中国物理B ›› 2024, Vol. 33 ›› Issue (8): 86601-086601.doi: 10.1088/1674-1056/ad5d9a

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Comparative study of nudged elastic band and molecular dynamics methods for diffusion kinetics in solid-state electrolytes

Aming Lin(林啊鸣)1,2, Jing Shi(石晶)3, Su-Huai Wei(魏苏淮)4,†, and Yi-Yang Sun(孙宜阳)1,2,‡   

  1. 1 State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China;
    2 Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;
    3 Department of Physics, Jiangxi Normal University, Nanchang 330022, China;
    4 Eastern Institute of Technology, Ningbo 315200, China
  • 收稿日期:2024-06-20 修回日期:2024-06-20 出版日期:2024-08-15 发布日期:2024-07-23
  • 通讯作者: Su-Huai Wei, Yi-Yang Sun E-mail:suhuaiwei@eitech.edu.cn;yysun@mail.sic.ac.cn
  • 基金资助:
    Project supported by the National Natural Science Foundation of China (Grant Nos. 12164019, 11991060, 12088101, and U1930402) and the Natural Science Foundation of Jiangxi Province of China (Grant No. 20212BAB201017).

Comparative study of nudged elastic band and molecular dynamics methods for diffusion kinetics in solid-state electrolytes

Aming Lin(林啊鸣)1,2, Jing Shi(石晶)3, Su-Huai Wei(魏苏淮)4,†, and Yi-Yang Sun(孙宜阳)1,2,‡   

  1. 1 State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China;
    2 Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;
    3 Department of Physics, Jiangxi Normal University, Nanchang 330022, China;
    4 Eastern Institute of Technology, Ningbo 315200, China
  • Received:2024-06-20 Revised:2024-06-20 Online:2024-08-15 Published:2024-07-23
  • Contact: Su-Huai Wei, Yi-Yang Sun E-mail:suhuaiwei@eitech.edu.cn;yysun@mail.sic.ac.cn
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Grant Nos. 12164019, 11991060, 12088101, and U1930402) and the Natural Science Foundation of Jiangxi Province of China (Grant No. 20212BAB201017).

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摘要： Considerable efforts are being made to transition current lithium-ion and sodium-ion batteries towards the use of solid-state electrolytes. Computational methods, specifically nudged elastic band (NEB) and molecular dynamics (MD) methods, provide powerful tools for the design of solid-state electrolytes. The MD method is usually the choice for studying the materials involving complex multiple diffusion paths or having disordered structures. However, it relies on simulations at temperatures much higher than working temperature. This paper studies the reliability of the MD method using the system of Na diffusion in MgO as a benchmark. We carefully study the convergence behavior of the MD method and demonstrate that total effective simulation time of 12 ns can converge the calculated diffusion barrier to about 0.01 eV. The calculated diffusion barrier is 0.31 eV from both methods. The diffusion coefficients at room temperature are $4.3\times 10^{-9}$ cm$^2\cdot$s$^{-1}$ and $2.2\times 10^{-9}$ cm$^2\cdot$s$^{-1}$, respectively, from the NEB and MD methods. Our results justify the reliability of the MD method, even though high temperature simulations have to be employed to overcome the limitation on simulation time.

关键词: nudged elastic band method, molecular dynamics, solid electrolyte, ion transport, density functional theory

Abstract: Considerable efforts are being made to transition current lithium-ion and sodium-ion batteries towards the use of solid-state electrolytes. Computational methods, specifically nudged elastic band (NEB) and molecular dynamics (MD) methods, provide powerful tools for the design of solid-state electrolytes. The MD method is usually the choice for studying the materials involving complex multiple diffusion paths or having disordered structures. However, it relies on simulations at temperatures much higher than working temperature. This paper studies the reliability of the MD method using the system of Na diffusion in MgO as a benchmark. We carefully study the convergence behavior of the MD method and demonstrate that total effective simulation time of 12 ns can converge the calculated diffusion barrier to about 0.01 eV. The calculated diffusion barrier is 0.31 eV from both methods. The diffusion coefficients at room temperature are $4.3\times 10^{-9}$ cm$^2\cdot$s$^{-1}$ and $2.2\times 10^{-9}$ cm$^2\cdot$s$^{-1}$, respectively, from the NEB and MD methods. Our results justify the reliability of the MD method, even though high temperature simulations have to be employed to overcome the limitation on simulation time.

Key words: nudged elastic band method, molecular dynamics, solid electrolyte, ion transport, density functional theory

中图分类号:  (Diffusion of impurities ?)

  • 66.30.J-
71.15.Mb (Density functional theory, local density approximation, gradient and other corrections)