Shaping the Future of Solid‐State Electrolytes through Computational Modeling

Abstract Advances and progress in computational research that aims to understand and improve solid‐state electrolytes (SSEs) are outlined. One of the main challenges in the development of all‐solid‐state batteries is the design of new SSEs with high ion diffusivity that maintain chemical and phase stability and thereby provide a wide electrochemical stability window. Solving this problem requires a deep understanding of the diffusion mechanism and properties of the SSEs. A second important challenge is the development of an understanding of the interface between the SSE and the electrode. The role of molecular simulations and modeling in dealing with these challenges is discussed, with reference to examples in the literature. The methods used and issues considered in recent years are highlighted. Finally, a brief outlook about the future of modeling in studying solid‐state battery technology is presented.