A theoretical perspective on solid-state ionic interfaces

Solid-state ionic conductors find application across various domains in materials science, particularly showcasing their significance in energy storage and conversion technologies. To effectively utilize these materials in high-performance electrochemical devices, a comprehensive understanding and precise control of charge carriers' distribution and ionic mobility at interfaces are paramount. A major challenge lies in unravelling the atomic-level processes governing ion dynamics within intricate solid and interfacial structures, such as grain boundaries and heterophases. From a theoretical viewpoint, in this Perspective article, my focus is to offer an overview of the current comprehension of key aspects related to solid-state ionic interfaces, with a particular emphasis on solid electrolytes for batteries, while providing a personal critical assessment of recent research advancements. I begin by introducing fundamental concepts for understanding solid-state conductors, such as the classical diffusion model and chemical potential. Subsequently, I delve into the modelling of space-charge regions, which are pivotal for understanding the physicochemical origins of charge redistribution at electrified interfaces. Finally, I discuss modern computational methods, such as density functional theory and machine-learned potentials, which offer invaluable tools for gaining insights into the atomic-scale behaviour of solid-state ionic interfaces, including both ionic mobility and interfacial reactivity aspects. This article is part of the theme issue 'Celebrating the 15th anniversary of the Royal Society Newton International Fellowship'.