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Register a new userAutonomously Probing Viscoelasticity in Disordered Suspensions
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Recent experiments show a strong rotational-diffusion enhancement for self-propelled microrheological probes in colloidal glasses. Here, we provide microscopic understanding using simulations with a frictional probe-medium coupling that converts active translation into rotation. Diffusive enhancement emerges from the mediums disordered structure and peaks at a second-order transition in the number of contacts. Our results reproduce the salient features of the colloidal glass experiment and support an effective description that is applicable to a broader class of viscoelastic suspensions.
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This is an integrated experimental and theoretical study of the dynamics and rheology of self-crosslinked, slightly charged, temperature responsive soft Poly(N-isopropylacrylamide) (pNIPAM) microgels over a wide range of concentration and temperature spanning the sharp change in particle size and intermolecular interactions across the lower critical solution temperature (LCST). Dramatic, non-monotonic changes in viscoelasticity are observed with temperature, with distinctive concentration dependences in the dense fluid, glassy, and soft-jammed states. Motivated by our experimental observations, we formulate a minimalistic model for the size dependence of a single microgel particle and the change of interparticle interaction from purely repulsive to attractive upon heating. Using microscopic equilibrium and time-dependent statistical mechanical theories, theoretical predictions are quantitatively compared with experimental measurements of the shear modulus. Good agreement is found for the nonmonotonic temperature behavior that originates as a consequence of the competition between reduced microgel packing fraction and increasing interpar-ticle attractions. Testable predictions are made for nonlinear rheological properties such as the yield stress and strain. To the best of our knowledge, this is the first attempt to quantitatively understand in a unified manner the viscoelasticity of dense, temperature-responsive microgel suspensions spanning a wide range of temperatures and concentrations.
Active chiral viscoelastic materials exhibit elastic responses perpendicular to the applied stresses, referred to as odd elasticity. We use a covariant formulation of viscoelasticity combined with an entropy production analysis to show that odd elasticity is not only present in active systems but also in broad classes of passive chiral viscoelastic fluids. In addition, we demonstrate that linear viscoelastic chiral solids do require activity in order to manifest odd elastic responses. In order to model the phenomenon of passive odd viscoelasticity we propose a chiral extension of Jeffreys model. We apply our covariant formalism in order to derive the dispersion relations of hydrodynamic modes and obtain clear imprints of odd viscoelastic behavior.
Owing to nonlinear viscoelasticity, materials often show characteristic features that resemble those of thixotropy. This issue has been debated in the literature over the past several decades, and several experimental protocols have been proposed to distinguish thixotropy from viscoelasticity. In this work, we assess these protocols by carrying out experiments using polymer solutions, thixotropic clay dispersions, and modeling their behavior, respectively, using the FENE-P constitutive equation and a viscoelastic aging model. We find that the criteria proposed in the literature, such as a step down jump in the shear rate and shear startup at different waiting times elapsed since preshear, are inadequate to distinguish thixotropy from viscoelasticity. In marked contrast, we show that the application of step-strain or step-stress after cessation of the preshear serves as a useful discriminant between thixotropy and viscoelasticity. In thixotropic materials, we observe that the application of step strain (or step stress) after cessation of the preshear eventually leads to slowing down of relaxation dynamics as a function of waiting time. However, for viscoelastic materials, the relaxation modulus (creep compliance) curve shifts to lower modulus (higher compliance) values as a function of waiting time until equilibrium is reached. While the proposed criterion offers a robust distinction between viscoelasticity and thixotropy for the systems studied here, further experimental investigations based on other systems are needed to establish its versatility and will lead to a greater insight into this long-standing issue in rheological categorization.
The mechanical response of active media ranging from biological gels to living tissues is governed by a subtle interplay between viscosity and elasticity. In this Letter, we generalize the canonical Kelvin-Voigt and Maxwell models to active viscoelastic media that break both parity and time-reversal symmetries. The resulting continuum theories exhibit viscous and elastic tensors that are both antisymmetric, or odd, under exchange of pairs of indices. We analyze how these parity violating viscoelastic coefficients determine the relaxation mechanisms and wave-propagation properties of odd materials.
We present a theoretical framework for the linear and nonlinear visco-elastic properties of reversibly crosslinked networks of semiflexible polymers. In contrast to affine models where network strain couples to the polymer end-to-end distance, in our model strain rather serves to locally distort the network structure. This induces bending modes in the polymer filaments, the properties of wich are slaved to the surrounding network structure. Specifically, we investigate the frequency-dependent linear rheology, in particular in combination with crosslink binding/unbinding processes. We also develop schematic extensions to describe the nonlinear response during creep measurements as well as during constant-strainrate ramps.
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