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Title: Hidden disorder in the α'→δ transformation of Pu-1.9 at.% Ga

Enthalpy and entropy are thermodynamic quantities critical to determining how and at what temperature a phase transition occurs. At a phase transition, the enthalpy and temperature-weighted entropy differences between two phases are equal (ΔH=TΔS), but there are materials where this balance has not been experimentally or theoretically realized, leading to the idea of hidden order and disorder. In a Pu-1.9 at. % Ga alloy, the δ phase is retained as a metastable state at room temperature, but at low temperatures, the δ phase yields to a mixed-phase microstructure of δ- and α'-Pu. The previously measured sources of entropy associated with the α'→δ transformation fail to sum to the entropy predicted theoretically. We report an experimental measurement of the entropy of the α'→δ transformation that corroborates the theoretical prediction, and implies that only about 65% of the entropy stabilizing the δ phase is accounted for, leaving a missing entropy of about 0.5 kB/atom. Some previously proposed mechanisms for generating entropy are discussed, but none seem capable of providing the necessary disorder to stabilize the δ phase. This hidden disorder represents multiple accessible states per atom within the δ phase of Pu that may not be included in our current understanding ofmore » the properties and phase stability of δ-Pu.« less
Authors:
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Publication Date:
OSTI Identifier:
1103511
Type:
Publisher's Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 85; Journal Issue: 22; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English