The microstructural change causing the failure of the Cox-Merz rule in Newtonian suspensions: experiments and simulations

Abstract

Newtonian non-Brownian concentrated suspensions show a mismatch between the steady state and the complex viscosity, whatever the strain amplitude imposed in the oscillatory flow. This result is counterintuitive in the two extreme cases of vanishing strain amplitude and very large one. In the first case, the oscillatory flow should not be able to alter the steady microstructure, as well as in the other opposite limit for which the strain amplitude is so high that the oscillatory flow resembles a steady flow reversal. If the microstructure is not altered with respect to the steady one, similarly the complex viscosity should be equal to the steady one. We here investigate experimentally and numerically the origin of the viscosities mismatch at any imposed strain amplitude. We focus on the first two or three cycles of oscillations and different particle concentrations. Experimental and numerical results agree and allow to prove that for intermediate amplitudes, the oscillatory shear induces the breakage of particle clusters and the microstructure modifies so to minimise particle collisions. For very small strain amplitudes, the oscillatory shear only induces the rotation of few couples of touching particles and the complex viscosity results slightly smaller than the steady one, while for very large strains, the oscillatory flow reshuffles the particles inducing a microstructure as clustered as the steady state one but with a different angular distribution function. We show that the vast majority of the microstructure rearrangement takes place in the first half cycle of oscillation.