The Glass Transition and Liquid-Gas Spinodal Boundaries of Metastable Liquids

TL;DR

This paper investigates the relationship between the glass transition and liquid-gas spinodal boundaries in metastable liquids using semi-analytical methods and liquid state theory, revealing their intersection at finite temperature.

Contribution

It introduces a semi-analytical approach combining liquid state theory and first-principles to study stability boundaries in glass-forming liquids, advancing prior simulation-based work.

Findings

Boundaries intersect at a finite temperature

Methodology combines liquid state theory with first-principles calculations

Results are consistent with previous simulation studies

Abstract

A liquid can exist under conditions of thermodynamic stability or metastability within boundaries defined by the liquid-gas spinodal and the glass transition line. The relationship between these boundaries has been investigated previously using computer simulations, the energy landscape formalism, and simplified model calculations. We calculate these stability boundaries semi-analytically for a model glass forming liquid, employing accurate liquid state theory and a first-principles approach to the glass transition. These boundaries intersect at a finite temperature, consistent with previous simulation-based studies.