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Randy H. Ewoldt

Publications and source records attributed to Randy H. Ewoldt.

23 records · Page 2Linked to original sources

Thermoresponsive stiffening with microgel particles in a semiflexible fibrin network

We report temperature-responsive soft composites of semiflexible biopolymer networks (fibrin) containing dispersed microgel colloidal particles of poly(N-isopropylacrylamide) (pNIPAM) that undergo a thermodynamically driven de-swelling transition above a Lower Critical Solution Temperature (LCST). Unlike standard polymer-particle composites, decreasing the inclusion volume of the particles (by increasing temperature)is concomitant with a striking increase of the overall elastic stiffness of the composite. We observe such a behavior over a wide composition space. The composite elastic shear modulus reversibly stiffens by up to 10-fold over a small change in temperature from 25-35°C. In isolation, the fibrin network and microgel suspension both soften with increased temperature, making the stiffening of the composites particularly significant. We hypothesize that stiffening is caused by contracting microgel particles adsorbing on the fibrin filaments and modifying the structure of the semiflexible network. We develop two phenomenological models that quantify this hypothesis in physically distinct manners, and the derived predictions are qualitatively consistent with our experimental data

cond-mat.soft↗

Linear and Nonlinear Rheology and Structural Relaxation in Dense Glassy and Jammed Soft Repulsive Microgel Suspensions

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.

cond-mat.soft↗

Unraveling hagfish slime

Hagfish slime is a unique predator defense material containing a network of long fibrous threads each ~ 10 cm in length. Hagfish release the threads in a condensed coiled state known as thread cells, or skeins (~ 100 microns), which must unravel within a fraction of a second to thwart a predator attack. Here we consider the hypothesis that viscous hydrodynamics can be responsible for this rapid unraveling, as opposed to chemical reaction kinetics alone. Our main conclusion is that, under reasonable physiological conditions, unraveling due to viscous drag can occur within a few hundred milliseconds, and is accelerated if the skein is pinned at a surface such as the mouth of a predator. We model a single thread cell unspooling as the fiber peels away due to viscous drag. We capture essential features by considering one-dimensional scenarios where the fiber is aligned with streamlines in either uniform flow or uniaxial extensional flow. The peeling resistance is modeled with a power-law dependence on peeling velocity. A dimensionless ratio of viscous drag to peeling resistance appears in the dynamical equations and determines the unraveling timescale. Our modeling approach is general and can be refined with future experimental measurements of peel strength for skein unraveling. It provides key insights into the unraveling process, offers potential answers to lingering questions about slime formation from threads and mucous vesicles, and will aid the growing interest in engineering similar bioinspired material systems.

cond-mat.soft↗

Liquid-solid impacts of yield-stress fluids

This is an entry to the Gallery of Fluid Motion at the 66th annual meeting of the APS-DFD, held November 2013 in Pittsburgh, PA. In this fluid dynamics video we demonstrate distinct features of yield-stress fluid droplets impacting pre-coated surfaces.

physics.flu-dyn↗

Fingerprinting Soft Materials: A Framework for Characterizing Nonlinear Viscoelasticity

We introduce a comprehensive scheme to physically quantify both viscous and elastic rheological nonlinearities simultaneously, using an imposed large amplitude oscillatory shear (LAOS) strain. The new framework naturally lends a physical interpretation to commonly reported Fourier coefficients of the nonlinear stress response. Additionally, we address the ambiguities inherent in the standard definitions of viscoelastic moduli when extended into the nonlinear regime, and define new measures which reveal behavior that is obscured by conventional techniques.

cond-mat.soft↗