Amorphous Li–P–S materials have been widely used as solid-state electrolytes for all-solid-state batteries because of their high ionic conductivity (10^–4 to 10^–3 S cm^–1) as well as good synthetic accessibility and processability. Despite the potential of these materials, their amorphous structures have made it challenging to quantify the relation between the structure and conductivity. In this paper, we use ab initio molecular dynamics simulations to investigate the role of the local structure and density in determining the conductivity of amorphous Li–P–S structures with different polyanion units. We observe similar rates for Li-ion hopping regardless of the local P–S polyanion environment in these amorphous materials, indicating that the path connectivity at a larger length scale may be controlling the overall Li conductivity. This finding will serve as an important guideline in the continued development of amorphous solid electrolytes for advanced all-solid-state batteries.

中文翻译：

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非晶 Li-P-S 超离子导体中聚阴离子环境与离子电导率的弱相关性

^{非晶 Li-P-S 材料因其高离子电导率（10 –4}至 10 ^–3 S cm ^–1）而被广泛用作全固态电池的固态电解质。) 以及良好的合成可及性和加工性。尽管这些材料具有潜力，但它们的非晶结构使得量化结构和电导率之间的关系变得具有挑战性。在本文中，我们使用从头算分子动力学模拟来研究局部结构和密度在确定具有不同聚阴离子单元的非晶 Li-P-S 结构的电导率中的作用。无论这些无定形材料中的局部 P-S 聚阴离子环境如何，我们都观察到相似的锂离子跳跃速率，这表明较大长度尺度的路径连通性可能控制着整体锂电导率。这一发现将作为继续开发用于先进全固态电池的非晶态固体电解质的重要指南。