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

Area of Science:

• Materials Science
• Computational Chemistry
• Spectroscopy

Background:

• X-ray absorption spectroscopy (XAS) is crucial for characterizing material properties.
• Understanding the local chemical environment of atoms is key in materials development.
• Lithium thiophosphates are important in energy storage applications.

Purpose of the Study:

• To develop a comprehensive database of sulfur K-edge XAS spectra for lithium thiophosphate materials.
• To establish correlations between spectral features and local atomic structures.
• To provide a valuable resource for the analysis of sulfide-based solid electrolytes.

Main Methods:

• Atomic structures of crystalline and amorphous lithium thiophosphates were used as input.
• Simulations were performed using the excited electron and core-hole pseudopotential approach.
• The Vienna Ab initio Simulation Package (VASP) was employed for calculations.

Main Results:

• A database of 2681 S K-edge XAS spectra for 66 distinct crystalline and glassy models was generated.
• This represents the most extensive collection of first-principles computational XAS spectra for these materials.
• The database facilitates the identification of different sulfur species based on their coordination and short-range order.

Conclusions:

• The developed XAS database is a significant resource for researchers studying sulfide-based solid electrolytes.
• It enables spectral fingerprinting and matching with experimental data.
• The data supports the development of machine learning models for materials characterization.