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Thermal transport of Li₃PS₄ solid electrolytes with ab initio accuracy

Davide Tisi1*, Federico Grasselli1, Lorenzo Gigli1, Michele Ceriotti1*

1 Laboratory of Computational Science and Modeling (COSMO), Institute of Materials, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Corresponding authors emails: davide.tisi@epfl.ch, michele.ceriotti@epfl.ch
DOI10.24435/materialscloud:nv-1g [version v1]

Publication date: Apr 16, 2024

How to cite this record

Davide Tisi, Federico Grasselli, Lorenzo Gigli, Michele Ceriotti, Thermal transport of Li₃PS₄ solid electrolytes with ab initio accuracy, Materials Cloud Archive 2024.57 (2024), https://doi.org/10.24435/materialscloud:nv-1g


The vast amount of computational studies on electrical conduction in solid-state electrolytes is not mirrored by comparable efforts addressing thermal conduction, which has been scarcely investigated despite its relevance to thermal management and (over)heating of batteries. The reason for this lies in the complexity of the calculations: on one hand, the diffusion of ionic charge carriers makes lattice methods formally unsuitable due to the lack of equilibrium atomic positions needed for normal-mode expansion. On the other hand, the prohibitive cost of large-scale molecular dynamics (MD) simulations of heat transport in large systems at ab initio levels has hindered the use of MD-based methods. In this work, we leverage recently developed machine-learning potentials targeting different ab initio functionals (PBEsol, r2SCAN, PBE0) and a state-of-the-art formulation of the Green-Kubo theory of heat transport in multicomponent systems to compute the thermal conductivity of a promising solid-state-electrolyte, Li3PS4, in all its polymorphs (α, β and γ). By comparing MD estimates with lattice methods on the low-temperature, non-diffusive γ-Li3PS4, we highlight strong anharmonicities and negligible nuclear quantum effects, hence further justifying MD-based methods even for non-diffusive phases. Finally, for the ion-conducting α and β phases, where the multicomponent Green-Kubo MD approach is mandatory, our simulations indicate a weak temperature dependence of the thermal conductivity, a glass-like behavior due to the effective local disorder characterizing these Li-diffusing phases.

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lab-cosmo machine learning solid-state-electrolytes thermal transport EPFL MARVEL Swissuniversities MaX SNSF

Version history:

2024.57 (version v1) [This version] Apr 16, 2024 DOI10.24435/materialscloud:nv-1g