Constant potential simulations on a mesh

Abstract

Molecular dynamics simulations in a constant potential ensemble are an increasingly important tool to investigate charging mechanisms in next-generation energy storage devices. We present a highly efficient approach to compute electrostatic interactions in simulations employing a constant potential method (CPM) by introducing a particle–particle particle–mesh solver specifically designed for treating long-range interactions in a CPM. Moreover, we present evidence that a dipole correction term—commonly used in simulations with a slab-like geometry—must be used with caution if it is also to be used within a CPM. It is demonstrated that artifacts arising from the usage of the dipole correction term can be circumvented by enforcing a charge neutrality condition in the evaluation of the electrode charges at a given external potential.