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Locally averaged free volume, not single-particle free volume, better predicts slowdown in glass-forming liquids. Anisotropy in free volume seeds relaxation events, crucial for understanding the glass transition.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Physics

Background:

  • Understanding dynamical slowdown in glass-forming liquids is a key challenge.
  • The role of free volume in structural relaxation is debated.

Purpose of the Study:

  • To investigate the relationship between different measures of free volume and dynamical heterogeneity.
  • To identify structural factors governing the glass transition.

Main Methods:

  • Employed molecular dynamics simulations of the 3D Kob-Andersen binary Lennard-Jones model.
  • Analyzed locally averaged free volume (V2) and single-particle free volume (V0).
  • Quantified correlations with spatial enrichment, probability density shifts, and local relaxation times.

Main Results:

  • Locally averaged free volume (V2) shows stronger correlations with dynamical heterogeneity and relaxation than V0.
  • Anisotropic free volumes are linked to enhanced particle mobility and configurational freedom.
  • The lifetime of particles with large, anisotropic free volumes (τlong) matches structural relaxation time (τa).
  • Cooling leads to a loss of "active regions" that suppress motion and drive super-Arrhenius growth of τa.

Conclusions:

  • A unified free volume framework is proposed, emphasizing local spatial correlations and anisotropy.
  • Anisotropy in free volume is identified as a key factor initiating relaxation events.
  • These findings provide insights into the super-Arrhenius slowdown observed in glass-forming liquids.