Delayed solidification of soft glasses: New experiments, and a theoretical challenge

TL;DR

This study investigates the delayed solidification of soft glasses under oscillatory shear, revealing experimental results that challenge existing theoretical models and highlight the need for new explanations.

Contribution

The paper presents new experimental data on delayed solidification in Laponite suspensions and critically examines the limitations of current SGR-type models.

Findings

Delayed solidification depends on stress amplitude, frequency, and age.

Existing models cannot fully explain large strain amplitudes observed.

Power-law distribution of barrier heights suggested by data.

Abstract

When subjected to large amplitude oscillatory shear stress, aqueous Laponite suspensions show an abrupt solidification transition after a long delay time tc. We measure the dependence of tc on stress amplitude, frequency, and on the age-dependent initial loss modulus. At first sight our observations appear quantitatively consistent with a simple soft-glassy rheology (SGR)-type model, in which barrier crossings by mesoscopic elements are purely strain-induced. For a given strain amplitude {\gamma}0 each element can be classified as fluid or solid according to whether its local yield strain exceeds {\gamma}0. Each cycle, the barrier heights E of yielded elements are reassigned according to a fixed prior distribution {\rho}(E): this fixes the per-cycle probability R({\gamma}0) of a fluid elements becoming solid. As the fraction of solid elements builds up, {\gamma}0 falls (at constant stress amplitude), so R({\gamma}0) increases. This positive feedback accounts for the sudden solidification after a long delay. The model thus appears to directly link macroscopic rheology with mesoscopic barrier height statistics: within its precepts, our data point towards a power law for {\rho}(E) rather than the exponential form usually assumed in SGR. However, despite this apparent success, closer investigation shows that the assumptions of the model cannot be reconciled with the extremely large strain amplitudes arising in our experiments. The quantitative explanation of delayed solidification in Laponite therefore remains an open theoretical challenge.