Thermodynamic model for the glass transition: deeply supercooled liquids as mixtures of solid-like and liquid-like micro-regions

Hiroshi Matsuoka

Published 2011-10-06, updated 2012-10-16Version 3

For a deeply supercooled liquid just above its glass transition temperature, we present a simple thermodynamic model, where the deeply supercooled liquid is assumed to be a mixture of solid-like and liquid-like micro regions. The mole fraction of the liquid-like regions controls the thermodynamic properties of the supercooled liquid while that of the solid-like regions controls its relaxation time or viscosity. From the universal temperature dependence of the molar excess entropy for the deeply supercooled liquids, we derive the temperature dependence of the mole fraction of the liquid-like regions to obtain the universal temperature dependence of the relaxation time or the viscosity for the deeply supercooled liquids. A central parameter of our model is then shown to be a measure for the fragility of a supercooled liquid. We also suggest a way to test our physical picture of deeply supercooled liquids by means of molecular dynamics simulations of model liquids.