Deep potential generation scheme and simulation protocol for the Li10GeP2S12-type superionic conductors
- 6 March 2021
- journal article
- research article
- Published by AIP Publishing in The Journal of Chemical Physics
- Vol. 154 (9), 094703
- https://doi.org/10.1063/5.0041849
Abstract
Solid-state electrolyte materials with superior lithium ionic conductivities are vital to the next-generation Li-ion batteries. Molecular dynamics could provide atomic scale information to understand the diffusion process of Li-ion in these superionic conductor materials. Here, we implement the deep potential generator to set up an efficient protocol to automatically generate interatomic potentials for Li10GeP2S12-type solid-state electrolyte materials (Li10GeP2S12, Li10SiP2S12, and Li10SnP2S12). The reliability and accuracy of the fast interatomic potentials are validated. With the potentials, we extend the simulation of the diffusion process to a wide temperature range (300 K-1000 K) and systems with large size (similar to 1000 atoms). Important technical aspects such as the statistical error and size effect are carefully investigated, and benchmark tests including the effect of density functional, thermal expansion, and configurational disorder are performed. The computed data that consider these factors agree well with the experimental results, and we find that the three structures show different behaviors with respect to configurational disorder. Our work paves the way for further research on computation screening of solid-state electrolyte materials.Funding Information
- National Natural Science Foundation of China (21861132015, 21991150, 21991151, 91745103, 22021001, 11871110)
- National Key Research and Development Program of China (2017YFB0102000, 2016YFB0201200, 2016YFB0201203)
- ONR Grant (N00014-13-1-0338)
- DOE award (DE-SC0019394)
- Beijing Academy of Artificial Intelligence
This publication has 87 references indexed in Scilit:
- Phase stability, electrochemical stability and ionic conductivity of the Li10±1MP2X12(M = Ge, Si, Sn, Al or P, and X = O, S or Se) family of superionic conductorsEnergy & Environmental Science, 2013
- Generalized Neural-Network Representation of High-Dimensional Potential-Energy SurfacesPhysical Review Letters, 2007
- Toward reliable density functional methods without adjustable parameters: The PBE0 modelThe Journal of Chemical Physics, 1999
- From ultrasoft pseudopotentials to the projector augmented-wave methodPhysical Review B, 1999
- Rationale for mixing exact exchange with density functional approximationsThe Journal of Chemical Physics, 1996
- Projector augmented-wave methodPhysical Review B, 1994
- Ionic conductivity of and phase transition in lithium thiophosphate Li3PS4Solid State Ionics, 1984
- The haven ratio in fast ionic conductorsSolid State Ionics, 1982
- Superionic conductors: Transitions, structures, dynamicsPhysics Reports, 1979
- Self-Consistent Equations Including Exchange and Correlation EffectsPhysical Review B, 1965