Electronic Signature of the Intermediate Phase in Ge_xSe_{1-x} Glasses: A Joint Theoretical and Experimental Study

TL;DR

This study combines experimental XANES measurements and ab initio molecular dynamics modeling to identify and characterize the electronic signature of the intermediate phase in Ge_xSe_{1-x} glasses, enhancing understanding of their atomic structure.

Contribution

It provides the first joint experimental and theoretical evidence of the electronic signature of the intermediate phase in GeSe glasses, with atomistic models aligning with experimental data.

Findings

XANES detects an electronic signature of the intermediate phase.

Atomistic models reproduce composition-dependent structural features.

Models accurately represent the structure of GeSe glasses near the intermediate phase.

Abstract

Raman and calorimetric studies on Ge_xSe_{1-x} glasses have provided evidence for the existence of the intermediate phase (IP) in chalcogenide and other glasses. Here, we present X-Ray Absorption Near Edge Structure (XANES) measurements on germanium selenide glasses in the IP composition range, and detect an electronic signature of the IP. Ab initio molecular dynamics (MD) based models of these glasses are discussed, and an atomistic picture of the IP, based upon the models and available experiments is presented. We show that these models reproduce detailed composition-dependent structure in the XANES measurements, and otherwise appear to properly represent the structure of the GeSe glasses near the IP.