Constrained dynamics of localized excitations causes a non-equilibrium phase transition in an atomistic model of glass formers

Abstract

Dynamic facilitation theory assumes short-ranged dynamic constraints to be the essential feature of supercooled liquids and draws much of its conclusions from the study of kinetically constrained models. While deceptively simple, these models predict the existence of trajectories that maintain a high overlap with their initial state over many structural relaxation times. We use molecular dynamics simulations combined with importance sampling in trajectory space to test this prediction through counting long-lived particle displacements. For observation times longer than the structural relaxation time exponential tails emerge in the probability distribution of this number. Reweighting trajectories towards low mobility corresponds to a phase transition into an inactive phase. While dynamics in these two phases is drastically different structural measures show only slight differences. We discuss the choice of dynamic order parameter and give a possible explanation for the microscopic origin of the effective dynamic constraints.

revised version

References in corpus (10)

• Glassy dynamics of kinetically constrained models
• Dynamic first-order phase transition in kinetically constrained models of glasses
• First-order dynamical phase transition in models of glasses: an approach based on ensembles of histories
• Growing length and time scales in glass forming liquids
• Understanding fragility in supercooled Lennard-Jones mixtures. I. Locally preferred structures
• Finite-temperature critical point of a glass transition
• A critical test of the mode-coupling theory of the glass transition
• Space-time thermodynamics and subsystem observables in a kinetically constrained model of glassy systems
• Preparation and relaxation of very stable glassy states of a simulated liquid
• Space-time Phase Transitions in Driven Kinetically Constrained Lattice Models

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