Accurate description of ion migration in solid-state ion conductors from machine-learning molecular dynamics

Takeru Miyagawa, Namita Krishnan, Manuel Grumet, Christian Reverón Baecker, Waldemar Kaiser, David A. Egger

Research output: Contribution to journalArticlepeer-review

1 Scopus citations


Solid-state ion conductors (SSICs) have emerged as a promising material class for electrochemical storage devices and novel compounds of this kind are continuously being discovered. High-throughout approaches that enable a rapid screening among the plethora of candidate SSIC compounds have been essential in this quest. While first-principles methods are routinely exploited in this context to provide atomic-level details on ion migration mechanisms, dynamic calculations of this type are computationally expensive and limit us in the time- and length-scales accessible during the simulations. Here, we explore the potential of recently developed machine-learning force fields for predicting different ion migration mechanisms in SSICs. Specifically, we systematically investigate three classes of SSICs that all exhibit complex ion dynamics including vibrational anharmonicities: AgI, a strongly disordered Ag+-conductor; Na3SbS4, a Na+ vacancy conductor; and Li10GeP2S12, which features concerted Li+ migration. Through systematic comparison with ab initio molecular dynamics data, we demonstrate that machine-learning molecular dynamics provides very accurate predictions of the structural and vibrational properties including the complex anharmonic dynamics in these SSICs. The ab initio accuracy of machine-learning molecular dynamics simulations at relatively low computational cost opens a promising path toward the rapid design of novel SSICs.

Original languageEnglish
Pages (from-to)11344-11361
Number of pages18
JournalJournal of Materials Chemistry A
Issue number19
StatePublished - 9 Apr 2024


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