Phase stabilization by electronic entropy in plutonium
Abstract
Abstract Plutonium metal undergoes an anomalously large 25% collapse in volume from its largest volume δ phase ( δ -Pu) to its low temperature α phase, yet the underlying thermodynamic mechanism has largely remained a mystery. Here we use magnetostriction measurements to isolate a previously hidden yet substantial electronic contribution to the entropy of δ -Pu, which we show to be crucial for the stabilization of this phase. The entropy originates from two competing instabilities of the 5 f -electron shell, which we show to drive the volume of Pu in opposing directions, depending on the temperature and volume. Using calorimetry measurements, we establish a robust thermodynamic connection between the two excitation energies, the atomic volume, and the previously reported excess entropy of δ -Pu at elevated temperatures.
- Authors:
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1619833
- Alternate Identifier(s):
- OSTI ID: 1825427
- Report Number(s):
- LA-UR-19-20229
Journal ID: ISSN 2041-1723; 3159; PII: 11166
- Grant/Contract Number:
- 89233218CNA000001; 20180025DR
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 10 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Citation Formats
Harrison, N., Betts, J. B., Wartenbe, M. R., Balakirev, F. F., Richmond, S., Jaime, M., and Tobash, P. H. Phase stabilization by electronic entropy in plutonium. United Kingdom: N. p., 2019.
Web. doi:10.1038/s41467-019-11166-0.
Harrison, N., Betts, J. B., Wartenbe, M. R., Balakirev, F. F., Richmond, S., Jaime, M., & Tobash, P. H. Phase stabilization by electronic entropy in plutonium. United Kingdom. https://doi.org/10.1038/s41467-019-11166-0
Harrison, N., Betts, J. B., Wartenbe, M. R., Balakirev, F. F., Richmond, S., Jaime, M., and Tobash, P. H. Thu .
"Phase stabilization by electronic entropy in plutonium". United Kingdom. https://doi.org/10.1038/s41467-019-11166-0.
@article{osti_1619833,
title = {Phase stabilization by electronic entropy in plutonium},
author = {Harrison, N. and Betts, J. B. and Wartenbe, M. R. and Balakirev, F. F. and Richmond, S. and Jaime, M. and Tobash, P. H.},
abstractNote = {Abstract Plutonium metal undergoes an anomalously large 25% collapse in volume from its largest volume δ phase ( δ -Pu) to its low temperature α phase, yet the underlying thermodynamic mechanism has largely remained a mystery. Here we use magnetostriction measurements to isolate a previously hidden yet substantial electronic contribution to the entropy of δ -Pu, which we show to be crucial for the stabilization of this phase. The entropy originates from two competing instabilities of the 5 f -electron shell, which we show to drive the volume of Pu in opposing directions, depending on the temperature and volume. Using calorimetry measurements, we establish a robust thermodynamic connection between the two excitation energies, the atomic volume, and the previously reported excess entropy of δ -Pu at elevated temperatures.},
doi = {10.1038/s41467-019-11166-0},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United Kingdom},
year = {2019},
month = {7}
}
https://doi.org/10.1038/s41467-019-11166-0
Web of Science
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