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Phase stabilization by electronic entropy in plutonium
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DOI：10.1038/s41467-019-11166-0.png)
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摘要
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Plutonium metal undergoes an anomalously large 25% collapse in volume from its largest volume delta phase (delta-Pu) to its low temperature a 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 delta-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 delta-Pu at elevated temperatures.
Keyword:
VOLUME MAGNETOSTRICTION
DELTA-PLUTONIUM
VALENCE TRANSITION
5F STATES
PU
FIELD
TRANSFORMATIONS
CONFIGURATION
PARAMETERS
STABILITY
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期刊
IF:
15.7
论文数:
9.4W
被引数:
91.2W
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分享收藏Dual nature of 5f electrons:: Effect of intra-atomic correlations on hopping anisotropies -: art. no. 115114.png)
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PHYSICAL REVIEW BIF3.7
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