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Reconstructions and Dynamics of β-Lithium Thiophosphate Surfaces

Hanna Türk, Davide Tisi, and Michele Ceriotti*

  • *Contact author: michele.ceriotti@epfl.ch
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PRX Energy 4, 033010 – Published 26 August, 2025

DOI: https://doi.org/10.1103/5hf9-hlj6

Abstract

Lithium thiophosphate (LPS) is a promising solid electrolyte for next-generation lithium-ion batteries due to its superior energy storage, high ionic conductivity, and low-flammability properties. Despite its potential, the high reactivity of LPS with common contaminants such as atmospheric water, preparation solvents, and electrode materials poses significant challenges for commercialization. The lack of understanding regarding the structure, morphology, and chemical behavior of the surface of LPS slows down the search for solutions to these issues. Here, we utilize a machine-learning interatomic potential to achieve a fundamental atomistic understanding of the mechanical and chemical properties of the β-Li3PS4 surfaces. Employing molecular-dynamics simulations, we identify relevant complexions formed by surface reconstructions, determine their surface energies, and compute the Wulff shape of β-LPS. The most stable complexions exhibit properties distinctly different from the bulk, including amorphization, increased density, decreased conductivity, and large deformation of the structural building blocks. We demonstrate that these surfaces are not static but undergo significant dynamical activity at room temperature, which is clearly identified by an analysis featuring a time-averaged structural descriptor. Finally, we examine the changes of the electronic structure induced by the surface complexions as well as their effect on the reaction enthalpy with water, which provides us with details on changes in surface reactivity and active sites, underlining the importance of investigating surface complexions under realistic conditions.

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Popular Summary

Lithium thiophosphate (LPS) is a promising solid electrolyte for next-generation lithium-ion batteries. However, its high reactivity with moisture, solvents, and electrode materials hinders its development as a mainstream technology. To address this challenge, this study used machine-learning-driven molecular dynamics simulations to investigate the surfaces of β-Li3PS4, a crystalline form of LPS with high conductivity. The authors identify dynamic surface reconstructions, known as complexions, that differ vastly from the bulk material and the ideal crystallographic surface in their structure, density, conductivity, electronic properties and chemical reactivity. These complexions are not static but undergo continual changes that affect their reactivity and stability. The authors’ analysis of the electronic structure of these complexions highlights how surface behavior influences chemical activity and the temporal evolution of reactive sites with and without exposure to water. The findings provide critical insights into the surface properties of LPS and offer a solid foundation for improving its stability and integration in the next generation of solid-state batteries.

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PRX Energy 4, 033010– Published 26 August, 2025
  • Received 15 April 2025
  • Revised 17 July 2025
  • Accepted 29 July 2025
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