Slow dynamics, dynamic heterogeneities, and fragility of supercooled liquids confined in random media

Abstract

Using molecular dynamics simulations, we study the slow dynamics of supercooled liquids confined in a random matrix of immobile obstacles. We study the dynamical crossover from glass-like to Lorentz-gas-like behavior in terms of the density correlation function, the mean square displacement, the nonlinear dynamic susceptibility, the non-Gaussian parameter, and the fragility. We find the cooperative and spatially heterogeneous dynamics to be suppressed as the obstacle density increases, leading to a more Arrhenius-like behavior in the temperature dependence of the relaxation time. Our findings are qualitatively consistent with the results of recent experimental and numerical studies for various classes of spatially heterogeneous systems. We also investigate the dependence of the dynamics of mobile particles on the protocol used to generate the random matrix. A re-entrant transition from the arrested phase to the liquid phase as the mobile particle density increases is observed for a class of protocols. This re-entrance is explained in terms of the distribution of the volume of the voids that are available to the mobile particles. © 2011 IOP Publishing Ltd.