Front propagation in ultrastable glasses is dynamically heterogeneous

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.

Automated summary

In this study, the heterogeneous transformation kinetics of ultrastable glassy films upon heating were simulated and analyzed. The results show a close correlation between the geometry and dynamics of the liquid-glass interface and the dynamic heterogeneity of the bulk liquid. This study provides a new approach to experimentally access the characteristic length scale of dynamic heterogeneity in supercooled liquids.