Machine learning molecular dynamics simulation identifying weakly negative effect of polyanion rotation on Li-ion migration

作     者：Zhenming Xu Huiyu Duan Zhi Dou Mingbo Zheng Yixi Lin Yinghui Xia Haitao Zhao Yongyao Xia 

作者机构：College of Materials Science and TechnologyNanjing University of Aeronautics and Astronautics210016 NanjingChina Center for Intelligent and Biomimetic SystemsShenzhen Institutes of Advanced Technology(SIAT)Chinese Academy of Sciences(CAS)518055 ShenzhenChina Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsInstitute of New EnergyiChEm(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan University200433 ShanghaiChina 

出 版 物：《npj Computational Materials》 (计算材料学（英文）)

年 卷 期：2023年第9卷第1期

页      面：1276-1286页

核心收录：

学科分类：07[理学] 070203[理学-原子与分子物理] 0703[理学-化学] 0702[理学-物理学] 

基　　金：This work is supported by the Young Scientists Fund of the National Natural Science Foundation of China(22209074) the Fundamental Research Funds for the Central Universities(NO.NS2022059,NO.NS2021039) the Talent Research Startup Funds of Nanjing University of Aeronautics and Astronautics,the Jiangsu Funding Program for Excellent Postdoctoral Talent,and the Selected Funding for Scientific and Technological Innovation Projects for Overseas Students in Nanjing This work is partially supported by High Performance Computing Platform of Nanjing University of Aeronautics and Astronautics 

主　　题：rotation dynamics effect 

摘      要：Understanding the physical picture of Li ion transport in the current ionic conductors is quite essential to further develop lithium superionic conductors for solid-state *** traditional practice of directly extrapolating room temperature ion diffusion properties from the high-temperature(600 K)ab initio molecular dynamics simulations(AIMD)simulations by the Arrhenius assumption unavoidably cause some ***,the ultralong-time molecular dynamics simulation based on the machine-learning interatomic potentials(MLMD)is a more suitable tool to probe into ion diffusion events at low temperatures and simultaneously keeps the accuracy at the density functional theory ***,by the low-temperature MLMD simulations,the non-linear Arrhenius behavior of Li ion was found for Li3ErCl6,which is the main reason for the traditional AIMD simulation overestimating its ionic *** 1μs MLMD simulations capture polyanion rotation events in Li_(7)P_(3)S_(11) at room temperature,in which four[PS_(4)]^(3−)tetrahedra belonging to a part of the longer-chain[P_(2)S_(7)]4−group are noticed with remarkable rotational motions,while the isolated group[PS_(4)]^(3−)does not ***,no polyanion rotation is observed in Li10GeP_(2)S12,β-Li3PS_(4),Li3ErCl6,and Li3YBr6 at 300 K during 1μs simulation ***,the ultralong-time MLMD simulations demonstrate that not only there is no paddle-wheel effect in the crystalline Li_(7)P_(3)S_(11) at room temperature,but also the rotational[PS_(4)]^(3−)polyanion groups have weakly negative impacts on the overall Li ion *** ultralong-time MLMD simulations deepen our understanding of the relationship between the polyanion rotation and cation diffusion in ionic conductors at room environments.