Despite governing heat management in any realistic device, the microscopic mechanisms of heat transport in all-solid-state electrolytes are poorly known: existing calculations, all based on simplistic semi-empirical models, are unreliable for superionic conductors and largely overestimate their thermal conductivity. In this work, we deploy a combination of state-of-the-art methods to calculate the thermal conductivity of a prototypical Li-ion conductor, the Li3ClO antiperovskite. By leveraging ab initio, machine learning, and force-field descriptions of interatomic forces, we are able to reveal the massive role of anharmonic interactions and diffusive defects on the thermal conductivity and its temperature dependence, and to eventually embed their effects into a simple rationale which is likely applicable to a wide class of ionic conductors.

Temperature- and vacancy-concentration-dependence of heat transport in Li3ClO from multi-method numerical simulations / Pegolo, Paolo; Baroni, Stefano; Grasselli, Federico. - In: NPJ COMPUTATIONAL MATERIALS. - ISSN 2057-3960. - 8:1(2022), pp. 1-9. [10.1038/s41524-021-00693-4]

Temperature- and vacancy-concentration-dependence of heat transport in Li3ClO from multi-method numerical simulations

Paolo Pegolo;Stefano Baroni;Federico Grasselli
2022-01-01

Abstract

Despite governing heat management in any realistic device, the microscopic mechanisms of heat transport in all-solid-state electrolytes are poorly known: existing calculations, all based on simplistic semi-empirical models, are unreliable for superionic conductors and largely overestimate their thermal conductivity. In this work, we deploy a combination of state-of-the-art methods to calculate the thermal conductivity of a prototypical Li-ion conductor, the Li3ClO antiperovskite. By leveraging ab initio, machine learning, and force-field descriptions of interatomic forces, we are able to reveal the massive role of anharmonic interactions and diffusive defects on the thermal conductivity and its temperature dependence, and to eventually embed their effects into a simple rationale which is likely applicable to a wide class of ionic conductors.
2022
8
1
1
9
24
10.1038/s41524-021-00693-4
https://arxiv.org/abs/2111.14976
Pegolo, Paolo; Baroni, Stefano; Grasselli, Federico
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.11767/133110
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