Accelerated Design of Battery Materials Interfaces by Embedded‐Atom‐Inspired Bond Valence Sum Forcefields. Issue 19 (8th August 2021)

• Record Type: Journal Article
• Authors: Pu, Yuhan; Dai, Ruoyu; Adams, Stefan
• Is Part Of: Physica status solidi. Volume 218:Issue 19(2021)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-08-08
• Subjects: battery materials -- bond valence -- computational materials design -- embedded atom method; Solid state physics -- Periodicals; Solids -- Industrial applications -- Periodicals; 530.41
• DOI: 10.1002/pssa.202100318
• Languages: English
• ISSNs: 1862-6300

Abstract

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. Abstract : A novel embedded‐atom‐method‐inspired bond valence sum‐based multibody forcefield is introduced to enhance the modeling of polycrystalline ceramic materials. It retains the transferability and computational efficiency of the bond valence site energy approach, but enables the modeling of free and buried interfaces as urgently required to accelerate the design of high‐performance all‐solid‐state energy storage systems.