,

I. SAVVATIMOVA Federal State Unitarian Enterprise Scientific Research Institute 142100, Podolsk, Zhelesnodorozhnaya Street, 24, Moscow region, E-mail: [email protected]

"Luch", Russia

Anomalous elemental changes have been observed on the Pd complexes after D2 gas permeation. This effect—effect Y. Iwamura—belongs to a new category of nuclear reactions. The effect of Y. Iwamura can stimulate development of physics of electromagnetic interaction neutrino including physics of relic neutrino and physics of the dineutrons. It is possible to suggest that low-energy neutrino and even relic neutrino can initiate effect of transmutation in special cases. The suggested hypothesis application about new class v~ nuclear reaction existence can be useful for the problems: alternative energetic, radioactive isotopes reducing and rare isotopes production.

1. Introduction Recently some experimental evidences confirming the assumed existence of the relic neutrino and the anomalous neutrino magnetic moment have been obtained. The said assumption is based on the concept of occurrence of stable dineutrons; the function of neutrino and dineutrons in phenomena studied by physical chemistry and low-energy physics. The existence of bound states of neutrino (latent) with protons, deuterons, and other nuclei follows from the well-known estimations of anomalous neutrino magnetic moment 1 and the Dirac's equation. 2 ' 3 The concept of relic neutrino leads to the possibility of the neutrino component of the matter. If we assume the existence of the neutrino component of the matter, the question arises as to whether these neutrinos are capable of initiating nuclear transmutations. Nuclear experimentation evidence shows that small quantities of nuclei occur in excited meta-stable nuclear states. Capture of neutrino by the said nuclei may trigger transition from the excited meta-stable states to the basic one and lead to the output of energy sufficient to initiate nuclear transmutations. 571

572

The above concept provides grounds to study the problems of neutrino and the dineutrons function in a number of processes, discovered in experiments in allied areas of physical chemistry and nuclear physics. One of the approaches to the study of neutrino physics may be focused on investigation of reactions of the following type.

ue + fX - £- 2 X + 2n +i e ,

(1)

where 2 n represents dineutrons. ve +

N

ve +

N

zX

zX

-^ -

N

zZp.

+

4

2Be

+ 2n + i e ,

£r 6 14 X + l2C + 2 n + ie,

(2) (3)

i e = e + ve e~ bound states of neutrino with the electron-positron pair (the particle called "iton" by Dr. T. Matsumoto). Reaction (1) may be termed as neutrino-dineutron reaction. ' 5 Reactions (2) and (3) may be regarded as initiated neutrino-cluster reactions of helium and carbon decay.6 The assumption on the occurrence of reactions (l)-(3) appeared as a result of the study of the background gamma spectra formation in germanium gamma spectrometers, used in astrophysical research. 4 Given below is experimental evidence on the existence of reactions (l)-(3). The data proving the existence of the above reactions are also provided f X +

2

n ^

£+ 2 X +

£ X + ^2C -+ ™*X

7,

(4)

+ 7,

(5)

£ X + ^He -+ £+24X +

7.

(6)

The study of the assumed existence of reactions (l)-(6) may be regarded as one of the goals of the present investigation. It is suggested that these reactions are accounted for by the electromagnetic low-energy neutrino interaction. According to the assumed hypothesis a number of protons p + and deuterons D + occur in plasma in bound states (latent) of protons and deuterons with neutrino (p+i^e and D+^ e , respectively). As a result of a collision, for example, of deuteron with neutrino in a latent state with the Pd cathode surface, part of the neutrino may be captured by Pd isotopes. D+i/e + P d ^ D + + P d ^ e .

(7)

The bound state of some isotopes with neutrino decays in some cases in accordance with reactions (l)-(3).

573

2. Experiments with Glow Discharge (GD) Proceeding from the assumed occurrence of reaction (3), isotopes with masses 90 and 91 are formed in the reactions. 7 ' 8 IgZr +l2C

+

2

v, + ^ P d

-

n+ie,

(8)

ve + IfPd

-+ %Zv + l2C + 2 n + i e .

(9)

Among stable Pd isotopes, only 1 0 5 Pd has other than zero magnetic moment. 1 0 7 Pd isotopes were discovered in the Pd cathode. This effect can be accounted for by the dineutron capture by 105 Pd (4). 2

n+105Pd-^

107

*Pd + 7 .

(10)

Figure 1 in Ref. 7 shows activity decrease curves in silver foils after the exposure in the vicinity of the Pu-Be neutron 105 C _1 -active source and after the exposure of Pd to D in the GD chamber (at the same distance). Both curves correlate with the silver 110 half decay period. The effect of the neutrons flow upon the silver foil may lead to 110 Ag isotope formation. n +

109

Ag

-•

110m

Ag

+

7.

(11)

Beta-minus 110 Ag isotopes decay leads to formation of beta-electrons with 2.87 MeV energy. The 110 Ag isotopes half decay period amounts to 24.6 s. The curves of the emission intensity sharply decline in the silver foil after the exposure to those of the GD exposure. Assumedly, GD emits a dineutrons flow and the exchange reaction takes place: 2n

+

107 A

g

_>

107mpd

+

d

(12)

It results in formation of 1 0 7 m p d isotopes meta-stable states. The half decay period of 1 0 7 m Pd isotopes meta-stable states is equal to 21.3 s. Therefore, it is essential to determine the type of the silver foil emission: electrons flow or gamma-emissions with 215 keV. Gamma quanta may be generated (occur) as a result of 1 0 7 Pd isotopes transfer from the meta-stable state to the basic state. Stable dineutrons were initially discovered in investigations of Japanese physicists.9 3. Nuclear Transmutations in Electrolysis 1 0 It was discovered that post-experimental Ni content in 2000 A -thick thin-film nickel coatings decreases markedly as a result of electro-chemical process and new elements appear in significant quantities among which there are Fe, Cu, Zn, and Mg. Specifically high carbon content is registered. The experiments provide evidence that lowenergy interactions in electro-chemical cells initiate nuclear transmutations. The said phenomenon was reproduced in Ref. 11 (Table 1). It was discovered that there

574

appeared about 24% of carbon isotopes in the Pd cathode near-surface layer as a result of the electro-chemical process. Presumably, reactions of carbon cluster decay (3), initiated by neutrino's capture occur in these processes. Table 1. Results of the SEM analysis on Pd thin foil cathode Element

Atomic concentration (%)

C Pd

23.68 76.32

4. Effect of Y. Iwamura (Nuclear Transmutation Induced by Deuterium Permeation through the P d Complexes) In Refs. 12-14 processes in multi-layer Pd were investigated. The Pd complex consisted of bulk Pd at the bottom, alternating CaO and Pd layers, and a Pd thin film at the top Fig. 5 in Ref. 12 outlines this process. In Ref. 12 it was discovered that some carbon isotopes are found on the surface of the Pd complex. The diffusion of deuterium through the Pd complex leads to the decrease of the carbon content on its surface. At the same time Mg isotopes appear (Fig. 2 in Ref. 13). The data obtained allows us to suggest that the following reactions take place. 12C

+

12C ^

24Mg

+

T

(13)

Presumably, the diffusion of D through the membrane should be regarded as neutrino transport (in neutrino-deuteron bound state) and initiation of neutrinotransfer reaction (7). As a result of neutrino capture, reactions (3) may be triggered, which lead to 12 isotopes formation. In one of the experiments, 7 Li isotopes had been implanted into the surface of the Pd complex. 1 9 F isotopes were discovered in the surface layer after D diffusion through the Pd complex. It is possible that the following reaction type was observed in Ref. 12 \U + ?C - l9F + 7 . (14) Natural Ba was deposited on some samples using the electrochemical method, in a 10 mM Ba(OH) 2 solution. On other samples, a special form of Ba with enriched 137 Ba was deposited, in 7.3 mM Ba(NC>3)2 solution. Figure la shows natural Ba mass spectrum. Mass peaks of 134, 135, 136, 137, and 138 are observed on the spectrum. Sm isotopes are discovered in the Pd complex with implanted Ba. Figure l b represents this effect. The quantity of formed 150 Sm isotopes is less than that of 148 Sm or 146 Sm isotopes. In D diffusion through the Pd complex the quantity of 150 Sm isotopes increases dramatically. The rate of odd Sm isotopes formation is relatively small. No odd mass peaks are observed within the spectrum (Fig. 1). Figure 1 shows two mass spectra within 146-150 mass range. One of the spectra was obtained as a result of Ba isotopes implantation into the Pd complex. Ba and Sm isotopes were registered in the Pd complex after the electro-chemical experiment.

575

2x104 B

Ba

1.5 x 1 0

4

1 x104 5000

JKJ^JU, 133

{134

1|35

1)36

1^37

[138 139

1500

1000

500

146

147

148

149

150

151

Figure 1. (a) The secondary ion mass spectrometry (SIMS) spectrum of natural Ba. (b) SIMS spectrum of Pd complex with natural Ba after D2 permeation.

The second mass spectrum was obtained after D diffusion through the Pd complex, containing Ba and Sm. A dramatic change in the intensity of the mass peaks was observed after D diffusion. The data in Fig. 1 was obtained with natural abundance barium isotopes. After barium had been implanted into the Pd complex 146, 148, and 150 mass peaks appeared in the mass spectrum. This may be explained by the assumption that the electrochemical process of Ba implantation triggers reaction (3) and fusion reaction (5) and the following reactions take place 134

56 136

56 138

56

Ba D a

+

12/-. 6 ^

-

6fSm

+ 7,

(15)

o a Ra

+

12ri 6 ^

-

IfSm

+ 7,

(16)

Ra u a

+

12/-. 6 ^

8°Sm + 7-

(17)

- y

No 147 and 149 mass peaks are observed on the spectrum in Fig. 1. This suggests that the cross-section of 12 C capture by odd 137 Ba isotopes is less than by even Ba isotopes (Ba mass spectrum, enriched with 1 3 7 Ba). 137 Ba content is about 60 times bigger than that of 138 Ba. As a result of D diffusion through the Pd complex (enriched with 137 Ba) 149 mass peak shows the maximal intensity. It suggests that the nuclear reaction of the below type is going on: 137 56 Ba

+ iC

IfSm

(18)

576 Nuclear reactions in diffusion processes are observed only in P d complexes containing an intermediary layer with Ca isotopes. 1 2 _ 1 4 T h e neutrino capture cross-section in reactions (3) with Ca isotopes is much bigger t h a n in reactions of this type with P d isotopes. In reactions (3) with Ca isotopes appear Si isotopes: i/e + $ C a 5.

-> l84Si + l2C

+

2

n +ie

(19)

Conclusion

T h e most controversial are the following problems: the existence of the neutrino component of the matter, the ability of low-energy neutrino to initiate nuclear transmutations, and the existence of stable dineutrons. Many researchers made a t t e m p t s to find stable dineutrons, but they failed. 15 T h e experiments aimed at discovery of stable dineutrons were based on o u t d a t e d estimation of bound energy between two neutrons in a dineutron. According to these estimations the bound energy between two neutrons in a dineutron was assumed equal to about 3 MeV. 1 5 New evidence shows t h a t the bound energy between two neutrons in a dineutron amounts t o a b o u t 22 MeV. T h e system of q u a n t a states in a dineutron was studied in Ref. 16. T h e first and the second q u a n t u m states with energies of 3.6 and 11.6 MeV, respectively, were discovered.

References 1. A. Suzuki, M. Mori, K. Numata, and Y. Oyama, Phys. Rev. D 4 3 (10), 3557 (1991). 2. I.M. Ternov, V.G. Bagrov, and P.V. Bozrikov, News of higher educational institutions, Physics 11, 38 (1971). 3. A.O. Barut and J. Kraus, J. Math. Phys. 17(4), 506 (1976). 4. V.I. Muromtsev, P.A. Muromtsev, and V.A. Chelishev, Gravitation and Cosmology, (Supplement) 8, 227 (2002) Moscow. 5. V.I. Muromtsev and V.A. Chelishev, Russian Fed. Patent #2145095 (2000). 6. K.N. Mukhin and O.O. Patarakin, Successes of Phys. Sci. 170(8), 855 (2000). 7. A.V. Karabut, Ya.R. Kucherov, and LB. Savvatimova, Fus.Tech. 20, 924 (1991). 8. LB. Savvatimova and A.B. Karabut, Surface, Vol.1, Moscow: RAN (1996). pp. 63-75. 9. M. Sakisaka and M. Tomita, J.Phys. Soc. Japan 16, 2597-2598 (1961). 10. G.H. Miley and J.A. Patterson, Infinite Energy 2(9), 932 (1996). 11. Dan Chicea, ICCF9, China (2002), p. 53. 12. Y. Iwamura, T. Itoh, and M. Sakano, ICCF8 (2000), p.141. 13. Y. Iwamura, M. Sakano, and T. Itoh, Jpn J. Appl. Phys. 4 1 , 4642-4648 (2002). 14. Y. Iwamura, T. Itoh, M. Sakano et al., ICCF11, Marseilles, France (2004). 15. JU.A. Alexandrov. Fundamental properties of a neutron, I., Atomizdat, 1976. 16. D.V. Alexandrov, E.JU. Nikolsky, B.G. Novatsky et al, Letters in J. Tech. Phys. 67 (11), 860-865 (1998).

A N E X P L A N A T I O N OF E A R T H Q U A K E S B Y T H E BLACKLIGHT PROCESS A N D H Y D R O G E N FUSION

HIROSHI YAMAMOTO 3110-17

Tsuzuki,

Mikkabi-Cho, Harnamatsu-City, Shizuoka-Pref. E-mail: [email protected]

431-1402,

Japan

The recent deployment of many seismometers and occurrences of earthquakes in Japan revealed explosive nature of earthquakes. There have been a few reports that earthquakes and eruption of helium gas took place simultaneously, but there has been no hypothesis to correlate each other. Recently, a new idea that atomic hydrogen can generate energy through a mechanism between chemical reaction and nuclear reaction by lowering the electron orbit from the ground state to lower state has emerged. A hydrogen atom with much lower orbit below the ground state naturally has lower Coulomb barrier and would be much easier to fuse each other, resulting in the generation of helium. It is known that water injection into deep wells can cause earthquakes. Water can be dissociated into atomic hydrogen by metals in a very hot condition at the mantle. This paper proposes a hypothesis that the power source of earthquakes is hydrogen fusion, which takes place after accumulation of atomic hydrogen gas and subsequent pressure drop due to cracks of the surrounding rocks.

1. Introduction The mechanism of earthquakes is currently explained by the plate-tectonics theory, which claims the earth's surface is covered with a series of crustal plates that can store elastic energy caused by relative movement of each plate. But recent observations of slow slips of crustal plates by Global Positioning System (GPS) dismiss this idea and more plausible explanation is requested. It seems there are two ways to generate excess energy from hydrogen and its isotope. One is fusion and the other is to drop the electron in hydrogen atom from the ground state to the lower one. The latter one is quite controversial to the current quantum physics and very few scientists in cold fusion research paid attention to it, but it was shown that it can explain anomalous combustion phenomena such as very powerful explosions of hydrogen and oxygen mixture dissociated from water due to nuclear irradiation at nuclear power plants. 1 If one cannot find the cause of earthquakes, then, the next step is to study how human activities induced earthquakes and then to deduce a possible mechanism of earthquakes from the correlations between what was done and what happened. 2. Earthquakes Induced by Human Activities In 1961, a deep well was drilled at northeast of Denver Colorado, USA for disposal of nuclear waste fluids. Injection was commenced March 1962, and shortly after 577

578

that, an unusual series of earthquakes erupted in the area where earthquakes are very seldom. Water injection had been discontinued and the number of quakes decreased dramatically. When the injection was resumed, quakes increased accordingly and the link between the water injection and earthquakes was established. 2 The most notable experience in this series of earthquakes is that many people heard extremely loud, explosive-like earth noises. 3. Horizontal Movement on the Surface at the First Shock Recently, many seismometers have been installed across Japan. In the event of the Niigata-ken Chuetsu earthquake, which took place October 2004, three seismometer stations within 7 km from the epicenter recorded the movement of the surface. Two of them are too close to the epicenter to evaluate the horizontal movement by the first shock but they clearly recorded sharp jerk as if an explosion took place just beneath the stations. Ojiya-Shirouchi is 7 km away from the epicenter and a good place to assess the first movement by the quake. According to the plate-tectonics theory, the movement of Ojiya-Shirouchi at the first shock should be toward the fault line as is shown in Fig. 1, but, the recorded movement is quite opposite. If it were assumed that an explosion took place at the epicenter (13 km underneath the ground), it can be expected that the movements of Ojiya-Shirouchi would be opposite direction to the epicenter. The recorded movement is toward west and is in accordance with this assumption as is shown in Fig. 1. This fact strongly suggests that earthquakes are driven by some kind of explosions.

•4

Qiya-Shirouchi

*

(7 km)

J

Fault line

X-.

Movement at the first shock .. . on the surface

-.,. • .,_ . , . V (Epicenter) .*

Movement anticipated by plate-tectonics

Figure 1. Location of a seismometer and direction of the movement at the first shock (Source: Japan Meteorological Agency home page, http://www.seisvol.kishou.go.jp/eq/kyoshin/ jismn/041023jiiigata/1756/nigata_main.htm).

579

4. Generation of Atomic Hydrogen The Earth's crust is divided into several separate solid plates. Subduction occurs when two plates collide and the edge of one dives beneath the other. The crust contains water and when it contacts with hot magma, metals in magma such as iron produce atomic hydrogen according to the following reaction. 3Fe + 4H 2 0 - • 8H + Fe 3 0 4

(1)

where "H" designates atomic hydrogen. Once atomic hydrogen is produced and if there is no heat sink at the collision point, just a collision of atomic hydrogen for instance; H + H —> H2 (molecular hydrogen) would not take place but just elastically repulse each other. This suggests that atomic hydrogen can exist much longer than normally expected. The pressure and temperature, for instance, at 30 km below the surface of the earth would be over 1 GPa and 1500°C. When the reaction (1) takes place at this condition and atomic hydrogen gas builds up, the pressure of the atomic hydrogen gas would be getting higher and higher and finally there would be cracks at the surrounding rocks, resulting in pressure drop of the hydrogen gas. 5. Anomalous Energy Release from Hydrogen Atom Mills has reported that hydrogen atoms can achieve lower states than ground state by a resonant collision with a nearby atom or combination of atoms having the capability to absorb the energy to effect the transition, namely, an integer multiple of the potential energy of the electron at atomic hydrogen, m x 27.2 eV (TO is an integer). 3 He named this shrunken hydrogen atom "hydrino" and claims that this hydrino can be a catalyst to shrink other hydrinos to further lower states. He named this reaction the BlackLight Process. Figure 2 shows the BlackLight Process. Based on his hypothesis, he developed a model in which energy is generated through a mechanism between chemical and nuclear reaction.

.

Catalyst /

Ionized and later reduced, resulting in energy release Hin

^ j, 0 ~^" ® 1/2 © Atomic hydrogen \Electrort-

v

y

n-l

S

Figure 2.

H

^ ^

V ^ Hydrinos can catalyze further collapse, ionizing one to normal hydrogen

l«

*„'

1 M/3 1,-

>

H,,

H1/n designates a hydrogen whose electron orbit is shrunken to 1/nthe radius of a normal one, named "hydrino"

Mechanism of "hydrino" generation and energy release.

580

The author postulated that 3-body reaction of atomic hydrogen and oxygen can make the BlackLight Process, because ionization energy of hydrogen and oxygen is very close as is shown below. Hydrogen; 13.598 eV, Oxygen; 13.618 eV. If the hydrino model holds, it can be expected that the following reactions can take place: 0 + 0 + H ^ H [ n = l/2]+20++2e",

(a)

H + H + O ^ H [ n = l/2] + H+ + 0 + + 2e-,

(b)

H + H + H ^ H [ n = l/2]+2H++2e~.

(c)

H[n = 1/2] designates a hydrogen whose electron orbit is shrunken to 1/2 the radius of a normal one and these will be shrunken further to lower orbits as reaction continues. Ions and electrons thus produced will recombine, resulting in generation of energy. It is reported that the BlackLight Process can produce up to 200W/cm 3 at 700mTorr. 4 If the BlackLight Process takes places at atmospheric pressure, the power density is about 300 kW/cm 3 , powerful enough to cause an explosion. 6. From Blacklight Process to Nuclear Fusion It can be postulated that if containing vessels are tight enough, well shrunken hydrinos which have a relatively small Coulomb barrier can fuse each other, resulting in generation of helium as a by-product. The Matsushiro swarm earthquakes, which took place in 1965 in Japan ceased after eruption of water and helium gas. 5 This incident strongly suggests that earthquakes are caused by hydrogen fusion. 7. What Triggers Hydrogen Explosion High-pressure molecular hydrogen gas up to 70 MPa is now being used for fuel cell cars but almost no technical information on the stability of high-pressure atomic hydrogen gas is available because it is almost impossible to make such a gas here on the ground. Only information available concerning the initiation of the BlackLight Process is the one carried out by BLACKLIGHT POWER Inc., but these are limited at very low pressure. The BlackLight Process is quite sensitive to the pressure and temperature. It can be expected that the same characteristic curve for the self ignition curve of the stoichiometric mixture of hydrogen and oxygen, known as the explosion peninsula would be applied for the BlackLight Process of 3-body reaction of atomic hydrogen. In the case of the stoichiometric mixture of hydrogen and oxygen at high temperature and high pressure, just a pressure drop can trigger ignition. When the gas pressure of atomic hydrogen reaches such a high pressure that surrounding rocks cannot sustain, gas leakage starts and the atomic hydrogen

581

gas plunges into the area of the BlackLight Process. At B L A C K L I G H T P O W E R Inc. magnetic wave is utilized to induce the BlackLight Process. This implies t h a t an electro-magnetic fluctuation due to solar activities might also be able to initiate the explosion. 8. C a n d i d a t e for t h e P r o o f of t h e P o s t u l a t i o n Lately J a p a n experienced a rather strange earthquake, namely, the Nhgata-KenChuestu earthquake, which occurred on the place with no prominent fault. The distribution p a t t e r n of epicenter of after-shocks is oval, in sharp contrast with typical earthquakes, which have a straight distribution p a t t e r n along the faults. This peculiar characteristic strongly suggests t h a t the CO2 injection into old n a t u r a l gas well located near-by the epicenter of the first major earthquake and subsequent water permeation into mantle might have initiated the earthquake. A probe to measure the permeation of CO2 is installed close to the old n a t u r a l gas well. T h e postulation t h a t earthquakes are caused by hydrogen fusion can be checked by measuring the concentration of helium before and after an after-shocks.

9.

Summary

In the past, it could have been hardly imagined atomic hydrogen gas can explode by itself but the BlackLight Process by Mills opened the way to investigate the cause of anomalous explosion of hydrogen from a new standpoint of view. Considering the very powerful explosion caused by atomic hydrogen and oxygen during cold fusion experiments a n d at nuclear power plants t h a t can not be explained by current combustion theory but can be explained by the BlackLight Process and the relationship between water injection into deep wells and occurrences of earthquakes, it can be reasonably concluded t h a t earthquakes are caused by the explosion of atomic hydrogen gas dissociated from water t h a t is brought deep into the earth by subduction of crustal plates. Furthermore, t h e eruption of helium gas after t h e earthquakes strongly suggests t h a t earthquakes are caused by hydrogen fusion.

References 1. H. Yamamoto, Revisiting Anomalous Explosion of Hydrogen and Oxygen Mixture from a View of Cold Fusion, Proc. 5th Meeting Jpn. CF Res. Soc, pp. 89-92 (2003). 2. N. Craig and R.L. Wesson, Earthquake Hazard Associated with Deep Well Injection-A Report to the U.S. Environmental Protection Agency: U.S. Geological Survey Bulletin 1951, 74 p. 3. R.L. Mills, P. Ray, B. Dhandapani, R.M. Mayo, and J. He, Comparison of excessive Balmer Alpha line broadening of glow discharge and microwave hydrogen plasmas with certain catalysts. J. Appl. Phys. 92(12), 7008-7022 (2002). 4. http://www.blacklightpower.com/pdf/ItalyTech%20Paper%203.27.03.pdf 5. H. Wakita et al., Helium spots: caused by Diapiric Magma from the upper mantle, Science 200, 430-432 (1978).

THEORETICAL MODELING OF ELECTRON FLOW ACTION O N P R O B A B I L I T Y OF N U C L E A R F U S I O N OF D E U T E R O N S

A. I. GONCHAROV* Department of Physics and Technology, Altai State University, Prospect Lenina, 61 Barnaul 656099, Russia E-mail: [email protected] V. A. KIRKINSKII Institute of Mineralogy and Petrography, Siberian Branch of the Russian Academy of Sciences, Prospect Akad. Koptyuga, 3, Novosibirsk 630090, Russia E-mail: [email protected]

In the context of classical mechanics, deuterium atom behavior is simulated under the action of a free electrons flow with no allowance made for the radiation. D-d fusion rate is estimated in a sample of deuterated palladium at temperature 350 K: A > 10"4s-1. A dynamic model of electron orbital deformation (EODD) developed earlier 1 , 2 makes it possible to allow for dynamic effects of outer electron shells on protons and deuteron screening. Now we will find out how metal conductance electrons affect the approach of deuterons and probability of nuclear fusion reactions. At the first stage, within the frame of classical (nonquantum) mechanics, the behavior of a single deuterium a t o m is simulated when acted upon by a flow of free electrons. It is assumed t h a t the particles do not radiate electromagnetic waves. T h e system consists of a deuteron a n d two electrons. At the initial moment, one of the electrons (orbital) is in the circular orbit of Bohr radius 0.529 A. T h e flow of incoming electrons is isotropic; the impact parameter is limited by the value 0.53 A. The incoming electrons appear at the 1 A distance from the deuteron; the kinetic energy of the incoming electrons follows the Fermi distribution with the parameters characteristic of free electrons in a P d crystal a t room t e m p e r a t u r e : 3 / ( e ) = consty/I/{l + exp[( £ -

e*)/kT}},

where e* = ft.2(3ne/7r)3'2/8me is the so-called characteristic energy, ne designates the free electrons concentration, h is Planck's constant, k is the Boltzmann constant; and the absolute t e m p e r a t u r e T is assumed to be equal to 350 K. According to Ref. 3, we assume t h a t for every a t o m there is a single free electron. T h e n n e « NA • p/A. "This work is supported by RFBR (Grant No. 05-05-64930). 582

583

For palladium, ne « 6.8 x 10 22 cm~ 3 , e*/k w 7 x 10 4 K. The average kinetic energy of free electrons in palladium is 3e*/5 « 3.6 eV, the average electron velocity v ?s 1.13 x 10 8 cm/s. After random initial conditions have been specified, particle trajectories are calculated by numerically solving a system, of differential equations of mechanics. Relativistic equations are used but without allowance for magnetic effects, i.e. the particle interaction is considered purely Coulomb interaction. The system of equations is solved by Runge-Kutta method of the fourth order with the relative error less than 10~ 5 . As has already been mentioned, at any instant three particles can be tracked, i.e., two electrons and one deuteron. When one of the electrons travels at a distance exceeding 10 A, the remaining system (unsteady state of deuterium D* atom) is bombarded by a new free electron, etc. iVmax = 104 model experiments have been conducted. Number I of free electrons collisions with the D* "atom" could reach up to / m a x = 100. When one of the electrons approached the deuteron at a distance less than 10~ 13 cm, trajectories were no longer calculated. This implementation of incoming electron parameters was excluded from consideration and a transition to a new implementation of a system took place with an initial Bohr orbit of the deuterium atom. Therefore, the number of simulated D* "atoms", which underwent I collisions with electrons, N{1) < Nmayi. For instance, JV(10) = 9101, N(50) = 3331, JV(80) = 1489, and iV(100) = 847. The total number N* of simulated D* "atoms"

N* = ] T N(l) = 420748 < iV max x J max = 106. i=i

A high proportion of electrons collisions with D* results in the decreased energy of D* and its size. For the D* size the distance r from the electron to the deuteron is taken at the apogee of the orbit. The size distribution density of D*, which underwent I collisions with electrons, will be designated as f(r\l). We had to exclude from our consideration trajectories in the region of small distances in order to prevent the degradation of the trajectories calculation accuracy and to enhance the program response. Special calculations showed that for a significant proportion of neglected trajectories there was a pronounced trend for the electron impingement on the deuteron, which could have resulted in the formation of a bineutron. The program, however, was not yet sufficient to calculate this process accurately enough. Part of the neglected trajectories could have also lead to the formation of D* of even smaller sizes. Those two possibilities potentially can significantly increase the theoretically estimated value of the fusion reaction rate and require supplementary research. For the time being, we assume that under more accurate trajectories calculation all the excluded implementations result in the formation of D* whose size obey the same distributions f(r\l). In this connection,

584

distributions are normalized similarly for any I: f(r\l)dr = 1. o The number I of the D* "atom" collisions with free electrons obeys Poisson distribution Pa(l) with the parameter a; the average number of collisions a is proportional to the electron flow density and time. The main contribution to the reaction rate is made by small D* ( r ~ 1 0 - 1 1 cm) characterized by high mobility. Therefore, the crystal lattice does not significantly preclude D*-D*-collisions. Let us designate the concentration and the total number of deuterons in the active volume of the crystal by n and N, respectively. The proportion of deuterons A, which reacted in a unite time (relative reaction rate) is: 1

A(a) =

'max

i AT

"iV"dT

=

'max

£

£

1=0 OO

PaQ)Pa(m)X(l,m),

m=Q

OO

OO

A(Z, m) = | j d n j dr 2 f(n\l)f(r2\m) 0

0

J dE

va(v)FM(E),

0

where v is the relative velocity of the deuterons, E = /iv2/2; ^ stands for the reduced mass of a deuteron pair; Fu{E) denotes the Maxwell distribution at room temperature normalized as: OO

jFu(E)dE=l. o The cross-section of D*-D*-collisions resulting in a fusion reaction in the quasiclassical approximation is equal to a(v) = SQP(E)/E, where So = 0.55 x 19 2 lCr cm eV; R

P{E) = exp I - y

/" y/2fj,[V{r) - E]dr o

r-l,

where R = V (E) is the turning point of a classical trajectory. It will be assumed that D* "atoms" with the shell sizes r\, r2 move freely if the "shells" do not overlap, i.e., if the distance between the D* "atoms" is r > r\ + r2. If the "shells" overlap, a purely Coulomb repulsion of the D* "atoms" is observed. The potential deuterons interaction energy in this approximation is equal to v ^ \e2/r-Es V{r) = < [0 2

ifr ri + r 2 ,

2

where Es = e /(r\ + r2) = mec re/(ri + r2) is the screening energy, r e = 2.82 x 10~ 13 cm is the classical radius of an electron. By integration, we obtain P(E) = exp (-993.09 eV 1 / 2 /v / - B + Es

585

Since at any energy E contributing to A there holds a condition E
=C

d n / dr2/(ri|Z)/(r2|m)W(ri+r-2), o o

where C = (nS0/2)(2/fiE)1/2, W{n+r2) = exp (-1.39y/(n + r 2 ) / r e ) . Taking into account the probabilistic sense of f{r\l), the reaction rates A(7, m), A(a) could be approximately calculated by the formulas N(l) N(m)

» » ) ^ E E »>."»+ r<»>), A(fl) = c

^^)%o/(ri+rj)'

where r ^ , i = 1, 2, 3 , . . . , N{1) are random implementations of the D* "atom" size with I collisions of electrons; 7-j, i — 1, 2, 3 , . . . , N* denotes the complete set of implementations. Let every octahedral site contain a deuterium atom. Then the deuterium concentration n = 6.8 x 1022 cm" 3 ; at T = 350 K, C factor = 1.2 x 10 10 s" 1 . The calculation results are given below. Table 1 presents the sizes of 10 D* "atoms", for which r < 2 x lO^ 1 1 cm. It follows from Table 1 that the "orbits" are usually rather prolate: r m ; n >C r, therefore making use of the r value as the size of the "atom" will result in the lower-bound estimate of A. By way of illustration, Table 2 present the number of events with the size r and the number of collisions I from the different ranges; AN* is the total number of events with I from these ranges. Table 1. Sizes of D* "atoms" at the apogee of r and at the perigee r m j n in units of 1 0 - 1 1 cm. I is the number of electron collisions with D* I r ^min

88 0.87 0.22

83 1.17 0.41

84 1.27 0.19

82 1.38 0.88

25 1.64 0.12

89 1.69 0.11

79 1.78 0.08

56 1.81 0.19

98 1.82 0.88

51 1.99 0.38

Figure 1 shows the functions X(l,l) and A(a). Averaging A (a) over a < Zmax, equivalent to the time averaging yields A f» 2 x 1 0 _ 4 s ^ 1 , which is 106 times greater than the value obtained in Refs. 1 and 2 on the basis of the dynamic model of electron orbital deformation (EODD). Taking into account that A(a) somewhat increases with the increase in a, the obtained average A should be treated as a lower-bound estimate. The contribution of 370 events presented in Table 2 to the

586 Table 2. Ranges of I

1-20 21-40 41-60 61-80 81-100

AN*

177731 114983 66531 39042 22461

Number of events with r and I from the indicated ranges Ranges of size r of the D* "atom" in units of 1 0 ~ n cm 0.5-1

1-1.5

1.5-2

2-2.5

2.5-3

3-3.5

3.5-4

4-4.5

4.5-5

0 0 0 0 1

0 0 0 0 3

0 1 2 1 2

0 5 10 3 2

2 4 9 7 2

4 14 16 13 3

7 19 23 17 8

2 25 25 10 11

0 43 36 22 18

obtained value of A is 99%, including the contribution of 10 events from Table 1 amounting to about 80 %. The application of classical mechanics usually provokes objections because classical mechanics enables one to put a shielding charge at any point and impart it any initial velocity (e.g., zero velocity). We deem it therefore important to emphasize that the equiprobable initial conditions we employed correspond to the real-life situation. In addition, the applied approach, which could be called the Bohr approach, is not a purely classical one, since the radiation has been "turned off". Quantummechanical models allowing for elastic processes only give a sufficiently accurate description of real physical processes for a very wide range of phenomena. It should be noted that from the quantum-mechanical viewpoint, D* is not a kind of a hypothetical atomic state with energies lower than that of the ground state. D* should be treated as an unsteady structure within many-particle nonradiating system.

1E+0 i

1E-1 1E-2 r

1E-5

1E-7

_

1E-8 1E-9 1E-10

^P ¥ J ! «

xr'

1E-6

-

I

-/

,A

1E-3 1E-4

/'

'•

1 \'=:

HP

'

r /

h

0

i

20

40

60

i

i

80

100

/, a

Figure 1.

Reaction rate. Dashed line denotes X(l,l)\ solid line designates A(a).

587

References 1. V. A. Kirkinskii and Yu.A. Novikov. Theoretical Modelling of Cold Fusion (Novosibirsk State University, Novosibirsk, 2002), p. 105. 2. V. A. Kirkinskii and Yu.A. Novikov, Europhys Lett 67, 362 (2004). 3. R. H. Fowler and E. A. Guggenheim Statistical Thermodynamics (Cambridge University Press, Cambridge, 1939).

This page is intentionally left blank

Author Index

A

F Falcioni, F., 377 Fauvarque, J.-F., 80 Fiore, R., 145 Fisher, J. C , 516 Fontana, F., 377 Frisone, F., 494 Fujii, M., 133 Fukuhara, M., 547 Furuyama, Y., 272

Adamenko, S. V., 356 Almaviva, S., 351 Amini, F., 163 Andreassi, V., 377 Aoki, Y., 253 Apicella, M., 117, 264 Arata, Y., 44

B

G

Ban, M., 411, 555 Bertolotti, M., 55

Gamberale, L., 377 Garbelli, D., 377 Gareev, F. A., 504 Gavritenkov, D. V., 231 Giacinti, O., 377 Goncharov, A. I., 582

c Cai, N. N., 482 Cao, D. X., 482 Capobianco, L., 117, 145 Castagna, E., 55, 117, 145, 156, 264, 351 Castano, C. H., 367 Celani, F., 289, 377, 404 Celia, E., 377 Chaudhary, I., 527 Chubb, S. R., 430 Chubb, T. A., 473 Clauzon, P. P., 80

H Hagelstein, P. L., Haque, M., 314 Higashizawa, M., Hubler, G., 264

441, 527 196

I Iizumi, K., 133 Ishikawa, T., 178 Itagaki, M., 188, 196 Itoh, T., 178 Iwai, H., 272 Iwamura, K., 178, 289

D D'Agostaro, G., 377 D'Aulerio, L., 117, 145 Dardik, I., 55 Dash, J., 86, 140 Del Prete, P. R., 145 Desyatov, A. V., 97 Di Stefano, V., 377, 404

K Kamiya, N., 133 Karabut, A. B., 214, 344

589

590

Kim, Y. E., 462 Kirkinskii, V. A., 542, 582 Kitamura, A., 272 Koldamasov, A. I., 97 Kornilova, A. A., 97, 206 Kornilova, J., 206 Kowalski, L., 171 Kuribayashi, S., 178 Kurihara, S., 196

L Lalleve, G. J.-M., 80 Lesin, S., 55 Li, X. Z., 26, 75, 278, 482 Lipson, A., 314 Lipson, A. G., 293, 304, 325, 336, 367 Little, S., 171 Liu, B., 75, 278, 482 Luce, G., 171 Lyakhov, B. F., 293, 304, 367

M Mancini, A., 377 Marchesini, M., 377 Marini, P., 377, 404 Marolo, T., 351 Mastromatteo, U., 377 Mazzitelli, G., 117 McConnell, D. B., 97 McKubre, M., 55, 117, 145, 264 McKubre, M. C. H., 392 Miley, G. H., 34, 293, 314, 325, 336, 367 Mitin, A. V., 367 Mitsushima, S., 133 Miura, H., 536 Mizuno, T., 65, 253 Momota, H., 325 Montereali, R. M., 351 Moretti, S., 55

Mueller, N., 75, 278 Muromtsev, V., 571

N Nakamura, M., 377 Narita, S., 188, 196, 284 Nishio, R., 272 Novaro, E., 377 Novikov, Y. A., 542 Numata, H., 411

o Odashima, T., 196, 284 Oehre, H., 75, 278 Ohmori, T., 253, 284 Ota, K.-L, 133

P Paoloni, S., 156 Percel, I., 314 Platonov, V., 571 Purchi, E., 377

Q Quercia, P.,

377

R Righi, E., 377 Rodionov, B., 421 Romer, M., 314 Rosada, A., 117, 264 Roussetski, A. S., 293, 304, 336

s Sakano, M., 178 Santoro, E., 117, 264 Sarto, F., 55, 117, 156, 264, 351 Satoh, R., 272 Saunin, E. I., 293, 304, 336

591

Savvatimova, L, 421, 571 Savvatimova, I. B., 231 Sawada, H., 196 Schoch, P., 75, 278 Shimadu, S., 284 Shrestha, P. J., 34 Sibilia, C , 55, 117, 156, 264, 351 Slaughter, R., 171 Sona, P. G., 377 Spallone, A., 377, 404 Storms, E., 108

T Takahashi, A., 1, 289, 454 Takahashi, D., 188 Taniguchi, S., 188, 196, 284 Taniike, A., 272 Tanzella, F., 55, 117, 145, 264 Tanzella, F. L., 392 Tashirev, A. B., 206 Terada, Y., 178 Teshima, N., 284 Todarello, F., 377 Toriyabe, Y., 65, 253 Trenta, G., 377 Tsivadze, A. Y., 367 Tsuchiya, K.-L, 521

U Ushirozawa, T.,

196

V Vincenti, M. A., 351 Violante, V., 55, 117, 145, 156, 264, 351 Vysotskii, V. I., 97, 206, 356

w Wagatsuma, Y., 188 Wang, Q., 86, 140 Wei, Q. M., 75, 278, 482

Y Yabuuchi, N., 564 Yamada, H., 188, 196, 284 Yamamoto, H., 577 Yamazaki, N., 178 Yang, H. I., 97 Yang, Y., 314

z Zhang, W.-S., 86 Zhang, Y.-C., 44 Zheng, S. X., 482 Zhidkova, I. E., 504 Zilov, T., 55 Zubarev, A. L., 462

Recent progress in the emerging field of condensed matter nuclear science (CMNS) is presented as a combination of basic nuclear science, energy, nanomaterials science, electrochemistry and nuclear physics. Key and selected papers from an important conference in this exciting area provide the latest advances in CMNS studies. Current results from cold fusion and condensed matter nuclear science are included.

clondensed mlatter nluclear science

World Scientific www.worldscientific.com 6190 he

ISBN 981-256-901-4