Local Elasticity in Nonlinear Rheology of Interacting Colloidal Glasses Revealed by Neutron Scattering and Rheometry

TL;DR

This study combines neutron scattering and rheometry to reveal a transient elastic zone in colloidal glasses, linking microscopic heterogeneity to macroscopic shear behavior and highlighting the role of electrostatic interactions.

Contribution

It introduces the concept of a transient elasticity zone (TEZ) as a microscopic signature of dynamical heterogeneity in colloidal glasses under shear.

Findings

TEZ is a short-lived, localized elastic response at particle level.

The size of TEZ decreases with increasing shear rate, indicating diminishing heterogeneity.

The local elastic stress in TEZ matches the macroscopic stress, linking micro- and macro-scale behavior.

Abstract

The flow of colloidal suspensions is ubiquitous in nature and industry. Colloidal suspensions exhibit a wide range of rheological behavior, which should be closely related to the microscopic structure of the systems. With in-situ small-angle neutron scattering complemented by rheological measurements, we investigated the deformation behavior of a charge-stabilized colloidal glass at particle level undergoing steady shear. A short-lived, localized elastic response at particle level, termed as transient elasticity zone (TEZ), was identified from the neutron spectra. The existence of the TEZ is a signature of the dynamical heterogeneity: The body of fluids under shear behaves like an elastic solid within the spatial range of TEZ but like fluid outside the TEZ. The size of TEZ shrinks as the shear rate increases in the shear thinning region, which shows that the shear thinning is accompanied by a diminishing dynamical heterogeneity. More interestingly, the TEZ is found to be the structural unit that provides the resistance to the imposed shear, as evidenced by the quantitative agreement between the local elastic stress sustained by TEZ and the macroscopic stress from rheological measurements at low and moderate shear rates. Besides the charged-stabilized colloidal suspension, a hard-sphere colloidal suspension at the same volume fraction and shear rates was also measured. The result highlights the key role of the electrostatic interparticle repulsion in promoting the local elasticity. Our findings provide an understanding on the nonlinear rheology of interacting colloidal glasses from a micro-mechanical view.