Heterogeneity-induced retraction in viscoelastic fluids following cessation of flow.

Abstract

Complex fluids including colloidal suspensions, microgels, and entangled wormlike micelles (WLMs) can develop heterogeneous flow regions under imposed steady shear. In some of these systems, the evolution to this flow state from rest is accompanied by flow reversal - when a portion of the fluid moves opposite to the imposed flow direction. Flow reversal was proposed to occur in shear startup when (1) the fluid has significant elasticity, and (2) the flow becomes heterogeneous immediately following the stress overshoot [McCauley et al., J. Rheol., 2023, 67, 661-681]. To verify this hypothesis, a new method is developed for measuring flow heterogeneity. Upon cessation of the imposed flow, elasticity and flow heterogeneity cause retraction of the fluid, which is quantified with particle tracking velocimetry. Flow is stopped at key times during shear startup in two systems: a gel-like WLM that exhibits flow reversal before heterogeneous flow and a viscoelastic, fluid-like WLM that does not. The degree of flow heterogeneity is inferred from the shape and magnitude of velocity profiles measured during retraction. Flow heterogeneity develops earlier in gel-like WLMs - supporting the proposed flow reversal criteria. For comparison, heterogeneous Couette flows described with the upper-convected Maxwell or Germann-Cook-Beris models are analyzed. These theoretical flow problems confirm that stark differences in rheological properties across the flow geometry can cause significant fluid retraction and reproduce key features of the experimentally observed retraction. This new method can be used to extract quantitative information about spatially heterogeneous flows in viscoelastic complex fluids, whether or not flow reversal occurs.