Predicting Glass-to-Glass and Liquid-to-Liquid Phase Transitions in Water using Classical Nucleation Temperature

TL;DR

This paper develops a classical nucleation model to predict phase transitions in water, including glass-to-glass and liquid-to-liquid, aligning with experimental thermodynamic observations.

Contribution

It introduces a comprehensive nucleation equation incorporating enthalpy differences, pressure, and excess, to predict phase transition temperatures in water.

Findings

Predicts double glass transition temperatures.

Identifies a first-order transition line between fragile and strong liquids.

Aligns thermodynamic predictions with experimental data.

Abstract

Glass-to-glass and liquid-to-liquid phase transitions are observed in bulk and confined water, with or without applied pressure. They result from the competition of two liquid phases separated by an enthalpy difference depending on temperature. The classical nucleation equation of these phases is completed by this quantity existing at all temperatures, a pressure contribution, and an enthalpy excess. This equation leads to two homogeneous nucleation temperatures in each liquid phase, the first one being the formation temperature of an ordered liquid phase below the melting temperature and the second one corresponding to the overheating temperature. Thermodynamic properties, double glass transition temperatures, sharp enthalpy and volume changes are predicted in agreement with experimental results. The first-order transition line between fragile and strong liquids joins two critical points. Glass phase above its transition temperature becomes ordered liquid phase disappearing at a first-order transition temperature at low pressure and at a temperature larger than the melting temperature at high pressure.