Nonequilibrium molecular dynamics for accelerated computation of ion–ion correlated conductivity beyond Nernst–Einstein limitation

Abstract Condensed matters with high ionic conductivities are crucial in various solid devices such as solid-state batteries. The conduction is characterized by the cooperative motion associated carrier density. However, cost of computing correlated has forced almost all ab initio molecular dynamics (MD) to rely on Nernst–Einstein dilute-solution approximation, which ignores cross-correlation effect. Here we develop a chemical color-diffusion nonequilibrium MD (CCD-NEMD) method, enables calculate fewer sampling steps than conventional MD. This CCD-NEMD demonstrated well evaluate representative electrolyte bulk Li 10 GeP 2 S 12 and 7 La 3 Zr O . We also applied grain boundary its applicability for calculating interfacial local conductivities, essential investigating boundaries composite electrolytes. can provide further accurate understanding ionics correlations promote developing devices.