Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature
Abstract
The electronic and thermodynamic complexity of plutonium has resisted a fundamental understanding for this important elemental metal. critical test of any theory is the unusual softening of the bulk modulus with increasing temperature, a result that is counterintuitive because no or very little change in the atomic volume is observed upon heating. This unexpected behavior has in the past been attributed to competing but never-observed electronic states with different bonding properties similar to the scenario with magnetic states in Invar alloys. When using the recent observation of plutonium dynamic magnetism, we construct a theory for plutonium that agrees with relevant measurements by using density-functional-theory (DFT) calculations with no free parameters to compute the effect of longitudinal spin fluctuations on the temperature dependence of the bulk moduli in δ-Pu. We also show that the softening with temperature can be understood in terms of a continuous distribution of thermally activated spin fluctuations.
- Authors:
-
- Los Alamos National Laboratory, Los Alamos, NM 87545,
- Lawrence Livermore National Laboratory, Livermore, CA 94551
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1325832
- Alternate Identifier(s):
- OSTI ID: 1336995; OSTI ID: 1343700
- Report Number(s):
- LLNL-JRNL-693599; LA-UR-16-23906
Journal ID: ISSN 0027-8424
- Grant/Contract Number:
- SC0001089; AC52-07NA27344; AC52-06NA25396
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 113 Journal Issue: 40; Journal ID: ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; δ plutonium; elastic properties; temperature; elastic moduli; thermal expansion; DFT
Citation Formats
Migliori, Albert, Söderlind, Per, Landa, Alexander, Freibert, Franz J., Maiorov, Boris, Ramshaw, B. J., and Betts, Jon B. Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature. United States: N. p., 2016.
Web. doi:10.1073/pnas.1609215113.
Migliori, Albert, Söderlind, Per, Landa, Alexander, Freibert, Franz J., Maiorov, Boris, Ramshaw, B. J., & Betts, Jon B. Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature. United States. https://doi.org/10.1073/pnas.1609215113
Migliori, Albert, Söderlind, Per, Landa, Alexander, Freibert, Franz J., Maiorov, Boris, Ramshaw, B. J., and Betts, Jon B. Mon .
"Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature". United States. https://doi.org/10.1073/pnas.1609215113.
@article{osti_1325832,
title = {Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature},
author = {Migliori, Albert and Söderlind, Per and Landa, Alexander and Freibert, Franz J. and Maiorov, Boris and Ramshaw, B. J. and Betts, Jon B.},
abstractNote = {The electronic and thermodynamic complexity of plutonium has resisted a fundamental understanding for this important elemental metal. critical test of any theory is the unusual softening of the bulk modulus with increasing temperature, a result that is counterintuitive because no or very little change in the atomic volume is observed upon heating. This unexpected behavior has in the past been attributed to competing but never-observed electronic states with different bonding properties similar to the scenario with magnetic states in Invar alloys. When using the recent observation of plutonium dynamic magnetism, we construct a theory for plutonium that agrees with relevant measurements by using density-functional-theory (DFT) calculations with no free parameters to compute the effect of longitudinal spin fluctuations on the temperature dependence of the bulk moduli in δ-Pu. We also show that the softening with temperature can be understood in terms of a continuous distribution of thermally activated spin fluctuations.},
doi = {10.1073/pnas.1609215113},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 40,
volume = 113,
place = {United States},
year = {Mon Sep 19 00:00:00 EDT 2016},
month = {Mon Sep 19 00:00:00 EDT 2016}
}
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https://doi.org/10.1073/pnas.1609215113
https://doi.org/10.1073/pnas.1609215113
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Cited by: 26 works
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