Density dependence of relaxation dynamics in glass formers, and the dependence of their fragility on the softness of inter-particle interactions

Abstract

Fragility, quantifying the rapidity of variation of relaxation times, is analysed for a series of model glass formers, which differ in the softness of their interparticle interactions. In an attempt to rationalize experimental observations in colloidal suspensions that softer interactions lead to stronger (less fragile) glass formers, we study the variation of relaxation dynamics with density, rather than temperature, as a control parameter. We employ density-temperature scaling, analyzed in recent studies, to address the question. We find that while employing inverse density in place of temperature leads to the conclusion that softer interactions lead to stronger behaviour, the use of scaled variables involving temperature and density lead to the opposite conclusion, similarly to earlier investigations where temperature variation of relaxation dynamics was analysed for the same systems. We rationalize our results by considering the Adam-Gibbs (AG) fragility, which incorporates the density dependence of the configurational entropy and an activation energy that may arise from other properties of a glass former. Within the framework of the Adam-Gibbs relation, by employing density temperature scaling for the analysis, we find that softer particles make more fragile glasses, as deduced from dynamical quantities, which is found to be consistent with the Adam-Gibbs fragility. We analyse fragility, which quantifies the rapidity of variation of relaxation times, using density as the control variable, for model glass formers with varying softness of interactions. Using scaled variables, we find – and rationalise thermodynamically by computing configurational entropy – that fragility increases with softness, contrary to previous work.