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Confocal Imaging of Confined Quiescent and Flowing Colloid-polymer Mixtures

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Equilibration of concentrated hard-sphere fluids.

Gabriel Pérez-Ángel¹, Luis Enrique Sánchez-Díaz, Pedro E Ramírez-González

¹Departamento de Física Aplicada, Centro de Investigación y de Estudios Avanzados del Instituto Politécnico Nacional, Unidad Mérida, Mérida, Yucatán, Mexico.

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics

|July 30, 2011

Summary

We studied hard-sphere fluids near the glass transition, finding that equilibration time increases sharply with volume fraction. This suggests equilibrium properties are experimentally impossible to measure at high volume fractions.

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Area of Science:

Physics
Materials Science
Chemical Engineering

Background:

Understanding the glass transition is crucial for materials science.
Metastable states in fluids near the glass transition pose significant challenges for equilibration.

Purpose of the Study:

To systematically investigate the isochoric equilibration of hard-sphere fluids.
To characterize relaxation times and diffusion coefficients during thermalization.

Main Methods:

Employed molecular dynamics simulations.
Prepared systems in nonequilibrium states with varying volume fractions (ϕ).
Monitored evolution of α-relaxation time (τ(α)(k)) and self-diffusion coefficient (D(L)) over waiting time (t(w)).

Main Results:

Identified distinct equilibration regimes based on volume fraction and waiting time.
Observed a crossover volume fraction (ϕ(c)(t(w))) that increases with waiting time and saturates around ϕ(a) ≈ 0.582.
Found equilibration time grows faster than equilibrium relaxation time, t(w)(eq)(ϕ) ≈ 0.27[τ(α)(eq)(k;ϕ)](1.43).

Conclusions:

Equilibration dynamics are strongly dependent on volume fraction and waiting time.
Suggests experimental measurement of equilibrium properties is infeasible at volume fractions near or exceeding ϕ(a).
Highlights the difficulty of achieving true equilibrium in dense hard-sphere systems.