Lattice-renormalized geometric frustration drives fast ionic transport

Abstract

Fast ionic transport is commonly understood from two complementary perspectives: soft lattices that facilitate ion migration, and frustrated ionic sublattices that host multiple nearly degenerate configurations. Here, we show that the host lattice and ionic geometric frustration are fundamentally coupled, and together shape a lattice-renormalized free-energy landscape that unifies these two perspectives. Starting from a coupled ion-lattice Hamiltonian and eliminating the adiabatic lattice response, we derive a configuration-dependent free-energy renormalization that takes a quadratic form of the ionic configurational forces weighted by the inverse stiffness of the host lattice. In a coarse-grained representation, this renormalization decomposes into local lattice relaxation and non-local interference between lattice-response fields. These two contributions reshape local ionic configurations and their correlations, thereby redistributing the configurational statistical weights underlying collective ionic transport. Atomistic simulations of cubic Li${}_7$La${}_3$Zr${}_2$O${}_{12}$ and AgCrSe${}_2$ substantiate this physical picture, from microscopic configurational rearrangements to macroscopic diffusion dynamics. This framework therefore recasts fast ionic transport as a lattice-renormalized geometric frustration problem, in which lattice softness, ionic frustration, and collective diffusion all arise from the same underlying landscape.