On the valence fluctuation in the early actinide metals

Soderlind, P.; Landa, A.; Tobin, J. G.; Allen, P.; Medling, S.; Booth, C. H.; Bauer, E. D.; Cooley, J. C.; Sokaras, D.; Weng, T. -C.; Nordlund, D.

doi:10.1016/j.elspec.2015.11.014

Title: On the valence fluctuation in the early actinide metals

Journal Article · Tue Dec 15 00:00:00 EST 2015 · Journal of Electron Spectroscopy and Related Phenomena

DOI:https://doi.org/10.1016/j.elspec.2015.11.014· OSTI ID:1248266

Soderlind, P. ^[1]; Landa, A. ^[1]; Tobin, J. G. ^[1]; Allen, P. ^[1]; Medling, S. ^[2]; Booth, C. H. ^[2]; Bauer, E. D. ^[3]; Cooley, J. C. ^[3]; Sokaras, D. ^[4]; Weng, T. -C. ^[4]; Nordlund, D. ^[4]

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.

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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

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Cited by: 10 works

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References (17)

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Density-functional theory for plutonium Söderlind, Per; Landa, A.; Sadigh, B. Advances in Physics, Vol. 68, Issue 1 https://doi.org/10.1080/00018732.2019.1599554	journal	January 2019

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