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Handbook of Nuclear Chemistry Frank Ro¨sch (Eds.) Handbook of Nuclear Chemistry Second Edition With 907 Figures and 312 Tables Attila Ve´rtes, Sa´ndor Nagy, Zolta´n Klencsa´r, Rezso˝ G. Lovas, Zolta´n Klencsa´r, Dr. Chemical Research Center Hungarian Academy of Sciences Pusztaszeri u´t 59-67 Budapest, 1025 Hungary 55128 Mainz Germany IS 2 k iev co pl e ISBN 978-1-4419-0719-6 e- DOI 10.1007/978-1-4419-0720-2 Print and electronic bundle ISBN: 978-1-4419-07 Springer Dordrecht Heidelberg London New Yor Library of Congress Control Number: 2010935459 � Springer ScienceþBusiness Media B.V. 2011 No part of this workmay be reproduced, stored in a retr electronic, mechanical, photocopying, microfilming, re the Publisher, with the exception of any material sup executed on a computer system, for exclusive use by th Printed on acid-free paper Springer is part of Springer ScienceþBusiness Media (ww BN 978-1-4419-0720-2 1-9 al system, or transmitted in any form or by any means, rding or otherwise, without written permission from ied specifically for the purpose of being entered and purchaser of the work. Budapest, 1518 Hungary Editors Attila Ve´rtes, Professor Emeritus Institute of Chemistry Eo¨tvo¨s Lora´nd University P.O. Box 32 Budapest, 1518 Hungary Sa´ndor Nagy, Professor Institute of Chemistry Eo¨tvo¨s Lora´nd University P.O. Box 32 Rezso˝ G. Lovas, Professor Institute of Nuclear Research (ATOMKI) Hungarian Academy of Sciences P.O. Box 51 Debrecen, 4001 Hungary Frank Ro¨sch, Professor Institute of Nuclear Chemistry Fritz-Strassmann-Weg 2 Johannes Gutenberg University Mainz w.springer.com) An important part of all this is widespread understanding of a field that is novel, but basically not particularly difficult to understand. This major five-volume publication is exceedingly useful for further research, understanding and application of the chemical aspect of nuclear science. Foreword The Future of Nuclear Energy and Research New ideas are hard to accept; popular mistrust and opposition often hinder the exploration and application of new sciences and technologies. We have to look only at the work and struggle of Galileo, Newton, and Einstein, among many others, to realize what obstacles there were in their paths. There can be no question that nuclear energy will become more important in the future in spite of the fact that there is general opposition toward the use of this form of energy. Conventional energy sources will soon become less available. Oil and gas are becoming more expensive and no great reserves appear to be available. Coal supplies are likely to last longer but I expect it to become more expensive even within this century. The other sources, like hydroelectricity, solar energy and geothermal energy will be in many cases important, but they will remain local and limited. I firmly expect that the source that will become of lasting and general importance for the world is nuclear energy. As we see it at the present, uranium will remain a satisfactory energy source for the third millennium. Energy from thorium (by transformation into uranium 233) is likely to remain available even longer. One obstacle appears to remain: fear of radioactivity. My main point is that the fear is not justified. Consider the damage in the last few decades due to the use of nuclear reactors, divided by the amount of available energy produced. Two well-known examples of such damage are at ThreeMile Island in the United States in 1979, and evenmore at Chernobyl in the Soviet Union in 1986. Both of these were caused by human error. At ThreeMile Island, the economic damage was great, but there was hardly any effect on health. In Chernobyl, the effect on human health was considerable, but still small compared to the publicity it generated. The main problem in nuclear energy is the fight against hysteria. I hope and believe that ways will be found to overcome such hysteria. I want to make just one recommendation. In developing nuclear energy for the future, primary emphasis should be given to one problem with double aspect. One aspect is safety of future nuclear reactors; the other is the public understanding of this safety. This is the field in which innovations are most necessary. For this, we need three things: one is careful planning and operation of nuclear energy production; other improvements in nuclear energy production will be made, but these are unimportant compared to the needed improvements in safety. The second point is the review of past damage in all phases connected with nuclear energy. The third andmost important part is the work for and execution of plans for the use of nuclear energy for the whole world, advanced and underdeveloped, with primary emphasis on safety and objective reporting. E. Teller{ {Editors’ note: The above sentences were dictated by Professor Edward Teller to his secretary in March 2003. The text was to be the Foreword of the first edition of the Handbook of Nuclear Chemistry (HNC) published in November 2003. Professor Teller died on September 9, 2003, just a fewmonths before the bookwas released.We still deeply regret that we lost the opportunity to present him with a complimentary copy of HNC as a token of our gratitude for his support. However, his words have not lost their timeliness over the years. We have decided to have them published unchanged thus expressing our respect for his memory. vi Foreword difficulties and hazards as well as regulating them (within reason) is necessary. Finding solutions to overcome them, however, is essential. (Olah 1998, pp 40–54) The editors of this handbook hope that this work contributes to the activity of a research field that helps us to learn more and more about nature and will remain dynamic for a long Preface In the twentieth century, 57 Nobel Prizes honored the chemical and physical results achieved by theoreticians and experimenters who can be rightly called nuclear scientists. This number alone proves that nuclear science was recognized as one of the most powerful engines pushing science to new heights in the past century, often referred to as the Nuclear Age. It is interesting to mention that until the middle of the twentieth century, the ratio of Nobel Prizes that honored nuclear results was 2:1 for physics and chemistry. However, after 1950, only two chemical results were awarded by this prize: E. M. McMillan and G. T. Seaborg for the production of 93Np and 94Pu in 1951, and W. F. Libby for working out the 14C age determi- nation in archeology and geophysics in 1960. R.S. Yalow was honored by the Nobel Prize in 1977 for a medical result. She developed the radioimmunoassays of peptide hormones. All other Nobel Prizes for nuclear results were awarded in the field of physics. The Nobel Prizes achieved by nuclear scientists are listed in >Table 1. A correlation between the period of the research work and the date of the award is demonstrated in > Fig. 1. One needs little imagination to foretell that the flagships of science will be informatics and biology in the twenty-first century. Nevertheless, there are many signs making us firmly believe that nuclear science will remain important in the future as well, in spite of the antinuclear sentiments caused by the unfortunate Chernobyl accident in 1986. Radiopharmaceutical chemistry is stimulating biomedical research and nuclear medicine (diagnosis and therapy). The development of particle physics keeps its dynamism as demonstrated by the Nobel Prizes awarded in this century (2002, 2004, and 2008.) There are well-supported opinions that nuclear fission and fusion will be among the important sources of energy in the twenty-first century. We cite George A. Olah who was awarded the Nobel Prize for his contributions to carbocation chemistry in 1994. He wrote (Olah GA (1998) Oil and hydrocarbons in the 21st century. In: Barkan P (ed) Chemical research 2000 and beyond. Amer Chem Soc, Washington, DC/OUP, New York, pp 40–54): " Generating energy by burning non-renewable fossil fuels including oil, gas and coal is feasible only for the relatively short future and even so, faces serious environmental problems. The advent of the atomic age opened up a wonderful new possibility, but also created dangers and concerns of safety. I feel that it is tragic that the latter considerations practically brought further development of atomic energy to a stand still at least in most of the Western world. Whether we like it or not we have in the long run no alternative but to rely increasingly on clean atomic energy, but we must solve safety problems including those of disposal and storage of radioactive waste-products. Pointing out time. . T a b le 1 T h e re su lt s o f n u cl e a r sc ie n ti st s h o n o re d b y N o b e l P ri ze s T h e h o n o re d re su lt s a s p h ra se d b y th e N o b e l C o m m it te e T h e p e ri o d o f th e a ct iv it y re su lt in g th e N o b e l P ri ze T h e n a m e (s ) o f th e a w a rd e d p e rs o n (s ) T h e y e a r o f d is ti n ct io n In re co g n it io n o f th e e xt ra o rd in ar y se rv ic e s h e h as re n d e re d b y h is d is co ve ry o f sp o n ta n e o u s ra d io ac ti vi ty 1 8 9 6 H .A .B e cq u e re l 1 9 0 3 (p h ys ic s) In re co g n it io n o f th e e xt ra o rd in ar y se rv ic e s th e y h av e re n d e re d b y th e ir jo in t re se ar ch e s o n th e ra d ia ti o n p h e n o m e n a d is co ve re d b y P ro fe ss o r H e n ri B e cq u e re l 1 8 9 7 – 1 9 0 3 M .C u ri e P .C u ri e In re co g n it io n o f h e r se rv ic e s to th e ad va n ce m e n t o f ch e m is tr y b y th e d is co ve ry o f th e e le m e n ts ra d iu m an d p o lo n iu m ,b y th e is o la ti o n o f ra d iu m an d th e st u d y o f th e n at u re an d co m p o u n d s o f th is re m ar ka b le e le m e n t 1 8 9 8 M .C u ri e 1 9 1 1 (c h e m is tr y) Fo r h is in ve st ig at io n s in to th e d is in te g ra ti o n o f th e e le m e n ts ,a n d th e ch e m is tr y o f ra d io ac ti ve su b st an ce s 1 8 9 8 – 1 9 0 0 E. R u th e rf o rd 1 9 0 8 (c h e m is tr y) In re co g n it io n o f th e se rv ic e s h e re n d e re d to th e ad va n ce m e n t o f p h ys ic s b y h is d is co ve ry o f e n e rg y q u an ta 1 9 0 1 M .P la n ck 1 9 1 8 (p h ys ic s) Fo r h is se rv ic e s to th e o re ti ca lp h ys ic s, an d e sp e ci al ly fo r h is d is co ve ry o f th e la w o f th e p h o to e le ct ri c e ff e ct 1 9 0 5 A .E in st e in 1 9 2 1 (p h ys ic s) Fo r h is w o rk o n th e e le m e n ta ry ch ar g e o f e le ct ri ci ty an d o n th e p h o to e le ct ri c e ff e ct 1 9 1 0 – 1 9 1 4 R .A .M ill ik an 1 9 2 3 (p h ys ic s) Fo r h is m e th o d o f m ak in g th e p at h s o f e le ct ri ca lly ch ar g e d p ar ti cl e s vi si b le b y co n d e n sa ti o n o f va p o r 1 9 1 2 C .T .R .W ils o n 1 9 2 7 (p h ys ic s) Fo r h is d is co ve ry o f co sm ic ra d ia ti o n 1 9 1 2 V .F .H e ss 1 9 3 6 (p h ys ic s) Fo r h is w o rk o n th e u se o f is o to p e s as tr ac e rs in th e st u d y o f ch e m ic al p ro ce ss e s 1 9 1 3 – 1 9 3 5 G .H e ve sy 1 9 4 3 (c h e m is tr y) Fo r h is co n tr ib u ti o n s to o u r kn o w le d g e o f th e ch e m is tr y o f ra d io ac ti ve su b st an ce s, an d h is in ve st ig at io n s in to th e o ri g in an d n at u re o f is o to p e s 1 9 1 3 – 1 9 1 6 F. So d d y 1 9 2 1 (c h e m is tr y) Fo r h is d is co ve ry o f th e e ff e ct n am e d af te r h im 1 9 2 3 A .H .C o m p to n 1 9 2 7 (p h ys ic s) Fo r th e d is co ve ry o f th e Ex cl u si o n P ri n ci p le ,a ls o ca lle d th e P au li P ri n ci p le 1 9 2 5 W .P au li 1 9 4 5 (p h ys ic s) Fo r th e d is co ve ry o f n e w p ro d u ct iv e fo rm s o f at o m ic th e o ry 1 9 2 6 E. Sc h ro¨ d in g e r 1 9 3 3 (p h ys ic s) P .A .M .D ir ac viii Preface Fo r th e in ve n ti o n an d d e ve lo p m e n t o f th e cy cl o tr o n an d fo r re su lt s o b ta in e d w it h it , e sp e ci al ly w it h re g ar d to ar ti fi ci al ra d io ac ti ve e le m e n ts 1 9 2 9 – 1 9 3 2 E. O .L aw re n ce 1 9 3 9 (p h ys ic s) Fo r h is re so n an ce m e th o d fo r re co rd in g th e m ag n e ti c p ro p e rt ie s fo r at o m ic n u cl e i 1 9 3 0 – 1 9 3 9 I. I. R ab i 1 9 4 4 (p h ys ic s) Fo r th e co in ci d e n ce m e th o d an d h is d is co ve ri e s m ad e th e re w it h 1 9 3 0 – 1 9 4 0 W .B o th e 1 9 5 4 (p h ys ic s) Fo r h is d e ve lo p m e n t o f th e W ils o n cl o u d ch am b e r m e th o d ,a n d h is d is co ve ri e s th e re w it h in th e fi e ld o f n u cl e ar p h ys ic s an d co sm ic ra d ia ti o n 1 9 3 1 – 1 9 3 3 P .M .S .B la ck e tt 1 9 4 8 (p h ys ic s) Fo r th e d is co ve ry o f th e n e u tr o n 1 9 3 2 J. C h ad w ic k 1 9 3 5 (p h ys ic s) Fo r h is d is co ve ry o f th e p o si tr o n 1 9 3 2 C .D .A n d e rs o n 1 9 3 6 (p h ys ic s) Fo r th e ir p io n e e ri n g w o rk o n th e tr an sm u ta ti o n o f at o m ic n u cl e ib y ar ti fi ci al ly ac ce le ra te d at o m ic p ar ti cl e s 1 9 3 2 J. D .C o ck cr o ft 1 9 5 1 (p h ys ic s) E. T .S .W al to n Fo r h is co n tr ib u ti o n s to th e d e ve lo p m e n t o f th e m o le cu la r ra y m e th o d an d h is d is co ve ry o f th e m ag n e ti c m o m e n t o f th e p ro to n 1 9 3 3 O .S te rn 1 9 4 3 (p h ys ic s) Fo r h is co n tr ib u ti o n s to th e th e o ry o f th e at o m ic n u cl e u s an d th e e le m e n ta ry p ar ti cl e s, p ar ti cu la rl y th ro u g h th e d is co ve ry an d ap p lic at io n o f fu n d am e n ta l sy m m e tr y p ri n ci p le s 1 9 3 3 – 1 9 3 7 E. P .W ig n e r 1 9 6 3 (p h ys ic s) In re co g n it io n o f th e ir sy n th e si s o f n e w ra d io ac ti ve e le m e n ts 1 9 3 4 F. J. C u ri e 1 9 3 5 (c h e m is tr y) I. C u ri e Fo r th e d is co ve ry an d th e in te rp re ta ti o n o f th e C h e re n ko v e ff e ct 1 9 3 4 – 1 9 3 7 P .A .C h e re n ko v 1 9 5 8 (p h ys ic s) I. M .F ra n k I. E. T am m Fo r h is d e m o n st ra ti o n s o f th e e xi st e n ce o f n e w ra d io ac ti ve e le m e n ts p ro d u ce d b y n e u tr o n ir ra d ia ti o n ,a n d fo r h is re la te d d is co ve ry o f n u cl e ar re ac ti o n s b ro u g h t ab o u t b y sl o w n e u tr o n s 1 9 3 4 – 1 9 3 6 E. Fe rm i 1 9 3 8 (p h ys ic s) Fo r h is p re d ic ti o n o f th e e xi st e n ce o f m e so n s o n th e b as is o f th e o re ti ca lw o rk o n n u cl e ar fo rc e s 1 9 3 5 H .Y u ka w a 1 9 4 9 (p h ys ic s) Fo r h is co n tr ib u ti o n s to th e th e o ry o f n u cl e ar re ac ti o n s, e sp e ci al ly h is d is co ve ri e s co n ce rn in g th e e n e rg y p ro d u ct io n in st ar s 1 9 3 8 H .A .B e th e 1 9 6 7 (p h ys ic s) Fo r h is d is co ve ry o f th e fi ss io n o f h e av y n u cl e i 1 9 3 8 O .H ah n 1 9 4 4 (c h e m is tr y) Preface ix . T a b le 1 (C o n ti n u e d ) T h e h o n o re d re su lt s a s p h ra se d b y th e N o b e l C o m m it te e T h e p e ri o d o f th e a ct iv it y re su lt in g th e N o b e l P ri ze T h e n a m e (s ) o f th e a w a rd e d p e rs o n (s ) T h e y e a r o f d is ti n ct io n Fo r th e ir d is co ve ri e s in th e ch e m is tr y o f th e tr an su ra n iu m e le m e n ts 1 9 4 0 E. M .M cM ill an 1 9 5 1 (c h e m is tr y) G .T .S e ab o rg Fo r h is m e th o d to u se ca rb o n -1 4 fo r ag e d e te rm in at io n in ar ch ae o lo g y, g e o lo g y, g e o p h ys ic s, an d o th e r b ra n ch e s o f sc ie n ce 1 9 4 6 W .F .L ib b y 1 9 6 0 (c h e m is tr y) Fo r th e ir d e ve lo p m e n t o f n e w m e th o d s fo r n u cl e ar m ag n e ti c p re ci si o n m e as u re m e n ts an d d is co ve ri e s in co n n e ct io n th e re w it h 1 9 4 6 – 1 9 4 8 F. B lo ch 1 9 5 2 (p h ys ic s) E. M .P u rc e ll Fo r th e ir fu n d am e n ta lw o rk in q u an tu m e le ct ro d yn am ic s, w it h d e e p -p lo u g h in g co n se q u e n ce s fo r th e p h ys ic s o f e le m e n ta ry p ar ti cl e s 1 9 4 6 – 1 9 4 8 S. -I .T o m o n ag a 1 9 6 5 (p h ys ic s) J. Sc h w in g e r R .P .F e yn m an Fo r h is d e ve lo p m e n t o f th e p h o to g ra p h ic m e th o d o f st u d yi n g n u cl e ar p ro ce ss e s an d h is d is co ve ri e s re g ar d in g m e so n s m ad e w it h th is m e th o d 1 9 4 6 – 1 9 5 0 C .F .P o w e ll 1 9 5 0 (p h ys ic s) Fo r th e ir d is co ve ri e s co n ce rn in g n u cl e ar sh e ll st ru ct u re 1 9 4 8 – 1 9 5 4 O .M .G o e p p e rt - M ay e r 1 9 6 3 (p h ys ic s) J. H .D .J e n se n Fo r th e in ve n ti o n o f th e b u b b le ch am b e r 1 9 5 2 D .A .G la se r 1 9 6 0 (p h ys ic s) Fo r th e d is co ve ry o f th e co n n e ct io n b e tw e e n co lle ct iv e m o ti o n an d p ar ti cl e m o ti o n in at o m ic n u cl e ia n d th e d e ve lo p m e n t o f th e th e o ry o f th e st ru ct u re o f th e at o m ic n u cl e u s b as e d o n th is co n n e ct io n 1 9 5 3 A .N .B o h r 1 9 7 5 (p h ys ic s) B .R .M o tt e ls o n L. J. R ai n w at e r Fo r h is p io n e e ri n g st u d ie s o f e le ct ro n sc at te ri n g in at o m ic n u cl e ia n d fo r h is th e re b y ac h ie ve d d is co ve ri e s co n ce rn in g th e st ru ct u re o f th e n u cl e o n s 1 9 5 3 – 1 9 6 0 R .H o fs ta d te r 1 9 6 1 (p h ys ic s) Fo r th e d e te ct io n o f th e n e u tr in o 1 9 5 3 – 1 9 6 0 F. R e in e s 1 9 9 5 (p h ys ic s) Fo r h is co n tr ib u ti o n to th e d e ve lo p m e n t o f h ig h -r e so lu ti o n e le ct ro n sp e ct ro sc o p y 1 9 5 4 – 1 9 5 8 K .M .S ie g b ah n 1 9 8 1 (p h ys ic s) Fo r th e ir d is co ve ry o f th e an ti p ro to n 1 9 5 5 E. G .S e g re 1 9 5 9 (p h ys ic s) O .C h e m b e rl ai n x Preface Fo r h is d e ci si ve co n tr ib u ti o n s to e le m e n ta ry p ar ti cl e p h ys ic s, in p ar ti cu la r, th e d is co ve ry o f a la rg e n u m b e r o f re so n an ce st at e s, m ad e p o ss ib le th ro u g h h is d e ve lo p m e n t o f th e te ch n iq u e o f u si n g h yd ro g e n b u b b le ch am b e r an d d at a an al ys is 1 9 5 5 – 1 9 5 7 L. W .A lv ar e z 1 9 6 8 (p h ys ic s) Fo r th e d e ve lo p m e n t o f n e u tr o n sp e ct ro sc o p y 1 9 5 5 – 1 9 6 0 B .N .B ro ck h o u se 1 9 9 4 (p h ys ic s) C .G .S h u ll Fo r p io n e e ri n g co n tr ib u ti o n s to as tr o p h ys ic s, in p ar ti cu la r, fo r th e d e te ct io n o f co sm ic n e u tr in o s 1 9 5 5 – 1 9 7 2 R .D av is 2 0 0 2 (p h ys ic s) M .K o sh ib a Fo r th e ir p e n e tr at in g in ve st ig at io n o f th e so -c al le d p ar it y la w s, w h ic h h as le d to im p o rt an t d is co ve ri e s re g ar d in g th e e le m e n ta ry p ar ti cl e s 1 9 5 6 T .D .L e e 1 9 5 7 (p h ys ic s) C .N .Y an g Fo r h is th e o re ti ca ls tu d ie s o f th e p h ys ic al p ro ce ss e s o f im p o rt an ce to th e st ru ct u re an d e vo lu ti o n o f th e st ar s 1 9 6 2 – 1 9 7 1 S. C h an d ra se kh ar 1 9 8 3 (p h ys ic s) Fo r h is th e o re ti ca la n d e xp e ri m e n ta ls tu d ie s o f th e n u cl e ar re ac ti o n s o f im p o rt an ce in th e fo rm at io n o f th e ch e m ic al e le m e n ts in th e u n iv e rs e 1 9 5 6 – 1 9 6 5 W .A .F o w le r Fo r h is re se ar ch e s co n ce rn in g th e re so n an ce ab so rp ti o n o fg am m a ra d ia ti o n an d h is d is co ve ry in th is co n n e ct io n o f th e e ff e ct th at b e ar s h is n am e 1 9 5 8 R .M o¨ ss b au e r 1 9 6 1 (p h ys ic s) Fo r th e ir co n tr ib u ti o n s to th e th e o ry o f th e u n if ie d w e ak an d e le ct ro m ag n e ti c in te ra ct io n b e tw e e n e le m e n ta ry p ar ti cl e s, in cl u d in g ,i n te r al ia ,t h e p re d ic ti o n o f th e w e ak n e u tr al cu rr e n t 1 9 5 8 – 1 9 7 0 S. L. G la sh o w 1 9 7 9 (p h ys ic s) A .S al am S. W e in b e rg Fo r th e d e ve lo p m e n t o f ra d io im m u n o as sa ys o f p e p ti d e h o rm o n e s 1 9 5 9 R .S .Y al o w 1 9 7 7 (m e d ic in e ) Fo r h is co n tr ib u ti o n s an d d is co ve ri e s co n ce rn in g th e cl as si fi ca ti o n o f e le m e n ta ry p ar ti cl e s an d th e ir in te ra ct io n s 1 9 6 0 – 1 9 6 5 M .G e ll- M an n 1 9 6 9 (p h ys ic s) Fo r th e d is co ve ry o f th e m e ch an is m o f sp o n ta n e o u s b ro ke n sy m m e tr y in su b at o m ic p h ys ic s 1 9 6 0 – 1 9 7 3 Y .N am b u 2 0 0 8 (p h ys ic s) Fo r p io n e e ri n g co n tr ib u ti o n s to as tr o p h ys ic s, w h ic h h av e le d to th e d is co ve ry o f co sm ic X -r ay so u rc e s 1 9 6 0 – 1 9 8 0 R .G ia cc o n i 2 0 0 2 (p h ys ic s) Preface xi . T a b le 1 (C o n ti n u e d ) T h e h o n o re d re su lt s a s p h ra se d b y th e N o b e l C o m m it te e T h e p e ri o d o f th e a ct iv it y re su lt in g th e N o b e l P ri ze T h e n a m e (s ) o f th e a w a rd e d p e rs o n (s ) T h e y e a r o f d is ti n ct io n Fo r th e n e u tr in o b e am m e th o d an d th e d e m o n st ra ti o n o f th e d o u b le t st ru ct u re o f th e le p to n s th ro u g h th e d is co ve ry o f th e m u o n n e u tr in o 1 9 6 3 L. Le d e rm an 1 9 8 8 (p h ys ic s) M .S ch w ar tz J. St e in b e rg e r Fo r th e d is co ve ry o f vi o la ti o n s o f fu n d am e n ta ls ym m e tr y p ri n ci p le s in th e d e ca y o f n e u tr al K -m e so n s 1 9 6 4 J. W .C ro n in 1 9 8 0 (p h ys ic s) V .L .F it ch Fo r th e ir p io n e e ri n g in ve st ig at io n s co n ce rn in g d e e p in e la st ic sc at te ri n g o fe le ct ro n s o n p ro to n s an d b o u n d n e u tr o n s, w h ic h h av e b e e n o f e ss e n ti al im p o rt an ce fo r th e d e ve lo p m e n t o f th e q u ar k m o d e li n p ar ti cl e p h ys ic s 1 9 6 8 J. I. Fr ie d m an 1 9 9 0 (p h ys ic s) H .W .K e n d al l R .E .T ay lo r Fo r h is in ve n ti o n an d d e ve lo p m e n t o f p ar ti cl e d e te ct o rs ,i n p ar ti cu la r, th e m u lt iw ir e p ro p o rt io n al ch am b e r 1 9 6 8 G .C h ar p ak 1 9 9 2 (p h ys ic s) Fo r th e d is co ve ry o ft h e o ri g in o ft h e b ro ke n sy m m e tr y, w h ic h p re d ic ts th e e xi st e n ce o f at le as t th re e fa m ili e s o f q u ar ks in n at u re 1 9 7 0 – 1 9 7 3 M .K o b ay as h i, 2 0 0 8 (p h ys ic s) T .M as ka w a Fo r e lu ci d at in g th e q u an tu m st ru ct u re o f e le ct ro w e ak in te ra ct io n s in p h ys ic s 1 9 7 2 M .J .G .V e lt m an 1 9 9 9 (p h ys ic s) G .’ t H o o ft Fo r h is th e o ry fo r cr it ic al p h e n o m e n a in co n n e ct io n w it h p h as e tr an si ti o n s 1 9 7 2 K .G .W ils o n 1 9 8 2 (p h ys ic s) Fo r th e d is co ve ry o f as ym p to ti c fr e e d o m in th e th e o ry o f th e st ro n g in te ra ct io n 1 9 7 3 – 1 9 7 4 D .J .G ro ss 2 0 0 4 (p h ys ic s) H .D .P o lit ze r F. W ilc ze k Fo r th e ir p io n e e ri n g w o rk in th e d is co ve ry o f a h e av y e le m e n ta ry p ar ti cl e o f a n e w ki n d 1 9 7 4 B .R ic h te r 1 9 7 6 (p h ys ic s) S. C .C .T in g Fo r th e d is co ve ry o f th e ta u le p to n 1 9 7 4 M .P e rl 1 9 9 5 (p h ys ic s) Fo r th e ir d e ci si ve co n tr ib u ti o n s to th e la rg e p ro je ct th at le d to th e d is co ve ry o f th e fi e ld p ar ti cl e s W an d Z ,c o m m u n ic at o rs o f w e ak in te ra ct io n 1 9 8 3 C .R u b b ia 1 9 8 4 (p h ys ic s) S. va n d e r M e e r xii Preface xiii . Fig. 1 A presentation of the time passed between the discoveries and Nobel Prizes related to the development of nuclear science and subatomic concepts (Nagy S (2007) Radiochemistry and nuclear chemistry. In: Encyclopedia of Life Support Systems (EOLSS), Developed under the auspices of the UNESCO. Eolss Publishers, Oxford [http://www.eolss.net]). The length of each drop-line shows the delay between award and achievement. Note that some achievements had been awarded almost promptly, whereas the longest delay was almost half a century. The drop- lines of the first few points are meaningless, as the Nobel Prize was first awarded in 1901 2010 2000 1990 2010 2000 1990 1890 1900 1910 1920 1930 1940 1950 1960 1970 1980 1990 2000 Preface The chapter Nuclear and Radiochemistry – the First 100 Years, dealing with the history of nuclear chemistry, was updated by Professors Friedlander andHerrmann in the Fall of 2008 and in the Spring of 2009. Alas, it was submitted for the 2nd edition by ProfessorHerrmann alone because Professor Friedlander died on September 6, 2009. Gerhart Friedlander was born on July 28, 1916, in Munich. He was a veteran of the Manhattan Project and a pioneer of nuclear chemistry who later exploited the first particle accelerators to domajor research as head of the chemistry department at Brookhaven National Laboratory. Many of us, nuclear chemists, used one of Professor Friedlander’s monographs to learn the basics of this field of science (e.g., Friedlander G, Kennedy JW, Macias ES, Miller JM (1981) Nuclear and radiochemistry. Wiley, New York). We warmly suggest that those who wish to get a bird’s eye view of the field of nuclear science should read the chapter Nuclear and Radiochemistry – the First 100 Years. They will find it not only enjoyable as a ‘story’ but also useful as a guide to all themain areas of interest, heights, crossroads, and the paths connecting the individual spots of the landscape underneath. The editors acknowledge the valuable work of Professor Ga´bor L. Molna´r who conceptu- alized and edited all the appendixes of the first edition. He died on January 6, 2004, and he could not see and enjoy the success of his work as a part of the Handbook of Nuclear Chemistry. 1980 1970 1960 1950 1940 1930 1920 1910 1900 1980 1970 1960 1950 1940 1930 1920 1910 1900 1890 1900 1910 1920 1930 1940 1950 1960 1970 1980 1990 2000 Approximate year of achievement Ye a r o f a w a rd Field of Nobel Prize Physics Chemistry Medicine We are sure that Ga´bor L. Molna´r’s work, which is mostly integrated into the 2nd edition as well, remains an important contribution to the mission of the Handbook of Nuclear Chemistry. The 63rd General Assembly of the United Nations adopted a resolution that 2011 would be the Year of Chemistry. The motivation was that Marie Curie was awarded the Nobel Prize of Chemistry a century ago, in 1911. This prize honored results achieved in the field of radio- and nuclear chemistry. It is a great pleasure for us that the 2nd edition of the Handbook of Nuclear Chemistry can welcome the start of the Year of Chemistry. The Editors October 2010 xiv Preface the Hungarian Academy of Sciences where he chaired the Division of Radiochemistry (1993–2002). He was also a member of the International Board on the Applications of the Mo¨ssbauer Effect (IBAME; 1990–1998) and holds editorial spots on some of the top journals in the field. Editorial Board Attila Ve´rtes (Tu¨rje, 1934) is a Professor Emeritus of nuclear chemistry at Eo¨tvo¨s Lora´nd University, Budapest. He studied the scattering of beta particles for his Master’s thesis in 1958 and has been dealing with different topics of nuclear chemistry ever since (e.g., Mo¨ssbauer and positron annihilation spectroscopy). Academic career highlights in Hungary include graduating from the Technical University of Budapest (MSc), 1958; Doctor of Science, Hungarian Academy of Sciences, 1973; Corresponding Member of the Hungarian Academy of Sciences, 1993; Ordinary Member of the Hungarian Academy of Sciences, 1998. Abroad, Prof. Ve´rtes studied at Lomonosov University and became a Candidate of Science, Russian Academy of Sciences, 1965. He was a Visiting Scientist at the University of New Castle (England) and a Humboldt Fellow at the Technical University, Munich (Germany) as well as a Guest Professor at Lehigh University, Bethlehem (USA), Tokyo University (Japan) and Johannes Gutenberg University, Mainz (Germany). He has published more than 500 papers in scientific periodicals and edited/authored nine monographs. Prof. Ve´rtes is an Honorary Doctor of Glasgow Caledonian University (England, 1996). He was awarded the Sze´chenyi Prize (given by the President of the Republic of Hungary, 2001) and the Hevesy Medal (Guildford, 2004). His significant position in the community is seen in his active participation in More about him at his site: www.chem.elte.hu/departments/magkem/vertesa/vertesaeng/ index.html. xvi Editorial Board Sa´ndor Nagy (Budapest, 1949) is a committed teacher of nuclear sciences employed by the Institute of Chemistry, Eo¨tvo¨s Lora´nd University (ELTE), Budapest. He graduated from chemistry in 1972, but his formal education also includes applied mathematics. He has been working for ELTE since his graduation there with some officially approved detours in the meantime. Thus he spent 14 months at the Sinclair Laboratory of Lehigh University, Bethlehem, USA (1979–1980); another 22 months at the Chemistry Department of Drexel University, Philadelphia (1987–1989); and paid several short visits to Belgium, Canada, Cuba, Denmark, Germany, Kazakhstan, the Netherlands, Romania, and Russia. Prof. Nagy has published over 100 scientific papers and a number of books and book chapters in English and Hungarian. Between 2005 and 2007, he acted as an Honorary Theme Editor of the theme Radiochemistry and Nuclear Chemistry for EOLSS (www.eolss.net/ E6-104-toc.aspx). He is an IUPAC Fellow and a member of the Board of Associate Editors of the Journal of Radioanalytical and Nuclear Chemistry. He also won some professional/teaching awards from the Institute of Chemistry, from the Faculty of Science, from ELTE and also from theMinistry of Education of Hungary. His latest pet project is developing a Nuclear Glossary in Hungarian (inspired by Rick Firestone, one of the Authors of this Handbook) stuffed with animations and simulations provided by scientists and teachers all around the world (www. chem.elte.hu/Sandor.Nagy/NewClearGlossy/). Apart from science, a few decades ago, he also authored some award-winning books on bicycling, and translated science fiction and children’s books etc. to Hungarian. He is also an enthusiastic gardener and the proud father of five daughters. For more details, visit his site at www.chem.elte.hu/Sandor.Nagy/. Editorial Board xvii Zolta´n Klencsa´r (Kaposva´r, 1971) is a senior research fellow at the Chemical Research Center of the Hungarian Academy of Sciences, Budapest. Dr. Klencsa´r received his PhD in physics from Eo¨tvo¨s Lora´nd University in 1999. He has been working as a researcher for the Hungarian Academy of Sciences (1998–2004, 2008–) and as an assistant and associate professor for the University of Kaposva´r, Hungary (2002–2008). His main field is Mo¨ssbauer spectroscopy and its applications in physics and chemistry. He has published over 50 articles in international journals, and authored several book chapters and lecture notes in the field of physical sciences. He is also an enthusiastic computer programmer who has developed numerous applications over the past two decades. In the field of Mo¨ssbauer spectroscopy he is recognized worldwide as the author of a software package used at many laboratories for the analysis of Mo¨ssbauer spectra. For more details see: www.siaweb.hu/klencsar/ xviii Editorial Board Rezso˝ G. Lovas (Debrecen, 1946) is a Research Professor at the Institute of Nuclear Research of the Hungarian Academy of Sciences in Debrecen, Hungary. Graduated from the University of Debrecen, he has been affiliated with the Debrecen Institute throughout his career. Meanwhile, he spent sabbatical-like years at the Nuclear Physics Laboratory, Oxford, at Daresbury Laboratory, at Kernforschungszentrum Karlsruhe and medium-term visits at the University of Utrecht, at Manne Siegbahn Laboratory, Stockholm, and at Niigata University. He was Director of the Debrecen Institute from 1997 to 2007. He is a Titular Professor at the University of Debrecen (1993) and a Corresponding Member of the Hungarian Academy of Sciences (2004). Formerly, he was member of the Board of the Nuclear Physics Division of the European Physical Society and of the Editorial Board of Nuclear Physics News International. At present he is Vice-President of the Physics Section of the Academy, member of the Council of the Research Institutions of the Academy, and chairs the Working Group on Energy Strategy of the Academy. His research field is nuclear theory: reactions, clustering, cluster decay and light exotic nuclei. He is a coauthor of the monograph Structure and Reactions of Light Exotic Nuclei (2003). Editorial Board xix Frank Ro¨sch (Chemnitz, 1955) is a Professor of nuclear chemistry at Johannes Gutenberg University, Mainz, Germany. He studied chemistry at the Technical University Dresden from 1976 to 1981. His diploma work was on the Production of 211At and investigations on cationic species of Astatine and their reactions and his PhD thesis 1984 On the chemistry of At(I)-complex formations. At the Joint Institute for Nuclear Research, Dubna, Sowjet Union, Laboratory for Nuclear Problems (1984–1987) he investigated Basics and perspectives of the continuous electromigration measurement of g-emitting radionuclides in homogeneous aqueous electrolytes free of supporting materials. Back in Germany, he spent some years (1987–1991) at the Central Institute for Nuclear Research (ZfK) Rossendorf, Department of Radioactive Isotopes, turning his research activities into the application of radionuclides in life sciences. In 1988 he succeeded with his habilitation and obtained the venia legendi for radiochemistry. His research on the production and potential medical application of radionuclides con- tinued at the Institute of Nuclear Chemistry, Research Centre Ju¨lich GmbH, Germany, from 1991–1996. In 1996 he was appointed a University Professor for Nuclear Chemistry at the Institute of Nuclear Chemistry, Johannes Gutenberg-University Mainz, Germany. His current research activities are focused on the development and evaluation of PET radiopharmaceuti- cals, including radionuclide generator-based radionuclides. He was honored with scientific awards of the ZfK Rossendorf and the JINR Dubna, and received other national prices. He has published more than 200 papers in peer review journals and edited/authored various book chapters. List 9 Stochastics and Nuclear Measurements . . . . . . . . . . . . . . . . . . . . . . . . . . . . 395 10 The Standard Model of Elementary Particles . . . . . . . . . . . . . . . . . . . . . . . . 457 D. Horva´th 11 Appendixes – Reference Data to Part I . . . . . . . . . . . . . . . . . . . . . . . . . . . . 475 G. L. Molna´r . R. B. Firestone S. Nagy 7 Kinetics of Radioactive Decay . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 333 S. Nagy 8 Interaction of Radiation with Matter . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 363 D. Horva´th . A. Ve´rtes 6 Nuclear Fusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 319 G. Veres 5 Tunneling Through Triple-Humped Fission Barriers . . . . . . . . . . . . . . . . . . 281 A. Krasznahorkay 4 Nuclear Fission . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 223 J. O. Denschlag 3 Nuclear Reactions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 143 L. G. Sobotka . V. E. Viola 2 Basic Properties of the Atomic Nucleus . . . . . . . . . . . . . . . . . . . . . . . . . . . . 39 T. Fe´nyes 1 Nuclear and Radiochemistry: the First 100 Years . . . . . . . . . . . . . . . . . . . . . . 3 G. Friedlander . G. Herrmann Basics of Nuclear Science Volume 1 of Contributors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xxvii Table of Contents Volume 2 H. C. Griffin H. C. Griffin G. Jancso´ R. Bowen R. Bowen Y. Nagame M. Hirata H. Nakahara G. Mu¨nzenberg M. Gupta J. V. Kratz D. C. Hoffman D. A. Shaughnessy R. B. Firestone Volume 3 xxii Chemical Applications of Nuclear Reactions and Radiations 23 Radiation Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1265 L. Wojna´rovits 24 Hot Atom Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1333 22 Appendix to Part II – Table of Nuclides . . . . . . . . . . . . . . . . . . . . . . . . . . . 1033 21 Superheavy Elements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1005 . 20 Chemistry of Transactinides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 925 19 Production and Identification of Transactinide Elements . . . . . . . . . . . . . . . 877 . 18 Production and Chemistry of Transuranium Elements . . . . . . . . . . . . . . . . . 817 . . 17 Radioactive Dating Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 761 16 Isotopic Paleoclimatology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 727 15 Isotope Effects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 699 14 Radioelements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 689 Elements and Isotopes Formation, Transformation, Distribution 12 Origin of the Chemical Elements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 613 T. Rauscher . A. Patko´s 13 Natural Radioactive Decay Chains . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 667 Table of Contents H. K. Yoshihara . T. Sekine 27 Positron Annihilation Spectroscopies . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1461 D. Horva´th L. Pusztai 31 32 33 34 F. Adams . B. Vekemans . G. Silversmit . B. De Samber . L. Vincze H. Haba . S. Motomura . S. Kamino . S. Enomoto Z. Homonnay . Z. Klencsa´r . R. B. Firestone . Z. Re´vay . G. L. Molna´r . Volume 4 37 xxiii 38 Reactor-Produced Medical Radionuclides . . . . . . . . . . . . . . . . . . . . . . . . . 1857 Introduction to the Fourth Volume . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1855 Radiochemistry and Radiopharmaceutical Chemistry in Life Sciences J. Csikai . R. Do´czi 36 Appendixes – Reference Data to Part III . . . . . . . . . . . . . . . . . . . . . . . . . . 1793 35 Tracer Technique . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1761 Sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1737 Microscopic X-ray Fluorescence Analysis with Synchrotron Radiation E. Koltay . F. Pa´szti . A´. Z. Kiss Chemical Applications of Ion Accelerators . . . . . . . . . . . . . . . . . . . . . . . . . 1695 J. Csikai . R. Do´czi Applications of Neutron Generators . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1673 Z. Re´vay . R. M. Lindstrom . E. A. Mackey . T. Belgya Neutron-Induced Prompt Gamma Activation Analysis (PGAA) . . . . . . . . . . 1619 30 Activation Analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1553 R. Zeisler . N. Vajda . G. Kennedy . G. Lamaze . G. L. Molna´r 29 Neutron Scattering Methods in Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . 1515 28 Exotic Atoms and Muonium . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1485 K. Su¨vegh . T. Marek 25 Mo¨ssbauer Spectroscopy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1379 E. Kuzmann . Z. Homonnay . S. Nagy . K. Nomura 26 Mo¨ssbauer Excitation by Synchrotron Radiation . . . . . . . . . . . . . . . . . . . . 1447 M. Seto Table of Contents S. Mirzadeh . L. F. Mausner . M. A. Garland S. M. Qaim F. Ro¨sch . F. F. (Russ) Knapp G. Antoni . T. Kihlberg . B. La˚ngstro¨m T. L. Ross . H. J. Wester R. Alberto . U. Abram 46 Instrumentation, Separation Techniques, Environmental Issues B. Kanya´r . G. J. Ko¨teles H. C. Griffin W. L. McLaughlin . A. Miller . A. Kova´cs . K. K. Mehta S. Biri . E. Koltay . A. Valek W. A. Van Hook xxiv Table of Contents 52 Solvent Extraction and Ion Exchange in Radiochemistry . . . . . . . . . . . . . . 2403 51 Isotope Separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2369 50 Particle Accelerators . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2319 49 Dosimetry Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2287 48 Radiation Detection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2259 47 Dosimetry and Biological Effects of Ionizing Radiation . . . . . . . . . . . . . . . 2213 Volume 5 M. R. Zalutsky Radionuclide Therapy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2179 44 Radioiodination Chemistry and Radioiodinated Compounds . . . . . . . . . . . 2121 M. Eisenhut . W. Mier 45 Radiometals (non-Tc, non-Re) and Bifunctional Labeling Chemistry . . . . . 2143 M. Fani . S. Good . H. R. Maecke 43 99mTc: Labeling Chemistry and Labeled Compounds . . . . . . . . . . . . . . . . . 2073 42 18F: Labeling Chemistry and Labeled Compounds . . . . . . . . . . . . . . . . . . . 2021 41 11C: Labeling Chemistry and Labeled Compounds . . . . . . . . . . . . . . . . . . . 1977 40 Radionuclide Generators . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1935 39 Cyclotron Production of Medical Radionuclides . . . . . . . . . . . . . . . . . . . . . 1903 G. Skarnemark 53 Radiochemical Separations by Thermochromatography . . . . . . . . . . . . . . 2429 A. F. Novgorodov . F. Ro¨sch . N. A. Korolev 54 Methods of Cosmochemical Analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2459 S. Lahiri . M. Maiti 56 Nuclear Energy Production and Safety Issues J. O. Denschlag E. O. Adamov Y. Fuji-ie N. E. Kukharkin N. N. Ponomarev-Stepnoi V. A. Usov G. Veres S. Zoletnik W. Jacob 63 Inde Table of Contents xxv x . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3017 M. Zendel . D. L. Donohue . E. Kuhn . S. Deron . T. Bı´ro´ Nuclear Safeguards Verification Measurement Techniques . . . . . . . . . . . . 2893 61 Radioactive Waste Management . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2797 P. A. Baisden . C. E. Atkins-Duffin 62 Nuclear Forensic Materials and Methods . . . . . . . . . . . . . . . . . . . . . . . . . . 2837 I. D. Hutcheon . P. M. Grant . K. J. Moody 60 Technical Developments for Harnessing Controlled Fusion . . . . . . . . . . . . 2759 . . 59 Nuclear Power Sources for Space Systems . . . . . . . . . . . . . . . . . . . . . . . . . 2731 . . 58 Developments and Tendencies in Fission Reactor Concepts . . . . . . . . . . . 2663 . 57 Technical Application of Nuclear Fission . . . . . . . . . . . . . . . . . . . . . . . . . . 2615 Volume 6 R. B. Firestone . G. L. Molna´r Appendix – Reference Data to Part V . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2565 55 Environmental Radiation Protection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2503 Y. Maeda . S. Osaki . A. Vincze o Gunnar Antoni Uppsala University Patricia A. Baisden Sa´ndor Biri Robert Bowen Uppsala Imanet AB P.O. Box 967 Uppsala S-751 09 Institute of Geology and Paleontology Westfa¨lische-Wilhelms Universita¨t Mu¨nster Roger Alberto Institute of Inorganic Chemistry University of Zurich Zu¨rich CH-8057 Switzerland ariel@aci.unizh.ch Freddy Adams Campus Drie Eiken University of Antwerp Universiteitsplein 1 Antwerp B-2610 Belgium freddy.adams@ua.ac.be Evgeny O. Adamov Research and Development Institute of Power Engineering (NIKIET) P.O. Box 788 Moscow 101000 Russia slp@nikiet.ru Ulrich Abram Institute of Inorganic Chemistry Freie Universita¨t Berlin Berlin D-14195 Germany abram@chemie.fu-berlin.de List of Contribut Sweden gunnar.antoni@ge.com Accelerator Center Institute of Nuclear Research of the Hungarian Academy of Sciences (ATOMKI) Bem te´r 18/C Debrecen H-4026 Hungary biri@atomki.hu Tama´s Belgya Institute of Isotopes Hungarian Academy of Sciences P.O. Box 77 Budapest H-1525 Hungary belgya@iki.kfki.hu Chemistry and Materials Science Directorate Lawrence Livermore National Laboratory Livermore, California USA baisden1@llnl.gov trish.baisden@nnsa.doe.gov Cindy E. Atkins-Duffin Energy and Environment Directorate Lawrence Livermore National Laboratory Livermore, California USA atkinsduffin1@llnl.gov rs Germany napierbowen@yahoo.co.uk Pasare´ti u´t 119 1/6 University of Debrecen Institute of Nuclear Techniques Institut fu¨r Kernchemie Neustadtgasse 1 Radiopharmacology Shuichi Enomoto Richard B. Firestone xxviii Langenzersdorf, Vienna A-2103 Austria deronfamily@wanadoo.fr David Lee Donohue International Atomic Energy Agency Vienna Universita¨t Mainz Mainz D-55128 Germany h.denschlag@uni-mainz.de Stein Deron International Atomic Energy Agency Budapest University of Technology and Economics P.O. Box 91 Budapest H-1521 Hungary doczi@reak.bme.hu Johannes O. Denschlag P.O. Box 105 Debrecen H-4010 Hungary csikai@falcon.phys.klte.hu Rita Do´czi Budapest H-1026 Hungary tbiro@sunserv.kfki.hu Julius Csikai Department of Experimental Physics Tama´s Bı´ro´ Institute of Isotopes Hungary Academy of Sciences List of Contributors Austria d.donohue@iaea.org Lawrence Berkeley National Laboratory MS 88R0192 Berkeley, California 94720 USA rbfirestone@lbl.gov Gerhart Friedlander{ Brookhaven National Laboratory Tibor Fe´nyes Institute of Nuclear Research of the Hungarian Academy of Sciences Bem-te´r 18/c Debrecen H-4026 Hungary h3813fen@ella.hu Melpomeni Fani Clinic for Nuclear Medicine University Hospital Freiburg Hugstetterstrasse 55 Freiburg D-79106 Germany melpomeni.fani@uniklinik-freiburg.de RIKENNishina Center for Accelerator–Based Science RIKEN Wako Institute 2‐1, Hirosawa Wako, Saitama 351-0198 Japan semo@riken.jp Cancer Research Center Heidelberg (DKFZ) Im Neuenheimer Feld, 280 Heidelberg D-69120 Germany m.eisenhut@dkfz-heidelberg.de Michael Eisenhut Department of Radiochemistry and Upton, NY 11973 USA 2‐1, Hirosawa Mainz D-55128 Tokai, Ibaraki 319-1195 Berkeley, CA Pa´zma´ny P. s. 1/A xxix Yoichi Fuji-ie Hiroshima University, Prof. Emeritus of Tokyo Institute of Technology 22‐1‐1221 Shirakawa Koto–ku Tokyo 135‐0021 Japan fujiie@ll.em-net.ne.jp ns.fuji-ie@atlas.plala.or.jp Marc A. Garland Nuclear Science and Technology Division Oak Ridge National Laboratory 1 Bethel Valley Road Oak Ridge, TN 37831-6423 USA garlandma@ornl.gov Stephan Good Division of Radiological Chemistry University Hospital Basel Petersgraben 4 Basel CH-4031 Switzerland stephan.good@unibas.ch Patrick M. Grant Forensic Science Center (FSC) and CSD Livermore National Laboratory Livermore, CA 94550 USA grant4@llnl.gov Henry C. Griffin Department of Chemistry University of Michigan Ann Arbor, Michigan 48109-1055 USA hcg@umich.edu Mohini Gupta MARG Manipal University Manipal 576104 Manipal, Karnataka India mohini.gupta@manipal.edu Budapest 1117 Hungary homonnay@ludens.elte.hu Dezso˝ Horva´th KFKI Research Institute for Particle and Nuclear Physics Budapest H–1525 USA dchoffman@lbl.gov Zolta´n Homonnay Institute of Chemistry Eo¨tvo¨s Lora´nd University Japan hirata.masaru@jaea.go.jp Darleane C. Hoffman Department of Chemistry University of California Germany guen.herrmann@t-online.de Masaru Hirata Advanced Science Research Center Japan Atomic Energy Agency Wako, Saitama 351‐0198 Japan haba@riken.jp Gu¨nter Herrmann Institut fu¨r Kernchemie Johannes Gutenberg-Universita¨t Hiromitsu Haba RIKENNishina Center for Accelerator–Based Science RIKEN Wako Institute List of Contributors Hungary horvath@mail.kfki.hu azkiss@namafia.atomki.hu z.klencsar@somogy.hu xxx Ian D. Hutcheon Chemical Sciences Division (CSD) and Seaborg Institute Livermore National Laboratory Livermore, CA 94550 USA hutcheon1@lln.gov Wolfgang Jacob Max-Planck-Institut fu¨r Plasmaphysik, Bereich Materialforschung, AG Reaktive Plasmaprozesse Boltzmannstrasse 2 Garching D-85748 Germany wolfgang.jacob@ipp.mpg.de Ga´bor Jancso´ KFKI Atomic Energy Research Institute P.O. Box 49 Budapest H-1525 Hungary jancso@aeki.kfki.hu Shinichiro Kamino Graduate School of Medicine, Dentistry, and Pharmaceutical Sciences Okayama University Okayama Okayama 700-8530 Japan Be´la Kanya´r Institute of Radiochemistry and Radioecology, University of Pannonia Veszpre´m Hungary kanyarb@almos.vein.hu Greg Kennedy Department of Engineering Physics Nuclear Engineering Institute, Ecole Polytechnique de Montreal P.O. Box 6079 Montreal, QC H3C 3A7 List of Contributors Canada greg.kennedy@polymtl.ca Ede Koltay Laboratory of Ion Beam Applications, Department of Electrostatic Accelerators Institute of Nuclear Research (ATOMKI), Hungarian Academy of Sciences Bem te´r 18/c Debrecen 4026 F. F. (Russ) Knapp Nuclear Medicine Program Nuclear Science and Technology Division Oak Ridge National Laboratory 2008 Oak Ridge, TN 37831-6229 USA knappffjr@ornl.gov Zolta´n Klencsa´r Chemical Research Center Hungarian Academy of Sciences Budapest Hungary A´rpa´d Z. Kiss Laboratory of Ion Beam Applications, Department of Electrostatic Accelerators Institute of Nuclear Research (ATOMKI), Hungarian Academy of Sciences Bem te´r 18/c Debrecen 4026 Hungary Tor Kihlberg Uppsala University Uppsala Imanet AB P.O. Box 967 Uppsala S-751 09 Sweden tor.kihlberg@ge.com Hungary koltay@atomki.hu korolev@nusun.jinr.ru jvkratz@uni-mainz.de xxxi Erwin Kuhn International Atomic Energy Agency Huettergasse 23 Wien, Vienna A-1140 Jens Volker Kratz Institute of Nuclear Chemistry, Johannes Gutenberg University Fritz Strassmann-Weg 2 Mainz D-55128 Germany Attila Krasznahorkay Division of Nuclear Physics Institute of Nuclear Research of the Hungarian Academy of Sciences (ATOMKI) Bem-te´r 18/c Debrecen Pf. 51, H-4001 Hungary kraszna@atomki.hu Andra´s Kova´cs Institute of Isotopes Hungarian Academy of Sciences P.O. Box 77 Budapest H-1525 Hungary akovacs@iki.kfki.hu Gyo¨rgy J. Ko¨teles National Research Institute for Radiobiology and Radiohygiene Budapest Hungary radbiol@hp.osski.hu Nikolai A. Korolev Joint Institute of Nuclear Research Dubna RUS-141980 Russian Federation Austria ekuhn@gmx.at Bengt La˚ngstro¨m Department of Biochemistry and Organic Chemistry Uppsala University Uppsala Imanet AB P.O. Box 967 Uppsala S-751 09 George Lamaze Analytical Chemistry Division National Institute of Standards and Technology 100 Bureau Drive, MS 8395 Gaithersburg, MD 20899-8395 USA george.lamaze@nist.gov Susanta Lahiri Chemical Sciences Division Saha Institute of Nuclear Physics 1/AF Bidhannagar Kolkata 700064 India susanta.lahiri@saha.ac.in Erno˝ Kuzmann Institute of Chemistry Eo¨tvo¨s Lora´nd University Pa´zma´ny P. se´ta´ny 1/A Budapest 1117 Hungary kuzmann@ludens.elte.hu Nikolay E. Kukharkin Russian Research Center ‘‘Kurchatov Institute’’ Kurchatov sq. 1 Moscow 123182 Russia ztm@adis.vver.kiae.ru List of Contributors Sweden bengt.langstrom@ge.com Gaithersburg, MD 20899 USA 100 Bureau Drive Gaithersburg, MD 20899 Hugstetterstrasse 55 Freiburg D-79106 Fukuoka 812-8581 Japan marek@chem.elte.hu USA walter.mier@med.uni-heidelberg.de xxxii y.maescc@osu.bbiq.jp Moumita Maiti Chemical Sciences Division Saha Institute of Nuclear Physics 1/AF Bidhannagar Kolkata 700064 Germany helmut.maecke@uniklinik-freiburg.de Yonezo Maeda Department of Chemistry Kyushu University Hakozaki, Higashi-ku USA lmackey@nist.gov Helmut R. Maecke Clinic for Nuclear Medicine University Hospital Freiburg richard.lindstrom@nist.gov Elizabeth A. Mackey Analytical Chemistry Division National Institute of Standards and Technology Richard M. Lindstrom Analytical Chemistry Division National Institute of Standards and Technology 100 Bureau Drive List of Contributors India moumita.maiti@saha.ac.in Arne Miller Risø High Dose Reference Laboratory Risø-DTU, Technical University of Denmark Frederiksborgvej 399, P.O. Box 49 Roskilde DK-4000 Walter Mier Department of Nuclear Medicine Radiopharmaceutical Chemistry, University of Heidelberg Im Neuenheimer Feld, 400 Heidelberg D-69120 Germany Kishor K. Mehta Arbeiterstrandbad Strasse 72 Vienna A-1210 Austria William L. McLaughlin{ National Institute of Standards and Technology Gaithersburg, MD 20902 Leonard F. Mausner Collider Accelerator Department Brookhaven National Laboratory P.O. Box 5000, Building 801 Upton, NY 11973-5000 USA mausner@bnl.gov Tama´s Marek Chemical Research Center Hungarian Academy of Sciences Budapest Hungary Denmark armi@risoe.dtu.dk Oak Ridge, TN 37831-6229 Darmstadt D64291 Pa´zma´ny P. se´ta´ny 1/A Budapest 1117 Department of Chemistry Tokyo Metropolitan University Kiyoshi Nomura Alexander F. Novgorodov Radioisotope Center Kyushu University xxxiii Germany g.muenzenberg@gsi.de Yuichiro Nagame Advanced Science Research Center Japan Atomic Energy Agency Tokai, Ibaraki 319-1195 Gottfried Mu¨nzenberg KPII GSI Helmholtzzentrum fu¨r Schwerionenforschung mbH Planckstr. 1 RIKEN Center for Molecular Imaging Science RIKEN Kobe Institute Chuo-ku Kobe, Hyogo 650-0047 Japan motomura@riken.jp Ken J. Moody Chemical Sciences Division and FSC Livermore National Laboratory Livermore, CA 94550 USA moody@llnl.gov Shinji Motomura USA mirzadehs@ornl.gov Ga´bor L. Molna´r{ Institute of Isotope and Surface Chemistry Chemical Research Center Budapest Hungary Saed Mirzadeh Nuclear Science and Technology Division Oak Ridge National Laboratory P.O. Box 2008, Mail Stop 6229 Japan nagame.yuichiro@jaea.go.jp Fukuoka Japan Ferenc Pa´szti{ KFKI Research Institute for Particle and Nuclear Physics Joint Institute of Nuclear Research Dubna RUS-141980 Russian Federation novgor@nusun.jinr.dubna.su Susumu Osaki Department of Applied Chemistry, Graduate School of Engineering The University of Tokyo Tokyo Japan k-nomura@t-adm.t.u-tokyo.ac.jp 1-7-14 Nakamachi Setagaya Tokyo 158-0091 Japan nakahara-hiromichi@c.metro-u.ac.jp Hungary nagy@chem.elte.hu Hiromichi Nakahara Sa´ndor Nagy Institute of Chemistry Eo¨tvo¨s Lora´nd University List of Contributors Budapest Hungary Hungary patkos@galaxy.elte.hu Russia niknik@kiae.ru Hungary laszlo.pusztai0@gmail.com Germany s.m.qaim@fz-juelich.de Hungary revay@iki.kfki.hu Germany ross@uni-mainz.de Germany frank.roesch@uni-mainz.de Belgium bjorn.desamber@ugent.be xxxiv Thomas Rauscher Department of Physics University of Basel Klingelbergstrasse 82 Basel CH-4056 Syed M. Qaim Institut fu¨r Nuklearchemie Forschungszentrum Ju¨lich GmbH P.O. Box 1913 Ju¨lich D-52425 La´szlo´ Pusztai Research Institute for Solid State Physics and Optics Hungarian Academy of Sciences P.O. Box 49 Budapest H-1525 Nikolay N. Ponomarev-Stepnoi Russian Research Center ‘‘Kurchatov Institute’’ Kurchatov sq. 1 Moscow 123182 Andra´s Patko´s Department of Atomic Physics Eo¨tvo¨s Lora´nd University Pa´zma´ny Pe´ter se´ta´ny 1/a Budapest H-1117 List of Contributors Switzerland thomas.rauscher@unibas.ch Tsutomu Sekine Center for the Advancement of Higher Education Tohoku University 41 Kawauchi, Aoba-ku Sendai Bjo¨rn De Samber Department of Analytical Chemistry Ghent University Krijgslaan 281 – S12 Gent Frank Ro¨sch Institute of Nuclear Chemistry Johannes Gutenberg-University of Mainz Fritz-Strassmann-Weg 2 Mainz D-55128 Tobias L. Ross Institute of Nuclear Chemistry Johannes Gutenberg-University Mainz Fritz-Strassmann-Weg 2 Mainz D-55128 Zsolt Re´vay Institute of Isotopes Hungarian Academy of Sciences P.O. Box 77 Konkoly-Thege Miklos street 29-33 Budapest H-1525 Japan tsekine@m.tohoku.ac.jp xxxv Makoto Seto Research Reactor Institute Kyoto University Kumatori-cho, Sennan-gun Osaka 590-0494 Japan seto@rri.kyoto-u.ac.jp Dawn A. Shaughnessy Chemical Sciences Division Lawrence Livermore National Laboratory P.O. Box 808, L-236 Livermore, CA 94551 USA shaughnessy2@llnl.gov Geert Silversmit Department of Analytical Chemistry Ghent University Krijgslaan 281 – S12 Gent Belgium geert.silversmit@ugent.be Gunnar Skarnemark Nuclear Chemistry, Department of Chemical and Biological Engineering Chalmers University of Technology Go¨teborg S-41296 Sweden gunnar.skarnemark@chalmers.se Lee G. Sobotka Departments of Chemistry and Physics Washington University St. Louis, Missouri 63130-4899 USA lgs@wuchem.wustl.edu Ka´roly Su¨vegh Institute of Chemistry Eo¨tvo¨s Lora´nd University Pa´zma´ny P. se´ta´ny 1/a Budapest 1117 Hungary suveghk@chem.elte.hu Veniamin A. Usov Russian Research Center ‘‘Kurchatov Institute’’ Kurchatov sq. 1 Moscow 123182 Russia vau@dhtp.kiae.ru No´ra Vajda RadAnal Ltd Budapest Hungary vajdanor@gmail.com vajdanor@reak.bme.hu Alada´r Valek Accelerator Center Institute of Nuclear Research of the Hungarian Academy of Sciences (ATOMKI) Bem te´r 18/C Debrecen H-4026 Hungary valek@atomki.hu W. Alexander Van Hook Chemistry Department University of Tennessee Knoxville, Tennessee 37996-1600 USA avanhook@utk.edu Bart Vekemans Department of Analytical Chemistry Ghent University Krijgslaan 281 – S12 Gent Belgium bart.vekemans@ugent.be Ga´bor Veres KFKI Research Institute for Particle and Nuclear Physics P.O. Box 49 Budapest H-1525 List of Contributors Hungary veres@rmki.kfki.hu xxxvi List of Contributors Attila Ve´rtes Institute of Chemistry Eo¨tvo¨s Lora´nd University Pa´zma´ny P. s. 1/A Budapest 1117 Hungary vertesa@chem.elte.hu A´rpa´d Vincze Department of Nuclear and Radioactive Materials Hungarian Atomic Energy Authority Budapest Hungary vincze@oah.hu La´szlo´ Vincze Department of Analytical Chemistry Ghent University Krijgslaan 281 – S12 Gent Belgium laszlo.vincze@ugent.be Victor E. Viola Department of Chemistry and IUCF Indiana University Bloomington, Indiana 47405 USA viola@indiana.edu Hans-Ju¨rgen Wester Department of Nuclear Medicine Klinikum rechts der Isar, Technische Universita¨t Mu¨nchen Mu¨nchen D-81675 Germany h.j.wester@lrz.tu-muenchen.de La´szlo´ Wojna´rovits Institute of Isotopes Hungarian Academy of Sciences P.O. Box 77 Budapest H-1525 Hungary wojn@iki.kfki.hu H. Kenji Yoshihara Isotope Data Institute Kusakidai 4-12-13 Iwaki city Japan kenji-yoshihara@nifty.com Michael R. Zalutsky Departments of Radiology and Biomedical Engineering Duke University Durham, NC 27710 USA zalut001@mc.duke.edu Rolf Zeisler Analytical Chemistry Division National Institute of Standards and Technology 100 Bureau Drive, MS 8395 Gaithersburg, MD 20899-8395 USA rolf.zeisler@nist.gov Manfred Zendel Department of Safeguards International Atomic Energy Agency Wagramer Strasse 5 P.O. Box 100 Vienna A-1140 Austria m.zendel@iaea.org Sa´ndor Zoletnik KFKI Research Institute for Particle and Nuclear Physics P.O. Box 49 Budapest H-1525 Hungary zoletnik@rmki.kfki.hu Volume 1 Basics of Nuclear Science 1 Nuclear and Radiochemistry: the First 100 Years G. Friedlander{1 . G. Herrmann2 1Brookhaven National Laboratory, Upton, NY, USA 2Johannes Gutenberg-Universita¨t, Mainz, Germany 1.1 The Pioneering Years . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 1.2.2 {Deceased Attila Ve´rte DOI 10.100 1.5 Current Trends . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29 1.4.5 Geo- and Cosmochronology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27 1.4.3 1.4.4 New Elements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22 Hot-Atom Chemistry and Tracer Applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25 1.4.1 1.4.2 Nuclear Reactions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 Nuclear Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20 1.4 The Golden Era . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 1.3 World War II . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16 1.2.5 Geo- and Cosmochronology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 1.2.3 1.2.4 Nuclear Reactions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9 Nuclear Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10 New Elements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13 Hot-Atom Chemistry and Tracer Applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14 1.2 The Growth Spurt of the 1930s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8 1.2.1 s, Sa´ndor Nagy, Zolta´n Klencsa´r, Rezso˝ G. Lovas & Frank Ro¨sch (eds.), Handbook of Nuclear Chemistry, 7/978-1-4419-0720-2_1, # Springer Science+Business Media B.V. 2011 same time, Otto Hahn’s treatise Applied Radiochemistry (Hahn 1936) clearly outlined the now generally accepted definition of ‘‘radiochemistry.’’ Almost immediately after the discovery of radioactivity, Marie Sklodowska Curie and 4 1 Pierre Curie beganmore detailed studies of the new phenomenon. Guided by their observation that some natural uranium ores, such as pitchblende, were more highly radioactive than corresponded to their uranium content (Sklodowska Curie 1898), they fractionated the ores chemically, using the intensity of radioactivity in the fractions as evidence for further radio- active substances. The result was the discovery, in June 1898, of a new radioactive element in the bismuth fraction (Curie and Curie, 1898); the Curies named it polonium in honor of Marie’s homeland. A few months later, in December 1898, they were able to report the discovery of another radioactive element, this one in the barium fraction separated from pitchblende (Curie et al. 1898); they named it radium. The subsequent isolation of radium from barium was accomplished by fractional crystallization of barium chloride, with radium chloride always being enriched in the crystalline phase. It soon became possible to characterize Abstract: This chapter gives a brief overview of the development of nuclear and radiochemistry fromMme. Curie’s chemical isolation of radium toward the end of the twentieth century. The first four sections deal with fairly distinct time periods: (1) the pioneering years when the only radioactive materials available were the naturally occurring ones; (2) the decade of rapid growth and expansion of both the fundamental science and its applications following the discoveries of the neutron and artificial radioactivity; (3) theWorldWar II period characterized by the intense exploration of nuclear fission and its ramifications; (4) what can be called the ‘‘golden era’’ – the 3 to 4 decades following World War II when nuclear science was generously supported and therefore flourished. In the final section, research trends pursued near the end of the century are briefly touched upon. 1.1 The Pioneering Years The field that became known as radiochemistry, dealing with the chemical manipulation of radioactive materials and the application of radioactivity to basic and applied chemical problems, originated very soon after Henri Becquerel had discovered the phenomenon of radioactivity during his studies of the fluorescence of uranium compounds (Becquerel 1896). The term ‘‘radiochemistry’’ for this field was introduced quite early, as indicated by the fact that it appeared in a book title in 1910 (Cameron 1910). However, the same termwas for some time also applied to what is now called ‘‘radiation chemistry,’’ the chemical action of radioactive (and other ionizing) radiations. Later, after the concept of the atomic nucleus was introduced in 1911 and especially after the discoveries of nuclear transmutations (1919) and of artificially produced radioactivity (1934), chemists became involved more broadly in the study of the production, properties, and reactions of atomic nuclei; in the 1930s, the term ‘‘nuclear chemistry’’ gained currency for this branch of the chemical sciences, quite analogous to organic chemistry being concerned with the synthesis, properties, and reactions of organic molecules. The creation, in 1937, of a new chair of ‘‘Chimie Nucle´aire’’ for Fre´de´ric Joliot at the Colle`ge de France was perhaps the first official recognition of the new branch of chemistry. At about the Nuclear and Radiochemistry: the First 100 Years radium spectroscopically by optical emission lines (Demarc¸ay 1898) and, thus, to confirm the discovery by an independent identification. By 1902, M. Curie had isolated 120
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