Oxygen Diffusion in Yttria-Stabilized Zirconia: A New Simulation Model

We present a multiscale modeling approach to study oxygen diffusion in cubic yttria‐stabilized zirconia. In this approach, we employ density functional theory methods to calculate activation energies for oxygen migration in different cation environments. These are used in a kinetic Monte Carlo framework to calculate long‐time oxygen diffusivities. Simulation results show that the oxygen diffusivity attains a maximum value at around 0.1 mole fraction yttria. This variation in the oxygen diffusivity with yttria mole fraction and the calculated values for the diffusivity agree well with experiment. The competing effects of increased oxygen vacancy concentration and increasing activation energy and correlation effects for oxygen diffusion with increasing yttria mole fraction are responsible for the observed dopant content dependence of the oxygen diffusivity. We provide a detailed analysis of cation‐dopant‐induced correlation effects in support of the above explanation.