We study experimentally the behavior of isotropic suspensions of noncolloidal particles in yield stress fluids. This problem has been poorly studied in the literature, and only on specific materials. In this paper, we manage to develop procedures and materials that allow us to focus on the purely mechanical contribution of the particles to the yield stress fluid behavior, independently of the physicochemical properties of the materials. This allows us to relate the macroscopic properties of these suspensions to the mechanical properties of the yield stress fluid and the particle volume fraction, and to provide results applicable to any noncolloidal particle in any yield stress fluid. We find that the elastic modulus-concentration relationship follows a Krieger-Dougherty law, and we show that the yield stress-concentration relationship is related to the elastic modulus-concentration relationship through a very simple law, in agreement with results from a micromechanical analysis.
We report rheological measurements of a noncolloidal particle suspension in a Newtonian solvent at 40% solid volume fraction. An anomalous, frequency-dependent complex viscosity is found under oscillatory shear (OS) flow, whereas a constant dynamic viscosity is found under the same shear rates in steady shear (SS) flow. We show that this contradiction arises from the underlying microstructural difference between OS and SS, mediated by weak interparticle forces. Discrete element simulations of proxy particle suspensions confirm this hypothesis and reveal an adhesion-induced, shear thinning mech…
Recent experiments report that slowly-sheared noncolloidal particle suspensions can exhibit unexpected rate($ω$)-dependent complex viscosities in oscillatory shear, despite a constant relative viscosity in steady shear. Using a minimal hydrodynamic model, we show that a weak interparticle attraction reproduces this behavior. At volume fractions $ϕ=20\sim50$%, the complex viscosities in both experiments and simulations display power-law reductions in shear, with a $ϕ$-dependent exponent maximum at $ϕ=40$%, resulting from the interplay between hydrodynamic, collision and adhesive interactions. F…
At the same solid volume fraction, bidisperse and polydisperse suspensions display lower viscosities, and weaker normal stress response, compared to monodisperse suspensions. The reduction of viscosity associated with size distribution can be explained by an increase of the maximum flowable, or jamming, solid fraction $ϕ_m$. In this work, dense suspensions are simulated under strong shearing, where thermal motion and repulsive forces are negligible, but we allow for particle contact with a mild frictional interaction with interparticle friction coefficient of $μ = 0.2$. Aspects of bidisperse s…
We present an experimental investigation of shear elastic wave propagation along the surface of a dense granular suspension. Using an ultrafast ultrasound scanner, we monitor the softening of the shear wave velocity inside the optically opaque medium as the driving amplitude increases. For such nonlinear behavior two regimes are found: in the first regime, we observe a significant shear modulus weakening, but without visible grain rearrangements. In the second regime, there is a clear grain rearrangement accompanied by a modulus decrease up to 88%. A friction model is proposed to describe the …
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 dynamic…
We investigate the origin of yield stress aging in semi-dense, saline, and turbid suspensions in which structural evolution is rapidly arrested by the formation of thermally irreversible roll-resisting interparticle contacts. By performing optical tweezer (OT) three-point bending tests on particle rods, we show that these contacts yield by overcoming a rolling threshold, the critical bending moment of which grows logarithmically with time. We demonstrate that this time-dependent contact-scale rolling threshold controls the suspension yield stress and its aging kinetics. We identify a simple co…
We explore the rheology predicted by a recently proposed constitutive model for jammed suspensions of soft elastic particles derived from particle-level dynamics [Cuny et al., Phys. Rev. Lett. 127, 218003 (2021)]. Our model predicts that the orientation of the anisotropy of the microstructure, governed by an interplay between advection 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 s…
The mechanical non-linear response of dense Brownian suspensions of polymer gel particles is studied experimentally and by means of numerical simulations. It is shown that the response to the application of a constant shear rate depends on the previous history of the suspension. When the flow starts from a suspension at rest, it exhibits an elastic response followed by a stress overshoot and then a plastic flow regime. Conversely, after flow reversal, the stress overshoot does not occur, and the apparent elastic modulus is reduced while numerical simulations reveal that the anisotropy of the l…
We experimentally characterize the impact response of concentrated suspensions consisting of cornstarch and water. We observe that the suspensions support a large normal stress -- on the order of MPa -- with a delay after the impactor hits the suspension surface. We show that neither the delay nor the magnitude of the stress can yet be explained by either standard rheological models of shear thickening in terms of steady-state viscosities, or impact models based on added mass or other inertial effects. The stress increase occurs when a dynamically jammed region of the suspension in front of th…
Foams made of complex fluids such as particle suspensions have a great potential for the development of advanced aerated materials. In this paper we study the rheological behavior of liquid foams loaded with granular suspensions. We focus on the effect of small particles, i.e. particle-to-bubble size ratio smaller than 0.1, and we measure the complex modulus as a function of particle size and particle volume fraction. With respect to previous work, the results highlight a new elastic regime characterized by unequaled modulus values as well as independence of size ratio. A careful investigation…
We show that particle roughness leads to changes in the number, shape and resulting capillary force of liquid bridges in capillary suspensions. We created fluorescently labeled, raspberry-like particles with varying roughness by electrostatically adsorbing silica nanoparticles with sizes between 40 nm and 250 nm on silica microparticles. Rougher particles require more liquid to fill the surface asperities before they form pendular bridges, resulting in smaller and weaker bridges. In a system where the effective bridge volume is adjusted, higher particle roughness leads to less clustered networ…
We investigate the rheology of strain-hardening spherical capsules, from the dilute to the concentrated regime under a confined shear flow using three-dimensional numerical simulations. We consider the effect of capillary number, volume fraction and membrane inextensibility on the particle deformation and on the effective suspension viscosity and normal stress differences of the suspension. The suspension displays a shear-thinning behaviour which is a characteristic of soft particles such as emulsion droplets, vesicles, strain-softening capsules, and red blood cells. We find that the membrane …
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…
Optical tweezers (OTs) can detect pico-Newton range forces operating on a colloidal particle trapped in a medium and have been successfully utilized to investigate complex systems with internal structures. Laponite clay particles in an aqueous medium self-assemble to form microscopic networks over time as electrostatic interactions between the particles gradually evolve in a physical aging process. We investigate the forced movements of an optically trapped micron-sized colloidal probe particle, suspended in an aging Laponite suspension, as the underlying Laponite microstructures gradually dev…
Repeated/cyclic shearing can drive amorphous solids to a steady-state encoding a memory of the applied strain amplitude. However, recent experiments find that the effect of such memory formation on the mechanical properties of the bulk material is rather weak. Here we study the memory effect in a yield stress solid formed by a dense suspension of cornstarch particles in paraffin oil. Under cyclic shear, the system evolves towards a steady-state showing training-induced strain stiffening and plasticity. A readout reveals that the system encodes a strong memory of the training amplitude as indic…
Elasticity of soft materials can be greatly influenced by the presence of air bubbles. Such a capillary effect is expected for a wide range of materials, from polymer gels to concentrated emulsions and colloidal suspensions. Whereas experimental results and theory exist for describing the elasto-capillary behavior of bubbly materials (i.e. with moderate gas volume fractions), foamy systems still require a dedicated study in order to increase our understanding of elasticity in aerated materials over the full range of gas volume fractions. Here we elaborate well-controlled foams with concentrate…
We experimentally characterize the impact response of concentrated suspensions of cornstarch and water. We hypothesize that the dynamically jammed region that propagates ahead of the impactor is responsible for the strong stress response to impact when it spans between solid boundaries. Using surface imaging and particle tracking at the boundary opposite the impactor, we observed that a visible structure and particle flow at the boundary occur with a delay after impact. We show the delay time is about the same time as the the strong stress response, confirming that the strong stress response r…
In this paper, we derive the closed form analytical solutions for the effective viscosity of the suspensions of solid spheres that take into account the size effects. This result is obtained using the solution for the effective shear modulus of particulate composites developed in the framework of the strain gradient elasticity theory. Assuming incompressibility of matrix and rigid behavior of particles and using a mathematical analogy between the theory of elasticity and the theory of viscous fluids we derive the generalized Einstein's formula for the effective viscosity. Generalized Brinkman'…
Pressure sensitivity in non-local flow behaviour of dense hydrogel particle suspensions
Van der Waals-Zeeman Institute, Institute of Physics, University of Amsterdam（阿姆斯特丹大学范德瓦耳斯-泽曼研究所物理学院）；Physical Chemistry and Soft Matter, Wageningen University & Research（瓦赫宁根大学与研究物理化学与软物质系）；Institute of Process and Particle Engineering, Graz University of Technology（格拉茨工业大学工艺与颗粒工程研究所）；Department of Mechanical Engineering, Indian Institute of Technology Bombay（印度孟买理工学院机械工程系）；Institute of Physics, Otto von Guericke University Magdeburg（马格德堡奥托·冯·格里克大学物理研究所）；School of Engineering, Brown University（布朗大学工程学院）
The yet virtually unexplored class of soft colloidal rods with small aspect ratio is investigated and shown to exhibit a very rich phase and dynamic behavior, spanning from liquid to nearly melt state. Instead of nematic order, these short and soft nanocylinders alter their organization with increasing concentration from isotropic liquid with random orientation to one with preferred local orientation and eventually a multi-domain arrangement with local orientational order. The latter gives rise to a kinetically suppressed state akin to structural glass with detectable terminal relaxation, whic…
We formulate a microscopic, force-level, activated dynamics-based statistical-mechanical theory for the continuous startup nonlinear shear-rheology of ultra-dense glass-forming hard-sphere fluids and colloidal suspensions in the context of the ECNLE approach. Activated structural relaxation is described as a coupled local-nonlocal event involving caging and longer-range collective elasticity which controls the characteristic stress relaxation time. Theoretical predictions for the deformation-induced mobility enhancement, onset of relaxation acceleration at low values of stress, strain, or shea…
We study the elastic response of concentrated suspensions of rigid wire frame particles to a step strain. These particles are constructed from infinitely thin, rigid rods of length $L$. We specifically compare straight rod-like particles to bent and branched wire frames. In dense suspensions the wire frames are frozen in a disordered state by the topological entanglements between their arms. We present a simple, geometric method to find the scaling of the elastic stress with concentration in these glassy systems. We apply this method to a simple 2D model system where a test particle is placed …
Unified Microscopic Theory of Stress Relaxation, Structural Evolution, and Memory Effects in Dense Glass Forming Brownian Suspensions After Flow Cessation
University of Illinois（伊利诺伊大学）；Department of Materials Science and Engineering, University of Illinois（伊利诺伊大学材料科学与工程系）；Materials Research Laboratory, University of Illinois（伊利诺伊大学材料研究实验室）；Department of Chemistry, University of Illinois（伊利诺伊大学化学系）；Department of Chemical & Biomolecular Engineering, University of Illinois（伊利诺伊大学化学与生物分子工程系）
Protein-stabilised emulsion gels can be studied in the theoretical framework of colloidal gels, because both protein assemblies and droplets may be considered as soft colloids. These particles differ in their nature, size and softness, and these differences may have an influence on the rheological properties of the gels they form. Pure gels made of milk proteins (sodium caseinate), or of sub-micron protein-stabilised droplets, were prepared by slow acidification of suspensions at various concentrations. Their microstructure was characterised, their viscoelasticity, both in the linear and non-l…
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 mod…
We study the elastic response of rigid, wire frame particles in concentrated, glassy suspensions to a step strain by applying the simple, geometric methods developed in part I. The wire frame particles are comprised of thin, rigid rods of length $L$ and their number density, $ρ$, is such that $ρL^3 \gg 1$. We specifically compare rigid rods to L-shapes made of two equal length rods joined at right angles. The behaviour of wire frames is found to be strikingly different from that of rods. The linear elasticity scales like $ρ^3 L^6$ for L-shaped particles, whereas it scales proportional to $ρ$ f…
Fat based pasty products are an essential part of food industries, both as process intermediate or end products. Such materials are made of a continuous fat phase in which solid particles are dispersed. Phenomena such as yield and fracture occur in those materials and depend heavily on the composition of the samples. The crystallization of fat is altered in presence of particle, which leads to products with different physical properties. However, because of the very complex aspect of the problem, very few studies have been trying to characterize the influence of the solid particles on the fina…
Solids deform and fluids flow, but soft glassy materials, such as emulsions, foams, suspensions, and pastes, exhibit an intricate mix of solid and liquid-like behavior. While much progress has been made to understand their elastic (small strain) and flow (infinite strain) properties, such understanding is lacking for the softening and yielding phenomena that connect these asymptotic regimes. Here we present a comprehensive framework for softening and yielding of soft glassy materials, based on extensive numerical simulations of oscillatory rheological tests, and show that two distinct scenario…
