A Topology‐Based Site‐to‐Site Jump Detection Method to Unlock Correlated Transport Mechanism in Superionic Conductors

Abstract

Atomic trajectories from molecular dynamics (MD) simulations are used to study multi‐ion correlated transport mechanism in superionic conductors (SICs). However, it remains challenging to assess the extent of correlated migration in these materials. Here, a topology‐based method is developed to detect site‐to‐site jumps of mobile ions and analyze correlations between jumps. The host lattice of SICs is partitioned into non‐overlapping polyhedra, with mobile ions assigned to these polyhedral site regions. Such a process discretizes the MD trajectories, enabling the extraction of the sequences and timings of jumps. Through appropriate spatial and temporal criteria, correlated jumps can be identified accurately in a straightforward way. Following this, two representative SICs, and , are assembled to demonstrate its potential utility and applications. Both materials exhibit correlated transport mechanism, with the former primarily featuring two‐ion jumps and the latter involving jumps of more than two ions. This method, extendable to other SICs with rigid frameworks, can assist in designing new descriptors for ionic conductivity and accelerate the discovery of SICs.