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.

中文翻译：

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网格上的恒电位模拟

恒定电位集合中的分子动力学模拟是研究下一代储能设备充电机制的越来越重要的工具。我们通过引入专为处理 CPM 中的长程相互作用而设计的粒子 - 粒子 - 粒子 - 网格求解器，提出了一种在采用恒定电位法 (CPM) 的模拟中计算静电相互作用的高效方法。此外，我们提供的证据表明，如果偶极子校正项（通常用于具有类似平板的几何形状的模拟中）也要在 CPM 中使用，则必须谨慎使用。结果表明，通过在给定外部电位下的电极电荷评估中强制执行电荷中性条件，可以避免因使用偶极校正项而产生的伪影。