Large Amplitude Oscillatory Shear Study of a Colloidal Gel at the Critical State

TL;DR

This study explores the nonlinear viscoelastic behavior of a colloidal gel at its critical state using large amplitude oscillatory shear rheology, revealing strain stiffening, shear thinning, and microstructural insights.

Contribution

It introduces a detailed nonlinear analysis of colloidal gels at the critical point and develops an integral model with a novel damping function for better predictive accuracy.

Findings

First harmonic decreases monotonically during transition

Observation of intracycle strain stiffening and shear thinning

Model with spectral damping function improves fit across conditions

Abstract

We investigate the nonlinear viscoelastic behavior of a colloidal dispersion at the critical gel state using large amplitude oscillatory shear (LAOS) rheology. The colloidal gel at the critical point is subjected to oscillatory shear flow with increasing strain amplitude at different frequencies. We observe that the first harmonic of the elastic and viscous moduli exhibits a monotonic decrease as the material undergoes a linear to nonlinear transition. We analyze the stress waveform across this transition and obtain the nonlinear moduli and viscosity as a function of frequency and strain amplitude. The analysis of the nonlinear moduli and viscosities suggests intracycle strain stiffening and intracycle shear thinning in the colloidal dispersion. Based on the insights obtained from the nonlinear analysis, we propose a potential scenario of the microstructural changes occurring in the nonlinear region. We also develop an integral model using the time-strain separable K-BKZ constitutive equation with a power-law relaxation modulus and damping function obtained from experiments. At low strain amplitudes, this model compares well with experimental data at all frequencies. However, a stronger damping function, which can be efficiently inferred using a spectral method, is required to obtain quantitative fits across the entire range of strain amplitudes and the explored frequencies.