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The dynamical crossover in attractive colloidal systems.

Francesco Mallamace1, Carmelo Corsaro, H Eugene Stanley

  • 1Dipartimento di Fisica e Scienze della Terra, Università di Messina and CNISM, I-98168 Messina, Italy.

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This study reveals that clustering effects dominate dynamics near the percolation threshold in colloidal systems, leading to a fragile-to-strong liquid crossover. Extended mode-coupling theory explains dynamic arrest by considering cage and hopping effects.

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Area of Science:

  • Colloid Science
  • Soft Matter Physics
  • Materials Science

Background:

  • Adhesive hard-sphere colloidal systems, like Pluronic-L64 micellar suspensions, exhibit complex phase behavior.
  • Mode-coupling theory (MCT) predicts attractive glass (AG) and repulsive glass (RG) phases with singularities.
  • Previous studies identified a percolation threshold (PT) line and reentrant AG-liquid-RG behavior in the T-φ phase diagram.

Purpose of the Study:

  • To investigate dynamical arrest in adhesive hard-sphere colloidal systems.
  • To analyze the T-φ phase diagram and its relation to glassy phases and percolation.
  • To explore the fragile-to-strong liquid crossover (FSC) and its connection to clustering dynamics.

Main Methods:

  • Utilized viscosity measurements and nuclear magnetic resonance (NMR) spectroscopy.
  • Applied MCT scaling laws to analyze shear viscosity as a function of temperature (T) and volume fraction (φ).
  • Examined the colloidal system's phase diagram, including PT and glass-to-glass transitions.

Main Results:

  • NMR data confirmed the colloidal system's phase diagram and indicated fractal-like percolating structures near the PT.
  • MCT scaling revealed a fragile-to-strong liquid crossover (FSC) near the PT, coinciding with developed clustering.
  • The critical parameters defining the PT line were found to be the locus of the FSC.

Conclusions:

  • Dynamic arrest in these colloidal systems is governed by clustering effects between the FSC and glass transition lines.
  • Extended MCT provides a framework to describe dynamic arrest, incorporating both cage and hopping effects.
  • The FSC phenomenon exhibits broader thermodynamic generality than previously assumed, linked to percolation and clustering.