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Propagation of Waves

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Cooling Rate Dependent Ellipsometry Measurements to Determine the Dynamics of Thin Glassy Films

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 Berthier^1,3

¹Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS, 34095 Montpellier, France.

The Journal of Chemical Physics

|September 19, 2023

Summary

Ultrastable glassy films transform into liquid upon heating via a propagating front. Simulations reveal this front

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Area of Science:

Materials Science
Condensed Matter Physics
Computational Chemistry

Background:

Ultrastable glassy films exhibit unique transformation behavior upon heating, transitioning to liquids through a propagating equilibration front.
This phenomenon resembles heterogeneous crystal melting, but a microscopic understanding is limited by experimental resolution.

Purpose of the Study:

To simulate and microscopically understand the heterogeneous transformation kinetics of ultrastable glassy films.
To resolve the liquid-glass interface and underlying particle motion during transformation.
To relate the front propagation dynamics to the bulk liquid properties.

Main Methods:

Utilized swap Monte Carlo algorithm to prepare ultrastable configurations for simulation.
Performed detailed spatiotemporal analysis of the liquid-glass interface and particle dynamics.
Conducted statistical analysis of interface geometry and kinetics across a range of temperatures.

Main Results:

Resolved the liquid-glass interface and particle motion, revealing heterogeneous spatial propagation and intermittent temporal dynamics of the equilibration front.
Demonstrated that the dynamic heterogeneity of the bulk liquid is imprinted onto the front.
Established a relationship between the averaged front velocity and the equilibrium diffusion coefficient of the liquid.

Conclusions:

The dynamic heterogeneity of the bulk liquid dictates the heterogeneous propagation of the equilibration front in ultrastable glassy films.
Experimental characterization of the interface geometry could provide access to the characteristic length scale of dynamic heterogeneity in supercooled liquids.