Accelerated Design of Battery Materials Interfaces by Embedded‐Atom‐Inspired Bond Valence Sum Forcefields

Abstract

To achieve higher energy density in safer energy storage systems, a transition to ceramic all‐solid‐state batteries is widely expected. Their performance and cycle‐life is largely controlled by processes at buried interfaces. While experimental operando probing of interfacial processes is under development, first‐principle computational methods are challenged by the complexity of the multiphase models and long simulation periods required to capture slow degradation processes. Thus, simpler empirical reactive forcefields have the potential to substantially accelerate the design and optimization of all‐solid‐state batteries, provided that parameters are available for a wide range of relevant atom types. The energy‐scaled bond valence‐based softBV forcefield has successfully enabled the design of new solid electrolytes or insertion‐type electrode materials and analyses of ion transport processes therein. As a two‐body forcefield, it enables fast simulations for complex structures over long periods, but inevitably shares the tendency of two‐body forcefields to maximize coordination numbers if free volume facilitates a reorganization of the atoms, which makes them less suitable for studying interfacial processes. Herein, this vulnerability of two‐body forcefields is overcome in a computationally efficient way by introducing an embedded‐atom‐method‐inspired bond‐valence‐sum‐based new class of transferable forcefields and its effective use for modeling of surfaces and interfaces is demonstrated.