Going against the Grain: Atomistic Modeling of Grain Boundaries in Solid Electrolytes for Solid-State Batteries

Abstract

Atomistic modeling techniques, including density functional theory and molecular dynamics, play a critical role in the understanding, design, discovery, and optimization of bulk solid electrolyte materials for solid-state batteries. In contrast, despite the fact that the atomistic simulation of microstructural inhomogeneities, such as grain boundaries, can reveal essential information regarding the performance of solid electrolytes, such simulations have so far only been limited to a relatively small selection of materials. In this Perspective, the fundamental properties of grain boundaries in solid electrolytes that can be determined and manipulated through state-of-the-art atomistic modeling are illustrated through recent studies in the literature. The insights and examples presented here will inspire future computational studies of grain boundaries with the aim of overcoming their often detrimental impact on ion transport and dendrite growth inhibition in solid electrolytes.