Noble Gas Bubbles in Bcc Metals: Ab Initio-Based Theory and Kinetic Monte Carlo Modeling

Abstract

Understanding the interactions of noble gases with metals is of fundamental importance for the design of radiation-resistant structural materials for fission and fusion nuclear reactors. Here we present a unified theory for describing the energetics of He, Ne, Ar, and Kr bubbles in bcc metals in group 5B (V, Nb, Ta), 6B (Cr, Mo, W) and 8B (Fe). Our predictive analytical model is based on the effective-medium and isotropic elasticity theories, and is parameterized using density functional theory (DFT) calculations of small gas-vacancy clusters. By performing kinetic Monte Carlo (KMC) simulations driven by our analytical model, we have predicted the lifetimes of noble gas bubbles and their coarsening by Ostwald ripening. Our most notable finding is the exceptionally higher thermal stability of Ne, Ar and Kr bubbles than He bubbles in bcc metals, conferring them outstanding resistance to Ostwald ripening. The physical origin of the unexpected stability of bubbles formed by large noble gas atoms has been further elucidated. Our theoretical finding is consistent with the experimental observation of He gas bubble superlattice (GBS) coarsening under thermal annealing, and provides new insights on the exceptional stability of fission GBS in bcc U-Mo up to a high homologous temperature of 0.78.