Abstract Surface properties play an important role in the application of antiperovskite Li3OCl as a promising solid-state electrolyte in all-solid-state Li-metal batteries. In this paper, we systematically investigated the stability, geometric structure, electronic properties and Li-ion mobility of a Li3OCl (1 0 0) surface using first-principles density functional theory calculations. Several geometric structure models were considered with different low Miller indices to obtain the most stable surface structure. The surface energies revealed that the Li3OCl (1 0 0) surface with Li- and Cl-termination on both sides was the most stable configuration, and the stability of the configuration was further verified by calculating the atomic relaxation and electronic properties. In addition, four types of point defects in the Li3OCl (1 0 0) surface were considered to study the Li-ion mobilities on the surface, and the results from calculating the defect formation energies and migration energy barriers showed that interstitial Li with a migration energy barrier of 0.086 eV is the most important carrier at the surface. The results provide fundamental insights into Li3OCl surface properties and Li-ion mobility at the surface.

中文翻译：

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反钙钛矿超离子导体Li3OCl(100)表面结构、电子和锂离子迁移率的第一性原理研究

摘要 表面性质在反钙钛矿 Li3OCl 作为一种有前途的固态电解质在全固态锂金属电池中的应用中起着重要作用。在本文中，我们使用第一性原理密度泛函理论计算系统地研究了 Li3OCl (1 0 0) 表面的稳定性、几何结构、电子性质和锂离子迁移率。考虑了几种具有不同低米勒指数的几何结构模型，以获得最稳定的表面结构。表面能表明，Li3OCl (1 0 0) 表面的Li-和Cl-终止是最稳定的构型，通过计算原子弛豫和电子性质进一步验证了该构型的稳定性。此外，Li3OCl (1 0 0) 表面的四种点缺陷被考虑用来研究表面上的锂离子迁移率，计算缺陷形成能和迁移能垒的结果表明，间隙锂的迁移能垒为0.086 eV 是表面最重要的载流子。结果提供了对 Li3OCl 表面特性和表面锂离子迁移率的基本见解。