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Properties of Group Five and Group Seven Transactinium Elements

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Properties of Group Five and Group Seven Transactinium Elements LBNL-47475 Properties of Group Five and Group Seven Transactinium Elements by Philip Arthur Wilk Ph.D. Thesis Department of Chemistry University of California, Berkeley Berkeley, CA 94720 and Nuclear Science Division Ernest Orlando Lawrence Berkeley National Laboratory Berkeley, CA 94720 May 2001 Properties of Group Five and Group Seven Transactinium Elements by Philip Arthur Wilk Bachelor of Arts (Reed College) 1995 A dissertation submitted in partial satisfaction of the Requirements for the degree of Doctor of Philosophy in Chemistry in the GRADUATE DIVISION of the UNIVERSITY OF CALIFORNIA AT BERKELEY Committee in charge: Professor Darleane C. Hoffman, Chair Professor Heino Nitsche Professor P. Buford Price May 2001 This work was supported in part by the Director, Office of Science, Office of High Energy and Nuclear Physics, Division of Nuclear Physics, of the U.S. Department of Energy under Contract No. DE-AC03-76SF00098 1 LBNL-47475 Properties of Group Five and Group Seven Transactinium Elements Copyright © 2001 by Philip Arthur Wilk Portions of this dissertation have been previously published by the author: P. A. Wilk, K. E. Gregorich, M. B. Hendricks, M. R. Lane, D. M. Lee, C. A. McGrath, D. A. Shaughnessy, D. A. Strellis, E. R. Sylwester, D. C. Hoffman, “Improved Half-life Measurement of 224Pa and its 209Bi(18O,3n)224Pa Production Cross Section”, Phys. Rev. C 56, 1626-8 (1997) and Erratum, Phys. Rev. C 58, 1352 (1998). P. A. Wilk, K. E. Gregorich, A. Türler, C. A. Laue, R. Eichler, V. Ninov, J. L. Adams, U. W. Kirbach, M. R. Lane1, D. M. Lee, J. B. Patin, D. A. Shaughnessy, D. A. Strellis, H. Nitsche, and D. C. Hoffman, “Evidence for New Isotopes of Element 107: 266Bh and 267Bh”, Phys. Rev. Lett. 85, 2697 (2000). R. Eichler, W. Brüchle, Ch. Düllmann, R. Dressler, B. Eichler, H.W. Gäggeler, K.E. Gregorich, T. Häfeli, U. Kirbach, D.C. Hoffman, S. Hübener, D.T. Jost, V.M. Lavanchy, C.A. Laue, H. Nitsche, J. Patin, D. Piguet, M. Schädel, D. Strellis, S. Taut, L. Tobler, Y. Tsyganov, A. Türler, A.Vahle, P.A. Wilk, A.B. Yakushev, P. Zimmermann, Nature 407, 63 (2000). The U.S. Department of Energy has the right to use this document for any purpose whatsoever including the right to reproduce all or any part thereof. Abstract Properties of Group Five and Group Seven Transactinium Elements by Philip Arthur Wilk Doctor of Philosophy in Chemistry University of California, Berkeley Professor Darleane Hoffman, Chair The detection and positive identification of the short-lived, low cross section isotopes used in the chemical studies of the heaviest elements are usually accomplished by measuring their α-decay, thus the nuclear properties of the heaviest elements must be examined simultaneously with their chemical properties. The isotopes 224Pa and 266,267Bh have been studied extensively as an integral part of the investigation of the heaviest members of the groups five and seven of the periodic table. The half-life of 224Pa was determined to be 855±19 ms by measuring its α-decay using our rotating wheel, solid state detector system at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron. Protactinium was produced by bombardment of a bismuth target. New neutron rich isotopes, 267Bh and 266Bh, were produced in bombardments of a 249Bk target and their decay was observed using the rotating wheel system. The 266Bh that was produced decays with a half-life of ≈1 s by emission of α- 1 particles with an average energy of 9.25±0.03 MeV. 267Bh was observed to decay with +14 a 17−6 s half-life by emission of α-particles with an average energy of 8.83±0.03 MeV. The chemical behavior of hahnium, Ha (element 105) was investigated using the fast on-line continuous liquid extraction and detection system SISAK-LISSY. Hahnium was not observed in this experiment following transport and extraction. Protactinium was used as on-line test of the apparatus to determine the experimental efficiency of the entire system. Unfortunately, the amount of protactinium observed after the extraction, compared to the amount produced, was extremely small, only 2.5%. The extraction of the protactinium test isotope indicated the efficiency of the apparatus was too low to observe the extraction of hahnium. The chemical behavior of oxychloride compounds of bohrium was investigated by isothermal gas adsorption chromatography in a quartz column at 180, 150, and 75°C. It was found to be less volatile than the corresponding compounds of the lighter group seven homologues, rhenium and technetium, which had been measured previously with the same apparatus. Assuming the bohrium compound to be BhO3Cl, the evaluated standard adsorption enthalpy, ∆Hads, of BhO3Cl on the quartz surface +9 was calculated from Monte Carlo fits to the volatility data to be - 75−6 kJ/mol. The +3 +3 adsorption enthalpies for TcO3Cl and ReO3Cl are - 51−3 and - 61−3 kJ/mol respectively. 2 1.1 Dedication This thesis is dedicated to the Reed Reactor Facility (RRF) of Reed College, Portland, Oregon and the Summer School in Nuclear Chemistry that was sponsored by the Division of Nuclear Chemistry and Technology of the American Chemical Society. These two institutions have maintained a commitment to undergraduate education in the field of nuclear chemistry that is unparalleled. It is my hope that Reed will soon replace the long missing radiochemistry professor of the chemistry department to echo this commitment to nuclear and radiochemistry. Without the education and the experience I received from the RRF and the contacts I made at the ACS summer school, I certainly would not be writing this thesis. Go Griffins! i 1.2 Acknowledgments First and foremost, I would like to thank Professor Darleane C. Hoffman, for giving me the chance to pursue nuclear chemistry at Berkeley. I am most indebted to the support and advice of the entire Hoffman group and affiliates overseas that I have had a chance to work with, especially the veteran group members Dawn Shaughnessy, Joshua Patin, Diana Lee, and Ken Gregorich for their extensive help. Its been great to work with you all during such exciting times in nuclear chemistry! I would like to give a special thank-you to Charlise Tiee and Scott Locklin for being great friends and colleagues. I quite literally could not have done it without you two. I would also like to thank my parents for their support throughout my entire education. I would like to thank the staff and crew of the LBNL 88-Inch Cyclotron for their assistance and support. I am indebted to the Office of Science, Office of Basic Energy Research, Division of Chemical Sciences, of the U.S. Department of Energy, for making the 249Bk target material available through the transplutonium element production program at the Oak Ridge National Laboratory. This work was supported in part by the Director, Office of Science, Office of High Energy and Nuclear Physics, Division of Nuclear Physics, of the U. S. Department of Energy under Contract No. DE-AC03-76SF00098. ii 1.3 Table of Contents 1.1 Dedication..................................................................................................................................i 1.2 Acknowledgments ....................................................................................................................ii 1.3 Table of Contents ....................................................................................................................iii 1.4 List of Figures...........................................................................................................................v 1.5 List of Tables ...........................................................................................................................vi CHAPTER 1: INTRODUCTION...........................................................................1 1.1 History.......................................................................................................................................1 1.2 Scope of Thesis .........................................................................................................................5 CHAPTER 2: THEORY ......................................................................................7 2.1 Nuclear Theory ........................................................................................................................7 2.1.1 N=162 Neutron Shell.........................................................................................................7 2.1.2 Nuclear structure of 266Bh and 267Bh..................................................................................8 2.1.2.1 Spontaneous fission...................................................................................................8 2.1.2.2 Alpha decay...............................................................................................................8 2.1.2.3 Electron-capture decay .............................................................................................9 2.2 Chemical Theory....................................................................................................................10 2.2.1 Importance of theory to the experimentalist....................................................................10 2.2.2 Relativistic calculations...................................................................................................10 2.2.3 Rutherfordium..................................................................................................................12 2.2.4 Hahnium ..........................................................................................................................15
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