Towards the reliable calculation of residence time for off-lattice kinetic Monte Carlo simulations

Kinetic Monte Carlo (KMC) methods have the potential to extend the accessible timescales of off-lattice atomistic simulations beyond the limits of molecular dynamics by making use of transition state theory and parallelization. However, it is a challenge to identify a complete catalog of events accessible to an off-lattice system in order to accurately calculate the residence time for KMC. Here we describe possible approaches to some of the key steps needed to address this problem. These include methods to compare and distinguish individual kinetic events, to deterministically search an energy landscape, and to define local atomic environments. When applied to the ground state ∑5(2 1 0) grain boundary in copper, these methods achieve a converged residence time, accounting for the full set of kinetically relevant events for this off-lattice system, with calculable uncertainty.