Structural evolution in the aging process of supercooled colloidal liquids.

Abstract

When a liquid is rapidly quenched to a temperature below the glass-transition point, it is driven out of equilibrium; it then slowly relaxes to a (quasi)equilibrium state. This slow relaxation process is called aging. By definition, any glasses are inevitably in the process of aging and actually slowly evolving with time. Thus the study of aging phenomena is of fundamental importance for understanding not only the nonequilibrium nature of the glass transition, but also the stability of glassy materials. Here we consider aging after a rather shallow quench, for which a system is still able to reach (metastable) equilibrium. By using polydisperse colloidal liquids as a model, we show the validity of dynamical scaling that there is only one relevant length scale not only for a quasiequilibrium supercooled state but also for a nonequilibrium process of aging, which is reminiscent of dynamical critical phenomena. Our finding indicates that the aging toward (metastable) equilibrium may be regarded as the growth process of critical-like fluctuations of static order associated with low-free-energy configurations, further suggesting that this ordering is the origin of cooperative slow dynamics in the systems studied. The generality of this statement for other glass-forming systems remains for a future study.