Structure stability of (U, Pu) C and (U, Pu) N compositions

Abstract Atomic scale computer simulations based on density functional theory (DFT) are used to calculate the formation energies and structures associated with phases in the U–N, Pu–N, U–C and Pu–C systems. Stable phases across the compositional spaces, from the metal to the nitrogen gas or graphite...

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Bibliographic Details
Main Authors: William A. Watson, Sophie Cooper, Matthew Horton, Robin W. Grimes
Format: Article
Language:English
Published: Nature Portfolio 2025-06-01
Series:Scientific Reports
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Online Access:https://doi.org/10.1038/s41598-025-03910-y
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Summary:Abstract Atomic scale computer simulations based on density functional theory (DFT) are used to calculate the formation energies and structures associated with phases in the U–N, Pu–N, U–C and Pu–C systems. Stable phases across the compositional spaces, from the metal to the nitrogen gas or graphite end members, are identified using convex hull analysis. Many predicted phases correspond to those known from experimental phase diagrams (e.g. UN, U2N3; PuN; UC, U2C3; Pu2C3). However, many phases only sit on the convex hull upon inclusion of a suitably characterised Hubbard parameter (i.e. DFT + U). A nonstoichiometric composition of UN2−x is identified on the U–N convex hull but others, including stoichiometric UN2, are close to the line. A stoichiometric structure for Pu3C2 with $$R\overline{3}c$$ symmetry is identified, alongside which a nonstoichiometric PuC1−x phase has a similar energy.
ISSN:2045-2322