The diffusion of point defects in uranium mononitride: Combination of DFT and atomistic simulation with novel potential

The properties of point defects in uranium mononitride (UN) are studied by ab initio calculations and molecular dynamics simulations with a new interatomic potential. Density functional theory (DFT) calculations are used for fitting of the parameters of the angular-dependent interatomic potential, as well as for evaluation of the defects formation and migration energies. Molecular dynamics (MD) simulations are applied to analyse what migration mechanisms are activated at finite temperatures and to calculate diffusion coefficients of point defects. It is shown that the U antisite defects play an important role in the U-rich UN1-x. During migration the interstitial uranium is able to knock-out nitrogen atom, and this act leads to formation of U in antisite and N interstitial. This effect results in dependence of the diffusivity of U-interstitials on the concentration of defects in the N sublattice. Another peculiarity of UN is the large athermal concentration of U-vacancies in the N-rich UN1+x. This is due to close formation energies of nitrogen Frenkel pairs and Schottky defects. In addition, the applicability of the new potential for description of various phase transitions in UN is discussed. (C) 2015 Elsevier B.V. All rights reserved.