Aging in Dense Colloids as Diffusion in the Logarithm of Time

TL;DR

This paper demonstrates that aging in dense colloids can be understood as diffusion in the logarithm of time, supported by experimental data and a phenomenological model that captures long-lived correlations and dynamic heterogeneity.

Contribution

It introduces a novel analysis confirming diffusion in the logarithm of time for dense colloids and proposes a stochastic model based on cluster dynamics to explain aging behaviors.

Findings

Mean square displacement is linear in time at low densities.

In dense colloids, displacement grows linearly with the logarithm of time.

Long-lived spatial correlations are observed in dense colloids.

Abstract

The far-from-equilibrium dynamics of glassy systems share important phenomenological traits. A transition is generally observed from a time-homogeneous dynamical regime to an aging regime where physical changes occur intermittently and, on average, at a decreasing rate. It has been suggested that a global change of the independent time variable to its logarithm may render the aging dynamics homogeneous: for colloids, this entails diffusion but on a logarithmic time scale. Our novel analysis of experimental colloid data confirms that the mean square displacement grows linearly in time at low densities and shows that it grows linearly in the logarithm of time at high densities. Correspondingly, pairs of particles initially in close contact survive as pairs with a probability which decays exponentially in either time or its logarithm. The form of the Probability Density Function of the displacements shows that long-ranged spatial correlations are very long-lived in dense colloids. A phenomenological stochastic model is then introduced which relies on the growth and collapse of strongly correlated clusters ("dynamic heterogeneity"), and which reproduces the full spectrum of observed colloidal behaviors depending on the form assumed for the probability that a cluster collapses during a Monte Carlo update. In the limit where large clusters dominate, the collapse rate is ~1/t, implying a homogeneous, log-Poissonian process that qualitatively reproduces the experimental results for dense colloids. Finally an analytical toy-model is discussed to elucidate the strong dependence of the simulation results on the integrability (or lack thereof) of the cluster collapse probability function.