Thermal conductivity and diffusion mechanisms of noble gases in uranium dioxide: A DFT plus U study

The bulk properties of uranium dioxide (UO2) have been investigated using Hubbard corrected density functional theory (DFT + U) calculations. Monitoring of the occupation matrix for 5f electrons of the uranium atoms is found to be crucial to avoid metastable state solutions and consequently to obtain the true ground state properties of bulk UO2. The lattice contribution to the thermal conductivity was obtained by the solution of the Boltzmann transport equation for phonons based on the interatomic force constants obtained from DFT thorn U calculations. Furthermore, the relative stabilities of noble gases (He, Ne, Ar, Kr, and Xe) in the octahedral interstitial site of bulk UO2 and their migration are revisited. The effect of the supercell approach for point defects is taken into account by considering the long-range elastic interactions. The computed incorporation energies and energy barriers indicate a size-dependent mechanism for the interstitial migration of noble gases. Crown Copyright (C) 2019 Published by Elsevier B.V. All rights reserved.