Understanding the connection between chemistry,structure,and ion migration in solid-state electrolytes(SSEs)is vital to enable safer,more efficient all-solid-state batteries and other advanced electrochemical devices....Understanding the connection between chemistry,structure,and ion migration in solid-state electrolytes(SSEs)is vital to enable safer,more efficient all-solid-state batteries and other advanced electrochemical devices.Atomistic simulations offer invaluable access to the intricacies of this connection.However,extracting meaningful insights often requires detailed crystallographic knowledge and painstaking examination of simulation trajectories.This work introduces a densitybased unsupervised method that accurately and efficiently identifies and categorizes crystallographic sites while providing a robust framework for analyzing ionic transport from ab initio and classic molecular dynamics simulations.Unlike previous schemes,it needs no prior structural knowledge and is adaptable to various material systems.Our approach,implemented in the open-source CrySF package and validated on representative SSEs such as Li_(7)La_(3)Zr_(2)O_(12)(a garnet),Li_(10)GeP_(2)S_(12)(a sulfide),and Li6PS5Br(an argyrodite),effectively analyzes the interplay between structure,ionic mobility and collective migration phenomena,offering a powerful tool to accelerate the development of highperformance SSEs.展开更多
基金supported by MICIU/AEI/10.13039/501100011033 and by ERDF A way for Europe under Grant PID2022-136585NB-C22by the Basque Government through ELKARTEK Program under Grants KK-2024/00062, KK-2023/00017 and through the BERC 2022-2025 program+3 种基金We acknowledge the financial support by the Ministry of Science and Innovation through BCAM Severo Ochoa accreditation CEX2021-001142-S / MICIU/ AEI / 10.13039/501100011033 and “PLAN COMPLEMENTARIO MATERIALES AVANZADOS 2022 -2025”, PROYECTO \({{\rm{N}}}^{\underline{{\rm{o}}}}\):1101288The authors acknowledge the financial support received from the grant BCAM-IKUR, funded by the Basque Government by the IKUR Strategy and by the European Union NextGenerationEU/PRTRM.R.B. acknowledges the support from Diputación Foral de Bizkaia through MODEL2RESISTthe Spanish research agency through RYC2022-036500-I. This work has been possible thanks to the support of the computing infrastructure of the i2BASQUE academic network, Barcelona Supercomputing Center (RES, QHS-2024-2-0032), DIPC Computer Center and the technical and human support provided by IZO-SGI SGIker of UPV/EHU.
文摘Understanding the connection between chemistry,structure,and ion migration in solid-state electrolytes(SSEs)is vital to enable safer,more efficient all-solid-state batteries and other advanced electrochemical devices.Atomistic simulations offer invaluable access to the intricacies of this connection.However,extracting meaningful insights often requires detailed crystallographic knowledge and painstaking examination of simulation trajectories.This work introduces a densitybased unsupervised method that accurately and efficiently identifies and categorizes crystallographic sites while providing a robust framework for analyzing ionic transport from ab initio and classic molecular dynamics simulations.Unlike previous schemes,it needs no prior structural knowledge and is adaptable to various material systems.Our approach,implemented in the open-source CrySF package and validated on representative SSEs such as Li_(7)La_(3)Zr_(2)O_(12)(a garnet),Li_(10)GeP_(2)S_(12)(a sulfide),and Li6PS5Br(an argyrodite),effectively analyzes the interplay between structure,ionic mobility and collective migration phenomena,offering a powerful tool to accelerate the development of highperformance SSEs.
