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Local-Average Free Volume Correlates with Dynamics in Glass Formers.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Chemical Physics

Background:

  • Glass-forming liquids exhibit significant slowdowns and increasing heterogeneity approaching the glass transition.
  • A key debate concerns whether this dynamical slowdown arises from dynamical heterogeneity and its structural origins.
  • Previous studies showed weak correlations between dynamical heterogeneity and single-particle free volume distribution.

Purpose of the Study:

  • To investigate the relationship between structural properties and dynamic heterogeneity in glass-forming liquids.
  • To determine if a purely structural origin for dynamic heterogeneity exists.
  • To clarify the role of free volume in particle rearrangements during activated hopping relaxation.

Main Methods:

  • Introduction of the 'local-average free volume' concept.
  • Numerical simulations to analyze correlations between structural properties and dynamics.
  • Examination of correlations over length scales of neighboring atomic shells.

Main Results:

  • Long-time dynamic heterogeneity shows significantly enhanced correlation with the average local free volume.
  • This correlation is observed over a length scale of a few neighboring shells.
  • The findings suggest a stronger link between structural free volume and dynamic heterogeneity than previously thought.

Conclusions:

  • Free volume plays a crucial role in particle rearrangements and activated hopping relaxation in glass formers.
  • The concept of local-average free volume provides a better structural descriptor for dynamic heterogeneity.
  • The 'local average' approach can be extended to other structural descriptors for analyzing glass-forming liquids.