Quantum mechanical calculations of uranium phases and niobium defects in γ-uranium

Depleted uranium (U) from fuel enrichment processes has a variety of applications due to its high density. With the addition of a small concentration of niobium (Nb), U becomes stainless. Nb is fully miscible with the high-temperature γ phase of U and tends to segregate upon cooling below 1050 K. The starting point of segregation is the configuration of Nb substitutional or interstitial defects. Using quantum mechanical calculations, the authors find that the formation energy of a single vacancy is 1.08 eV, that of Nb substitution 0.59 eV, that of Nb interstitial at octahedral site 1.58 eV, and that of Nb interstitial at tetrahedral site 2.35 eV in the dilute limit of isolated defects; all with reference to a reservoir of the pure γ phase U and pure Nb. The analysis of electronic structures reveals the correlation of formation energies of Nb defects with the local perturbations of electron distribution. Higher formation energy of Nb defects correlates with larger perturbation. Based on this study, Nb atoms thermodynamically prefer to occupy substitutional sites in the γ phase U.