The glass transition of soft colloids

TL;DR

This study investigates the glass transition in soft colloids, revealing that softness influences dynamics mainly at high densities where non-equilibrium effects dominate, leading to unique relaxation behaviors.

Contribution

It demonstrates that particle softness affects colloidal glass dynamics primarily at high packing fractions, highlighting a transition to a stress-driven, non-equilibrium regime with weak density dependence.

Findings

Structural relaxation time grows steeply with volume fraction in supercooled regime.

Softness becomes relevant only at very high packing fractions.

Non-equilibrium regime shows weak dependence of relaxation time on density.

Abstract

We explore the glassy dynamics of soft colloids using microgels and charged particles interacting by steric and screened Coulomb interactions, respectively. In the supercooled regime, the structural relaxation time $\tau_\alpha$ of both systems grows steeply with volume fraction, reminiscent of the behavior of colloidal hard spheres. Computer simulations confirm that the growth of $\tau_\alpha$ on approaching the glass transition is independent of particle softness. By contrast, softness becomes relevant at very large packing fractions when the system falls out of equilibrium. In this non-equilibrium regime, $\tau_\alpha$ depends surprisingly weakly on packing fraction and time correlation functions exhibit a compressed exponential decay consistent with stress-driven relaxation. The transition to this novel regime coincides with the onset of an anomalous decrease of local order with increasing density typical of ultrasoft systems. We propose that these peculiar dynamics results from the combination of the non-equilibrium aging dynamics expected in the glassy state and the tendency of colloids interacting through soft potentials to refluidize at high packing fractions.