paper

Inherent-State Melting and the Onset of Glassy Dynamics in Two-Dimensional Supercooled Liquids

arXiv:2204.07528 · doi:10.1073/pnas.2209144120

Abstract

Below the onset temperature , the equilibrium relaxation time of most glass-forming liquids exhibits glassy dynamics characterized by super-Arrhenius temperature dependence. In this supercooled regime, the relaxation dynamics also proceeds through localized elastic excitations corresponding to hopping events between inherent states, i.e., potential-energy minimizing configurations of the liquid. Despite its importance in distinguishing the supercooled regime from the high-temperature regime, the microscopic origin of is not yet known. Here, we construct a theory for the onset temperature in two dimensions and find that inherent-state melting transition, described by the binding-unbinding transition of dipolar elastic excitations, delineates the supercooled regime from the high-temperature regime. The corresponding melting transition temperature is in good agreement with the onset temperature found in various two-dimensional atomistic models of glass formers. We discuss the predictions of our theory on the displacement and density correlations of two-dimensional supercooled liquids, which are consistent with observations of the Mermin-Wagner fluctuations in recent experiments and molecular simulations.

8 pages, 4 figures, 1 table

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