We describe an approach based on non-equilibrium molecular dynamics (NEMD) simulations to calculate the ionic mobility of solid ion conductors such as solid electrolytes from first-principles. The calculations are carried out in finite slabs of the material, where an electric field is applied and the dynamic response of the mobile ions is measured. We compare our results with those obtained from diffusion calculations, under the non-interacting ion approximation, and with experiment. This method is shown to provide good quantitative estimates for the ionic mobilities of two silver conductors, \(\alpha\)-AgI and \(\alpha\)-RbAg\(_4\)I\(_5\). In addition to being convenient and numerically robust, this method accounts for ion-ion correlations at a much lower computational cost than exact approaches.

我们描述了一种基于非平衡分子动力学 (NEMD) 模拟的方法，以根据第一性原理计算固体离子导体（例如固体电解质）的离子迁移率。计算是在有限的材料板中进行的，其中施加了电场并测量了移动离子的动态响应。我们将我们的结果与在非相互作用离子近似下通过扩散计算获得的结果进行比较，并与实验进行比较。这种方法被证明可以为两个银导体的离子迁移率提供良好的定量估计，\(\alpha\) -AgI 和\(\alpha\) -RbAg \(_4\) I \(_5\). 除了方便和数值稳健之外，该方法还以比精确方法低得多的计算成本来解释离子-离子相关性。