基于蒙特卡罗模拟的离子导体热力学与动力学特性

刘金平, 蒲博伟, 邹喆乂, 李铭清, 丁昱清, 任元, 罗亚桥, 李杰, 李亚捷, 王达, 何冰, 施思齐

Investigating thermodynamic and kinetic properties of ionic conductors via Monte Carlo simulation

Jinping LIU, Bowei PU, Zheyi ZOU, Mingqing LI, Yuqing DING, Yuan REN, Yaqiao LUO, Jie LI, Yajie LI, Da WANG, Bing HE, Siqi SHI

图12 几个KMC计算过程的对比：(a) LLZO的通道连接关系与仅考虑几何效应下的离子电导率示意图[20]；(b) BVSE计算得到的离子输运通道与通过KMC模拟得到的电导率与实验值的比较。实心蓝色曲线和填充圆表示KMC所模拟的电导率。实红线表示有效计算的电导率(来自高温KMC模拟)，虚线表示对较低温度下离子电导率的推断。三角形绿色曲线表示实验电导率数据[8]；(c) 几种典型的离子排布状态与基于局域结构团簇展开的KMC计算得到的离子扩散系数[46]

Fig. 12 Comparison of several KMC calculation processes: (a) schematic diagram of channel connection and ionic conductivity of LLZO only considering geometric effects; (b) ionic transport channel calculated by BVSE and the comparison of ion conductivity calculated by KMC with experimental observation. Solid blue curves and filled circles represent the ion conductivity simulated by KMC. The solid red line represents the ion conductivity effectively calculated (from the KMC simulation at high temperatures) and the dashed line represents the inferred ionic conductivity at lower temperatures. The triangular green curve represents the experimental observation conductivity; (c) several typical ion distribution states and the ion diffusion coefficient calculated by KMC based on cluster expansion[46]