Dynamically correlated regions and configurational entropy in supercooled liquids

TL;DR

This paper investigates the relationship between dynamically correlated regions and configurational entropy in supercooled liquids, revealing a universal link to relaxation times and supporting theoretical models of the glass transition.

Contribution

It introduces a method to quantify domain sizes in supercooled liquids and demonstrates their inverse relationship with configurational entropy at the glass transition.

Findings

Relaxation time is a universal function of configurational entropy.

Domain size and entropy are anti-correlated at the glass transition.

Data supports the Adam-Gibbs and Random First Order Theory predictions.

Abstract

When a liquid is cooled below its melting temperature, if crystallization is avoided, it forms a glass. This phenomenon, called glass transition, is characterized by a marked increase of viscosity, about 14 orders of magnitude, in a narrow temperature interval. The microscopic mechanism behind the glass transition is still poorly understood. However, recently, great advances have been made in the identification of cooperative rearranging regions, or dynamical heterogeneities, i.e. domains of the liquid whose relaxation is highly correlated. The growth of the size of these domains is now believed to be the driving mechanism for the increase of the viscosity. Recently a tool to quantify the size of these domains has been proposed. We apply this tool to a wide class of materials to investigate the correlation between the size of the heterogeneities and their configurational entropy, i.e. the number of states accessible to a correlated domain. We find that the relaxation time of a given system, apart from a material dependent pre-factor, is a universal function of the configurational entropy of a correlated domain. As a consequence, we find that at the glass transition temperature, the size of the domains and the configurational entropy per unit volume are anti-correlated, as originally predicted by the Adam-Gibbs theory. Finally, we use our data to extract some exponents defined in the framework of the Random First Order Theory, a recent quantitative theory of the glass transition.