Cluster dynamics simulation of xenon diffusion during irradiation in UO2

Abstract Diffusion of fission gas in UO2 nuclear fuel impacts several important performance metrics, such as fission gas release, swelling, and thermal conductivity. Current empirical models of fission gas release have significant uncertainty, some of which derives from the bulk diffusion rate and its dependence on, for example, fuel chemistry and irradiation. We have applied the previously-developed Free Energy Cluster Dynamics (FECD) methodology in the code Centipede to calculate xenon cluster concentrations in UO2 under intrinsic (high temperature) and irradiation-enhanced (intermediate temperature) conditions in order to develop a model of the xenon diffusion coefficient based on the atomic scale mechanisms responsible for transport. While the diffusion mechanism for xenon in UO2 is adequately described by the Xe + U2O vacancy cluster for intrinsic conditions, a similar process is not capable of capturing measured in-pile fission gas diffusivity at intermediate temperatures. Therefore, a different diffusion mechanism must dominate under this regime. Using calculated atomistic data, we have shown that irradiation-enhanced diffusion at intermediate temperatures occurs via the larger Xe + U4Oy vacancy clusters, which have lower migration barriers and increase in concentration by several orders of magnitude compared to intrinsic conditions. This mechanism is enabled by the increased uranium vacancy concentration under irradiation due to Frenkel pair production. In addition, the fast migration of uranium interstitials with two attached oxygen interstitials lowers the total uranium interstitial concentration through reactions with sinks. This allows the extended defects, such as Xe + U4Oy vacancy clusters, to maintain high concentrations by limiting annihilation with attached vacancies. Predictions using th-e Xe + U4Oy diffusion mechanism are in good agreement with experiment, albeit with some differences in the Arrhenius slope, which we believe may be related to either experimental or model parameter uncertainty. Finally, an analytical expression suitable for application in fuel performance simulations was derived to capture the predictions of the Centipede simulations.