Slow relaxations and stringlike jump motions in fragile glass-forming liquids: Breakdown of the Stokes-Einstein relation

Abstract

We perform molecular dynamics simulation on a glass-forming liquid binary mixture with the soft-core potential in three dimensions. We investigate crossover of the configuration changes caused by stringlike jump motions. With lowering the temperature $T$, the motions of the particles composing strings become larger in sizes and displacements, while those of the particles surrounding strings become smaller. Then, the contribution of the latter to time-correlation functions tends to be long-lived as $T$ is lowered. As a result, the relaxation time $τ_α$ and the viscosity $η$ grow more steeply than the inverse diffusion constant $D^{-1}$ at low $T$, leading to breakdown of the Stokes-Einstein relation. At low $T$, the diffusion occurs as activation processes and may well be described by short-time analysis of rare jump motions with broken bonds and large displacements. Some characteristic features of the van Hove self-correlation function arise from escape jumps over high potential barriers.