On the valence fluctuation in the early actinide metals
Abstract
© 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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- 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 Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1248266
- Alternate Identifier(s):
- OSTI ID: 1252027; OSTI ID: 1409777; OSTI ID: 1436591
- Report Number(s):
- LLNL-JRNL-672996; LA-UR-17-24461
Journal ID: ISSN 0368-2048
- Grant/Contract Number:
- AC52-07NA27344; AC52-06NA25396; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Electron Spectroscopy and Related Phenomena
- Additional Journal Information:
- Journal Volume: 207; Journal Issue: C; Journal ID: ISSN 0368-2048
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; valence fluctuations; actinides; X-ray emission spectroscopy; density functional theory
Citation Formats
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., and Nordlund, D. On the valence fluctuation in the early actinide metals. United States: N. p., 2015.
Web. doi:10.1016/j.elspec.2015.11.014.
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. On the valence fluctuation in the early actinide metals. United States. https://doi.org/10.1016/j.elspec.2015.11.014
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., and Nordlund, D. Tue .
"On the valence fluctuation in the early actinide metals". United States. https://doi.org/10.1016/j.elspec.2015.11.014. https://www.osti.gov/servlets/purl/1248266.
@article{osti_1248266,
title = {On the valence fluctuation in the early actinide metals},
author = {Soderlind, P. and Landa, A. and Tobin, J. G. and Allen, P. and Medling, S. and Booth, C. H. and Bauer, E. D. and Cooley, J. C. and Sokaras, D. and Weng, T. -C. and Nordlund, D.},
abstractNote = {© 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.},
doi = {10.1016/j.elspec.2015.11.014},
journal = {Journal of Electron Spectroscopy and Related Phenomena},
number = C,
volume = 207,
place = {United States},
year = {Tue Dec 15 00:00:00 EST 2015},
month = {Tue Dec 15 00:00:00 EST 2015}
}
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Works referencing / citing this record:
Density-functional theory for plutonium
journal, January 2019
- Söderlind, Per; Landa, A.; Sadigh, B.
- Advances in Physics, Vol. 68, Issue 1