Structure of glassy lithium sulfate films sputtered in nitrogen (LISON): Insight from Raman spectroscopy and ab initio calculations

TL;DR

This study combines Raman spectroscopy and ab initio calculations to analyze nitrogen-incorporated lithium sulfate glass films sputtered in nitrogen, revealing how nitrogen affects their structure and prevents crystallization.

Contribution

It provides new insights into the atomic structure of nitrogen-doped lithium sulfate glasses using combined experimental and computational methods.

Findings

Nitrogen incorporation alters the glass structure.

Agreement achieved by replacing oxygen with nitrogen in models.

Nitrogen bonding prevents crystallization.

Abstract

Raman spectra of thin solid electrolyte films obtained by sputtering a lithium sulfate target in nitrogen plasma are measured and compared to ab initio electronic structure calculations for clusters composed of 28 atoms. Agreement between measured and calculated spectra is obtained when oxygen atoms are replaced by nitrogen atoms and when the nitrogen atoms form bonds with each other. This suggests that the incorporation of nitrogen during the sputtering process leads to structures in the film, which prevent crystallization of these thin film salt glasses.