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Cooling Rate Dependent Ellipsometry Measurements to Determine the Dynamics of Thin Glassy Films
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Disconnecting structure and dynamics in glassy thin films.

Daniel M Sussman1, Samuel S Schoenholz2, Ekin D Cubuk3

  • 1Department of Physics, Syracuse University, Syracuse, NY 13244; dmsussma@syr.edu.

Proceedings of the National Academy of Sciences of the United States of America
|September 21, 2017
PubMed
Summary

Thin glassy films exhibit unique dynamics compared to bulk materials. Structure-independent processes, not local structure, explain these differences, especially near surfaces.

Keywords:
glassmachine learningthin film

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Area of Science:

  • Materials Science
  • Polymer Physics
  • Statistical Mechanics

Background:

  • Nanometrically thin glassy films show distinct dynamical behaviors compared to bulk polymers.
  • Local structure is a key predictor of particle rearrangement dynamics in bulk glasses.

Purpose of the Study:

  • To investigate if dynamical differences in thin polymeric glass films stem from microscopic structural variations.
  • To understand the role of structure-dependent and structure-independent processes in thin film glass dynamics.

Main Methods:

  • Utilized machine learning to analyze local structure and particle dynamics.
  • Compared structural properties of particles at the film center versus near the surface.
  • Analyzed the contributions of structure-dependent and structure-independent dynamical processes.

Main Results:

  • Particles in thin films are structurally indistinguishable at the center and surface, despite differing dynamics.
  • Structure-independent dynamical processes are crucial for understanding thin film behavior.
  • Two distinct dynamical processes coexist: one structure-dependent and one purely Arrhenius and structure-independent.

Conclusions:

  • Glassy dynamics in thin films cannot be solely explained by local structure.
  • A structure-independent, Arrhenius-type process, enhanced near the surface, significantly influences thin film dynamics.
  • The interplay between structure-dependent and structure-independent dynamics governs glassy behavior across different film thicknesses.