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Lattice constant in nonstoichiometric uranium dioxide from first principles

Abstract : Nonstoichiometric uranium dioxide experiences a shrinkage of its lattice constant with increasing oxygen content, in both the hypostoichiometric and the hyperstoichiometric regimes. Based on first-principles calculations within the density functional theory (DFT)+$U$ approximation, we have developed a point defect model that accounts for the volume of relaxation of the most significant intrinsic defects of UO$_2$. Our point defect model takes special care of the treatment of the charged defects in the equilibration of the model and in the determination of reliable defect volumes of formation. In the hypostoichiometric regime, the oxygen vacancies are dominant and explain the lattice constant variation with their surprisingly positive volume of relaxation. In the hyperstoichiometric regime, the uranium vacancies are predicted to be the dominating defect,in contradiction with experimental observations. However, disregarding uranium vacancies allows us to recover a good match for the lattice-constant variation as a function of stoichiometry. This can be considered a clue that the uranium vacancies are indeed absent in UO$_{2+x}$ , possibly due to the very slow diffusion of uranium.
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Fabien Bruneval, Michel Freyss, Jean-Paul Crocombette. Lattice constant in nonstoichiometric uranium dioxide from first principles. Physical Review Materials, American Physical Society, 2018, 2, pp.023801. ⟨10.1103/PhysRevMaterials.2.023801⟩. ⟨cea-02063621⟩



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