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. We also visualize the particle motions at string formation taking place in a very short time.