Electrostatic estimation of intercalant jump-diffusion barriers using finite-size ion models

We report on a scheme for estimating intercalant jump-diffusion barriers that are typically obtained from demanding density functional theory-nudged elastic band calculations. The key idea is to relax a chain of states in the field of the electrostatic potential that is averaged over a spherical volume using different finite-size ion models. For magnesium migrating in typical intercalation materials such as transition-metal oxides, we find that the optimal model is a relatively large shell. This data-driven result parallels typical assumptions made in models based on Onsager’s reaction field theory to quantitatively estimating electrostatic solvent effects. Because of its efficiency, our p otential o f e lectrostatics- f inite i on s ize ( PfEFIS ) barrier estimation scheme will enable rapid identification of materials with good ionic mobility.