On the valence fluctuation in the early actinide metals
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
© 2015 Elsevier B.V. All rights reserved. Recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f 3 and f 4 configurations, respectively, with only minor contributions from other configurations. For plutonium (both α and δ phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f 6 compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.
- Research Organization:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- AC52-07NA27344; AC52-06NA25396; AC02-05CH11231
- OSTI ID:
- 1248266
- Alternate ID(s):
- OSTI ID: 1252027; OSTI ID: 1409777; OSTI ID: 1436591
- Report Number(s):
- LLNL-JRNL-672996; LA-UR-17-24461
- Journal Information:
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 207, Issue C; ISSN 0368-2048
- Publisher:
- ElsevierCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Density-functional theory for plutonium
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journal | January 2019 |
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