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Register a new userFirst-principle predictions for the rheology of soft jammed suspensions
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We explore the rheology predicted by a recently proposed constitutive model for jammed suspensions of soft elastic particles derived from microscopic dynamics [Cuny et al., arXiv:2102.05938]. Our model predicts that the orientation of the anisotropy of the microstructure, governed by an interplay between flow vorticity and contact elasticity, plays a key role at yielding and in flow. It generates normal stress differences contributing significantly to the yield criterion and Trouton ratio. It gives rise to non-trivial transients such as stress overshoots in step increases of shear rates, residual stresses after flow cessation and power law decay of the shear rate in creep. Finally, it explains the collapse of storage modulus as measured in parallel superposition for a yielded suspension.
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We present an integrated experimental and quantitative theoretical study of the mechanics of self-crosslinked, neutral, repulsive pNIPAM microgel suspensions over concentration (c) range spanning the fluid, glassy and putative soft jammed regimes. In the glassy regime we measure a linear elastic dynamic shear modulus over 3 decades which follows an apparent power law concentration dependence G~$c^{5.64}$, followed by a sharp crossover to a nearly linear growth at high concentrations. We formulate a theoretical approach to address all three regimes within a single conceptual Brownian dynamics framework. A minimalist single particle description is constructed that allows microgel size to vary with concentration due to steric de-swelling effects. Using a Hertzian repulsion interparticle potential and a suite of statistical mechanical theories, quantitative predictions under quiescent conditions of microgel collective structure, dynamic localization length, elastic modulus, and the structural relaxation time are made. Based on a constant inter-particle repulsion strength parameter which is determined by requiring the theory to reproduce the linear elastic shear modulus over the entire concentration regime, we demonstrate good agreement between theory and experiment. Theoretical predictions of how quiescent structural relaxation time changes under deformation, and how the yield stress and strain change as a function of concentration has been made. Reasonable agreement with our observations is obtained. To the best of our knowledge, this is the first attempt to quantitatively understand structure, quiescent relaxation and shear elasticity, and nonlinear yielding of dense microgel suspensions using microscopic force based theoretical methods that include activated hopping processes. We expect our approach will be useful for other soft polymeric particle suspensions in the core-shell family.
The rheology of suspensions of Brownian, or colloidal, particles (diameter $d lesssim 1$ $mu$m) differs markedly from that of larger grains ($d gtrsim 50$ $mu$m). Each of these two regimes has been separately studied, but the flow of suspensions with intermediate particle sizes (1 $mutextrm{m} lesssim d lesssim 50$ $mu$m), which occur ubiquitously in applications, remains poorly understood. By measuring the rheology of suspensions of hard spheres with a wide range of sizes, we show experimentally that shear thickening drives the transition from colloidal to granular flow across the intermediate size regime. This insight makes possible a unified description of the (non-inertial) rheology of hard spheres over the full size spectrum. Moreover, we are able to test a new theory of friction-induced shear thickening, showing that our data can be well fitted using expressions derived from it.
Dense suspensions of hard particles in a Newtonian liquid can be jammed by shear when the applied stress exceeds a certain threshold. However, this jamming transition from a fluid into a solidified state cannot be probed with conventional steady-state rheology because the stress distribution inside the material cannot be controlled with sufficient precision. Here we introduce and validate a method that overcomes this obstacle. Rapidly propagating shear fronts are generated and used to establish well-controlled local stress conditions that sweep across the material. Exploiting such transient flows, we are able to track how a dense suspension approaches its shear jammed state dynamically, and can quantitatively map out the onset stress for solidification in a state diagram.
Microcapsules are commonly used in applications ranging from therapeutics to personal care products due to their ability to deliver encapsulated species through their porous shells. Here, we demonstrate a simple and scalable approach to fabricate microcapsules with porous shells by interfacial complexation of cellulose nanofibrils and oleylamine, and investigate the rheological properties of suspensions of the resulting microcapsules. The suspensions of neat capsules are viscous liquids whose viscosity increases with volume fraction according to a modified Kreiger-Dougherty relation with a maximum packing fraction of 0.73 and an intrinsic viscosity of 4. When polyacrylic acid (PAA) is added to the internal phase of the microcapsule, however, the suspensions become elastic and display yield stresses with power-law dependencies on capsule volume fraction and PAA concentration. The elasticity appears to originate from associative interactions between microcapsules induced by PAA that resides within the microcapsule shells. These results demonstrate that it is possible to tune the rheological properties of microcapsule suspensions by changing only the composition of the internal phase, thereby providing a novel method to tailor complex fluid rheology.
We study the rheology of a soft particulate system where the inter-particle interactions are weakly attractive. Using extensive molecular dynamics simulations, we scan across a wide range of packing fractions ($phi$), attraction strengths ($u$) and imposed shear-rates ($dot{gamma}$). In striking contrast to repulsive systems, we find that at small shear-rates generically a fragile isostatic solid is formed even if we go to $phi ll phi_J$. Further, with increasing shear-rates, even at these low $phi$, non-monotonic flow curves occur which lead to the formation of persistent shear-bands in large enough systems. By tuning the damping parameter, we also show that inertia plays an important role in this process. Furthermore, we observe enhanced particle dynamics in the attraction-dominated regime as well as a pronounced anisotropy of velocity and diffusion constant, which we take as precursors to the formation of shear bands. At low enough $phi$, we also observe structural changes via the interplay of low shear-rates and attraction with the formation of micro-clusters and voids. Finally, we characterize the properties of the emergent shear bands and thereby, we find surprisingly small mobility of these bands, leading to prohibitely long time-scales and extensive history effects in ramping experiments.
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