Simulated sulfur K-edge X-ray absorption spectroscopy database of lithium thiophosphate solid electrolytes

TL;DR

This paper presents a comprehensive database of sulfur K-edge X-ray absorption spectra for lithium thiophosphate electrolytes, generated through first-principles simulations, facilitating spectral analysis and material characterization.

Contribution

It introduces the largest computational XAS spectra database for lithium thiophosphates, enabling better correlation of spectral features with local chemical environments.

Findings

Largest collection of simulated S K-edge XAS spectra for lithium thiophosphates

Database includes 2681 spectra for 66 structures

Open access via Materials Cloud for research and machine learning

Abstract

X-ray absorption spectroscopy (XAS) is a premier technique for materials characterization, providing key information about the local chemical environment of the absorber atom. In this work, we develop a database of sulfur K-edge XAS spectra of crystalline and amorphous lithium thiophosphate materials based on the atomic structures reported in Chem. Mater., 34, 6702 (2022). The XAS database is based on simulations using the excited electron and core-hole pseudopotential approach implemented in the Vienna Ab initio Simulation Package. Our database contains 2681 S K-edge XAS spectra for 66 crystalline and glassy structure models, making it the largest collection of first-principles computational XAS spectra for glass/ceramic lithium thiophosphates to date. This database can be used to correlate S spectral features with distinct S species based on their local coordination and short-range ordering in sulfide-based solid electrolytes. The data is openly distributed via the Materials Cloud, allowing researchers to access it for free and use it for further analysis, such as spectral fingerprinting, matching with experiments, and developing machine learning models.