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Origin of Intrinsically Low Thermal Conductivity in a Garnet-Type Solid Electrolyte: Linking Lattice and Ionic Dynamics with Thermal Transport

Yitian Wang1,*, Yaokun Su2,*, Jesús Carrete3,*, Huanyu Zhang4,5, Nan Wu6, Yutao Li6, Hongze Li6, Jiaming He6, Youming Xu1 et al.

Shucheng Guo1, Qingan Cai7, Douglas L. Abernathy8, Travis Williams8, Kostiantyn V. Kravchyk4,5, Maksym V. Kovalenko4,5, Georg K.H. Madsen9, Chen Li2,7, and Xi Chen1,†

  • *These authors contributed equally to this work.
  • †Contact author: xichen@ucr.edu
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PRX Energy 4, 033004 – Published 17 July, 2025

DOI: https://doi.org/10.1103/6wj2-kzhh

Abstract

Understanding thermal transport in solid electrolytes is essential for improving the performance, reliability, and safety of all-solid-state batteries. Garnet-type lithium-ion conductors are promising candidates for solid electrolytes, yet their thermal-transport mechanisms remain poorly understood. Here, we connect the lattice and ion dynamics of single-crystal garnet-type Li6.5La3Zr1.5Ta0.5O12 to its intrinsically low thermal conductivity. Our study reveals that the single crystals grown by the floating-zone method exhibit remarkably low glasslike thermal conductivity. Using first-principles calculations and inelastic-neutron-scattering measurements, we identify both the acoustic and numerous optical phonon modes, which stem from the complex crystal structure of the material. Notably, a low-energy optical branch exhibits an avoided crossing with acoustic phonons near 7 meV. These optical modes can enhance the scattering of heat-carrying acoustic phonons and reduce thermal conductivity. Furthermore, the calculated Grüneisen parameters are large, especially for the vibrational modes around 6 meV, indicating strong anharmonicity, with a noticeable contribution from lithium-ion vibrations. A two-channel thermal-transport model is employed to describe the weak temperature dependence of the thermal conductivity, which can be attributed to the substantial contribution of diffuson transport facilitated by the abundance of optical phonons and intrinsic anharmonicity. These results offer valuable insights into the thermal transport in a broad class of ionic conductors of interest for energy conversion and storage applications.

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Popular Summary

Thermal management stands as a critical challenge in developing next-generation all-solid-state batteries, directly impacting their safety, efficiency, and longevity. Current battery technologies face limitations due to incomplete understanding of heat transport within solid electrolytes, particularly at the atomic scale where crucial ionic movements occur. Here the authors employ advanced neutron scattering techniques and theoretical calculations to explore the fundamental thermal transport mechanisms in a garnet-type lithium ion conductor Li6.5La3Zr1.5Ta0.5O12, a promising solid electrolyte material for all-solid-state batteries. The findings reveal that this material has an intrinsically low thermal conductivity, which can be attributed to unusual lattice and ion dynamics. By understanding how heat moves through these materials at the atomic level, better thermal management strategies for solid-state batteries can be developed.

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PRX Energy 4, 033004– Published 17 July, 2025
  • Received 30 January 2025
  • Revised 1 May 2025
  • Accepted 23 June 2025
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