Machine-learning-driven modelling of amorphous and polycrystalline BaZrS3

Abstract

The chalcogenide perovskite material BaZrS3 is of growing interest for emerging thin-film photovoltaics. Here we show how machine-learning-driven modelling can be used to describe the material's amorphous precursor as well as polycrystalline structures with complex grain boundaries. Using a bespoke machine-learned interatomic potential (MLIP) model for BaZrS3, we study the atomic-scale structure of the amorphous phase, quantify grain-boundary formation energies, and create realistic-scale polycrystalline structural models which can be compared to experimental data. Beyond BaZrS3, our work exemplifies the increasingly central role of MLIPs in materials chemistry and marks a step towards realistic device-scale simulations of materials that are gaining momentum in the fields of photovoltaics and photocatalysis.