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Phase stabilization by electronic entropy in plutonium

Author

Listed:
  • 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)

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.

Suggested Citation

  • N. Harrison & J. B. Betts & M. R. Wartenbe & F. F. Balakirev & S. Richmond & M. Jaime & P. H. Tobash, 2019. "Phase stabilization by electronic entropy in plutonium," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11166-0
    DOI: 10.1038/s41467-019-11166-0
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