Real space origin of temperature crossovers in supercooled liquids

Abstract

We show that the various crossovers between dynamical regimes observed in experiments and simulations of supercooled liquids can be explained in simple terms from the existence and statistical properties of dynamical heterogeneities. We confirm that dynamic heterogeneity is responsible for the slowing down of glass formers at temperatures well above the dynamic singularity T_c predicted by mode coupling theory. Our results imply that activated processes govern the long-time dynamics even in the temperature regime where they are neglected by mode-coupling theory. We show that alternative interpretations based on topographic properties of the potential energy landscape are complicated and inefficient ways of describing simple physical features which are naturally accounted for within our approach. We show in particular that the reported links between mode coupling and landscape singularities do not exist.

14 pages, 10 figures; v2: minor stylistic changes and refs added

References in corpus (11)

• Glassy dynamics of kinetically constrained models
• Geometrical explanation and scaling of dynamical heterogeneities in glass forming systems
• Coarse-grained microscopic model of glass formers
• Energy Barriers and Activated Dynamics in a Supercooled Lennard-Jones Liquid
• Hopping in a Supercooled Lennard-Jones Liquid: Metabasins, Waiting Time Distribution, and Diffusion
• Non-topographic description of inherent structure dynamics in glass formers
• Quasi-saddles as relevant points of the potential energy surface in the dynamics of supercooled liquids
• Finite size scaling analysis of the glass transition
• General features of the energy landscape in Lennard-Jones like model liquids
• Effect of physical aging on the low-frequency vibrational density of states of a glassy polymer
• The distance between Inherent Structures and the influence of saddles on approaching the mode coupling transition in a simple glass former

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