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Cooling Rate Dependent Ellipsometry Measurements to Determine the Dynamics of Thin Glassy Films
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Intermolecular forces and the glass transition.

Randall W Hall1, Peter G Wolynes

  • 1Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70808, USA. rhall@lsu.edu

The Journal of Physical Chemistry. B
|November 10, 2007
PubMed
Summary

Random first-order transition theory reveals the interplay of attractive and repulsive forces in supercooled liquids. This study elucidates the microscopic origins of liquid dynamics and scaling relations, supporting key theoretical temperature intersections.

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Area of Science:

  • Condensed Matter Physics
  • Theoretical Chemistry
  • Materials Science

Background:

  • Understanding the dynamics of supercooled liquids is crucial for explaining the glass transition.
  • The roles of attractive and repulsive interactions in liquid dynamics remain incompletely understood.
  • Existing theories often lack a microscopic basis for observed phenomena like density-temperature scaling.

Purpose of the Study:

  • To determine the specific roles of attractive and repulsive forces in supercooled liquid dynamics using Random First-Order Transition (RFOT) theory.
  • To microscopically explain empirical density-temperature scaling relations observed in supercooled liquids.
  • To investigate the relationship between the spinodal and Kauzmann temperatures as a function of density.

Main Methods:

  • Application of Random First-Order Transition (RFOT) theory.
  • Utilized Self-Consistent Phonon (SCP) theory for glassy configurations and liquid-state approximations for the liquid phase.
  • Employed liquid-state perturbation theory for free energy calculations.

Main Results:

  • Calculated key transition temperatures: T*A (onset of activated behavior), T*C (barrierless motion), T*K (Kauzmann temperature), and T*g (glass transition temperature).
  • Demonstrated agreement between calculated relationships and experimental/simulation data for van der Waals liquids.
  • Validated empirical density-temperature scaling relations for alpha-relaxation time, revealing their microscopic origin.
  • Provided evidence supporting the intersection of spinodal and Kauzmann temperatures at low densities.

Conclusions:

  • RFOT theory successfully describes the dynamics of supercooled liquids, highlighting the balance of interparticle forces.
  • The study provides a microscopic foundation for observed scaling laws in supercooled liquids.
  • Microscopic calculations support a theoretical link between the spinodal and Kauzmann temperatures.