Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userLinear and Nonlinear Rheology and Structural Relaxation in Dense Glassy and Jammed Soft Repulsive Microgel Suspensions
141
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
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.
rate research
Read More
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.
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.
We explore the origins of slow dynamics, aging and glassy rheology in soft and living matter. Non-diffusive slow dynamics and aging in materials characterised by crowding of the constituents can be explained in terms of structural rearrangement or remodelling events that occur within the jammed state. In this context, we introduce the jamming phase diagram proposed by Liu and Nagel to understand the ergodic-nonergodic transition in these systems, and discuss recent theoretical attempts to explain the unusual, faster-than-exponential dynamical structure factors observed in jammed soft materials. We next focus on the anomalous rheology (flow and deformation behaviour) ubiquitous in soft matter characterised by metastability and structural disorder, and refer to the Soft Glassy Rheology (SGR) model that quantifies the mechanical response of these systems and predicts aging under suitable conditions. As part of a survey of experimental work related to these issues, we present x-ray photon correlation spectroscopy (XPCS) results of the aging of laponite clay suspensions following rejuvenation. We conclude by exploring the scientific literature for recent theoretical advances in the understanding of these models and for experimental investigations aimed at testing their predictions.
We report studies of the frequency dependent shear modulus, $G^*(omega)=G(omega)+iG(omega)$, of the liquid crystal octylcyanobiphenyl (8CB) confined in a colloidal aerosil gel. With the onset of smectic order, $G$ grows approximately linearly with decreasing temperature, reaching values that exceed by more than three orders of magnitude the values for pure 8CB. The modulus at low temperatures possesses a power-law component, $G^*(omega) sim omega^alpha$, with exponent $alpha$ that approaches zero with increasing gel density. The amplitude of $G$ and its variation with temperature and gel density indicate that the low temperature response is dominated by a dense population of defects in the smectic. In contrast, when the 8CB is isotropic or nematic, the modulus is controlled by the elastic behavior of the colloidal gel.
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.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
