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

J. R. Jeffries, M. E. Manley, M. A. Wall, K. J.M. Blobaum, A. J. Schwartz

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4 Scopus citations

Abstract

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 k B/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 of the properties and phase stability of δ-Pu.

Original languageEnglish
Article number224104
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume85
Issue number22
DOIs
StatePublished - Jun 6 2012
Externally publishedYes

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