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Microstructure and thickening of dense suspensions under extensional and shear flows

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 Added by Ryohei Seto
 Publication date 2017
  fields Physics
and research's language is English




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Dense suspensions are non-Newtonian fluids which exhibit strong shear thickening and normal stress differences. Using numerical simulation of extensional and shear flows, we investigate how rheological properties are determined by the microstructure which is built under flows and by the interactions between particles. By imposing extensional and shear flows, we can assess the degree of flow-type dependence in regimes below and above thickening. Even when the flow-type dependence is hindered, nondissipative responses, such as normal stress differences, are present and characterise the non-Newtonian behaviour of dense suspensions.



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The phenomenon of shear-induced jamming is a factor in the complex rheological behavior of dense suspensions. Such shear-jammed states are fragile, i.e., they are not stable against applied stresses that are incompatible with the stress imposed to create them. This peculiar flow-history dependence of the stress response is due to flow-induced microstructures. To examine jammed states realized under constant shear stress, we perform dynamic simulations of non-Brownian particles with frictional contact forces and hydrodynamic lubrication forces. We find clear signatures that distinguish these fragile states from the more conventional isotropic jammed states.
Shear thickening denotes the rapid and reversible increase in viscosity of a suspension of rigid particles under external shear. This ubiquitous phenomenon has been documented in a broad variety of multiphase particulate systems, while its microscopic origin has been successively attributed to hydrodynamic interactions and frictional contact between particles. The relative contribution of these two phenomena to the magnitude of shear thickening is still highly debated and we report here a discriminating experimental study using a model shear-thickening suspension that allows us to tune independently both the surface chemistry and the surface roughness of the particles. We show here that both properties matter when it comes to continuous shear thickening (CST) and that the presence of hydrogen bonds between the particles is essential to achieve discontinuous shear thickening (DST) by enhancing solid friction between closely contacting particles. Moreover, a simple argument allows us to predict the onset of CST, which for these highly-textured particles occurs at a critical volume fraction much lower than that previously reported in the literature. Finally, we demonstrate how mixtures of particles with opposing surface chemistry make it possible to finely tune the shear-thickening response of the suspension at a fixed volume fraction, paving the way for a fine control of shear-thickening transition in engineering applications.
Nearly all dense suspensions undergo dramatic and abrupt thickening transitions in their flow behavior when sheared at high stresses. Such transitions occur when the dominant interactions between the suspended particles shift from hydrodynamic to frictional. Here, we interpret abrupt shear thickening as a precursor to a rigidity transition, and give a complete theory of the viscosity in terms of a universal crossover scaling function from the frictionless jamming point to a rigidity transition associated with friction, anisotropy, and shear. Strikingly, we find experimentally that for two different systems -- cornstarch in glycerol and silica spheres in glycerol -- the viscosity can be collapsed onto a single universal curve over a wide range of stresses and volume fractions. The collapse reveals two separate scaling regimes, due to a crossover between frictionless isotropic jamming and a frictional shear jamming point with different critical exponents. The material-specific behavior due to the microscale particle interactions is incorporated into an additive analytic background (given by the viscosity at low shear rates) and a scaling variable governing the proximity to shear jamming that depends on both stress and volume fraction. This reformulation opens the door to importing the vast theoretical machinery developed to understand equilibrium critical phenomena to elucidate fundamental physical aspects of the shear thickening transition.
Dense suspensions of particles are relevant to many applications and are a key platform for developing a fundamental physics of out-of-equilibrium systems. They present challenging flow properties, apparently turning from liquid to solid upon small changes in composition or, intriguingly, in the driving forces applied to them. The emergent physics close to the ubiquitous jamming transition (and to some extent the glass and gelation transitions) provides common principles with which to achieve a consistent interpretation of a vast set of phenomena reported in the literature. In light of this, we review the current state of understanding regarding the relation between the physics at the particle scale and the rheology at the macroscopic scale. We further show how this perspective opens new avenues for the development of continuum models for dense suspensions.
Molecular dynamics simulations confirm recent extensional flow experiments showing ring polymer melts exhibit strong extension-rate thickening of the viscosity at Weissenberg numbers $Wi<<1$. Thickening coincides with the extreme elongation of a minority population of rings that grows with $Wi$. The large susceptibility of some rings to extend is due to a flow-driven formation of topological links that connect multiple rings into supramolecular chains. Links form spontaneously with a longer delay at lower $Wi$ and are pulled tight and stabilized by the flow. Once linked, these composite objects experience larger drag forces than individual rings, driving their strong elongation. The fraction of linked rings generated by flow depends non-monotonically on $Wi$, increasing to a maximum when $Wisim1$ before rapidly decreasing when the strain rate approaches the relaxation rate of the smallest ring loops $sim 1/tau_e$.
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