Constant potential simulations on a mesh

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. (c) 2021 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).

Automated summary

This study presents an efficient approach for computing electrostatic interactions in constant potential ensemble simulations and warns about the cautious use of a dipole correction term. By enforcing a charge neutrality condition during the evaluation of electrode charges at a given external potential, artifacts arising from the dipole correction term can be avoided.