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Colloidal particle diffusion deviates from theory in supercooled liquids. Assigning an effective mass to correlated clusters recovers theoretical diffusion, enabling measurement of static correlations near the glass transition.

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Area of Science:

  • Colloid science
  • Condensed matter physics
  • Statistical mechanics

Background:

  • Diffusion coefficients of colloidal particles are crucial for understanding liquid behavior.
  • Existing models based on random collisions fail to predict diffusion in supercooled regimes.
  • Probing structural correlations is key to understanding the glass transition.

Purpose of the Study:

  • To measure diffusion coefficients of colloidal particles at varying concentrations using video microscopy.
  • To investigate deviations from theoretical predictions in the supercooled regime.
  • To develop an indirect method for probing static correlation length scales near the glass transition.

Main Methods:

  • Video microscopy was employed to measure long-time diffusion coefficients.
  • Theoretical diffusion relations were modified by assigning an effective mass to correlated clusters.
  • The method was validated using quasi-two-dimensional experiments of mono-disperse colloid crystallization.

Main Results:

  • Diffusion coefficients deviated from random collision models in the supercooled regime.
  • Assigning effective mass proportional to cluster size recovered theoretical diffusion relations.
  • Correlation length in a binary colloidal liquid followed a power law toward a critical packing fraction of ~0.79.
  • System relaxation time showed a power-law dependence on correlation length.

Conclusions:

  • The effective mass approach provides an indirect method to probe static correlation length scales.
  • This method is validated for studying crystallization and approaching the glass transition.
  • Observed power-law dependencies align with dynamical facilitation theories.