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Updated: Jul 16, 2025

Cooling Rate Dependent Ellipsometry Measurements to Determine the Dynamics of Thin Glassy Films
Published on: January 26, 2016
Front propagation in ultrastable glasses is dynamically heterogeneous
Cecilia Herrero1, Mark D Ediger2, Ludovic Berthier1,3
1Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS, 34095 Montpellier, France.
Abstract:
Upon heating, ultrastable glassy films transform into liquids via a propagating equilibration front, resembling the heterogeneous melting of crystals. A microscopic understanding of this robust phenomenology is, however, lacking because experimental resolution is limited. We simulate the heterogeneous transformation kinetics of ultrastable configurations prepared using the swap Monte Carlo algorithm, thus allowing a direct comparison with experiments. We resolve the liquid-glass interface both in space and in time as well as the underlying particle motion responsible for its propagation. We perform a detailed statistical analysis of the interface geometry and kinetics over a broad range of temperatures. We show that the dynamic heterogeneity of the bulk liquid is passed on to the front that propagates heterogeneously in space and intermittently in time. This observation allows us to relate the averaged front velocity to the equilibrium diffusion coefficient of the liquid. We suggest that an experimental characterization of the interface geometry during the heterogeneous devitrification of ultrastable glassy films could provide direct experimental access to the long-sought characteristic length scale of dynamic heterogeneity in bulk supercooled liquids.
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