Phase stabilization by electronic entropy in plutonium

N. Harrison (), J. B. Betts, M. R. Wartenbe, F. F. Balakirev, S. Richmond, M. Jaime and P. H. Tobash
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N. Harrison: Los Alamos National Laboratory, Los Alamos
J. B. Betts: Los Alamos National Laboratory, Los Alamos
M. R. Wartenbe: Los Alamos National Laboratory, Los Alamos
F. F. Balakirev: Los Alamos National Laboratory, Los Alamos
S. Richmond: Los Alamos National Laboratory, Los Alamos
M. Jaime: Los Alamos National Laboratory, Los Alamos
P. H. Tobash: Los Alamos National Laboratory, Los Alamos

Nature Communications, 2019, vol. 10, issue 1, 1-9

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 5f-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.

Date: 2019
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DOI: 10.1038/s41467-019-11166-0

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