The rheology near jamming of a suspension of soft colloidal spheres is studied using a custom microfluidic rheometer that provides stress versus strain rate over many decades. We find non-Newtonian behavior below the jamming concentration and yield stress behavior above it. The data may be collapsed onto two branches with critical scaling exponents that agree with expectations based on Hertzian contacts and viscous drag. These results support the conclusion that jamming is similar to a critical phase transition, but with interaction-dependent exponents.
This is a comment on the recent letter by Wang and Brady on "Constant stress and pressure rheology of colloidal suspensions", Phys. Rev. Lett. 115, 158301 (2015).
A first principles approach to the nonlinear flow of dense suspensions is presented which captures shear thinning of colloidal fluids and dynamical yielding of colloidal glasses. The advection of density fluctuations plays a central role, suppressing the caging of particles and speeding up structural relaxation. A mode coupling approach is developed to explore these effects.
Using a novel bi-axial confocal rheoscope, we investigate the structure and rheology of sheared colloidal suspensions under confinement. Consistent with previous work [X. Cheng \textit{et al., Proc. Natl. Acad. Sci. U. S. A.}, 2011, 109, 63], we observe a vorticity-aligned string phase in moderate concentrated colloidal suspensions under uniaxial shear. Using bi-axial shear protocols, we directly manipulate the orientation and morphology of the string structures. Simultaneously, we measure the suspension rheology along both the flow and vorticity directions with a bi-axial force measurement de…
Many colloidal systems display very non-Newtonian and solid-like behaviour when concentrated, a striking feature being the apparition of a yield stress. After recalling some basics about the interactions between colloidal particles, I present a few experimental facts commonly observed in these systems: aging and non-linear rheology. A simple phenomenological model is then introduced, in which the local state of the system is described by a single scalar parameter, the fluidity. I proceed with comments on heterogeneous flows in some of these systems. These notes are not intended to be a compreh…
We simulate an experiment in which a colloidal probe is pulled through an active nematic fluid. We find that the drag on the particle is non-Stokesian (not proportional to its radius). Strikingly, a large enough particle in contractile fluid (such as an actomyosin gel) can show negative viscous drag in steady state: the particle moves in the opposite direction to the externally applied force. We explain this, and the qualitative trends seen in our simulations, in terms of the disruption of orientational order around the probe particle and the resulting modifications to the active stress.
Magnetic nanoparticles in a colloidal solution self-assemble in various aligned structures, which has a profound influence on the flow behavior. However, the precise role of the microstructure in the development of the rheological response has not been reliably quantified. We investigate the self-assembly of dipolar colloids in simple shear using hybrid molecular dynamics and multi-particle collision dynamics simulations with explicit coarse-grained hydrodynamics; conduct simulated rheometric studies and apply micromechanical models to produce master curves, showing evidence of the universalit…
The nonlinear rheology of glass-forming colloidal suspensions with short-ranged attractions is discussed within the integration-through transients framework combined with the mode-coupling theory of the glass transition (ITT-MCT). Calculations are based on the square-well system (SWS), as a model for colloid-polymer mixtures. The high-density regime featuring reentrant melting of the glass upon increasing the attraction strength, and the crossover from repulsive glasses formed at weak attraction to attractive glasses formed at strong attraction, are discussed. Flow curves are found in qualitat…
Encapsulation of chemicals using polymer membranes enables to control their transport and delivery for applications such as agrochemistry or detergency. To rationalize the design of polymer capsules, it is necessary to understand how the membranes' mechanical properties control the transport and release of the cargo. In this article, we use microfluidics to produce model polymer capsules and study in situ their behavior in controlled elongational flows. Our model capsules are obtained by assembling polymer mono and hydrogen-bonded bilayers at the surface of an oil droplet in water. We also use…
The flow of colloidal suspensions is ubiquitous in nature and industry. Colloidal suspensions exhibit a wide range of rheological behavior, which should be closely related to the microscopic structure of the systems. With in-situ small-angle neutron scattering complemented by rheological measurements, we investigated the deformation behavior of a charge-stabilized colloidal glass at particle level undergoing steady shear. A short-lived, localized elastic response at particle level, termed as transient elasticity zone (TEZ), was identified from the neutron spectra. The existence of the TEZ is a…
We investigated the viscoelastic properties of colloid-polymer mixtures at intermediate colloid volume fraction and varying polymer concentrations, thereby tuning the attractive interactions. Within the examined range of polymer concentrations, the samples ranged from fluids to gels. Already in the liquid phase the viscoelastic properties significantly changed when approaching the gelation boundary, indicating the formation of clusters and transient networks. This is supported by an increasing correlation length of the density fluctuations, observed by static light scattering and microscopy. A…
The effects of the addition of sub-micrometer sized colloidal silica spheres on the linear and nonlinear rheology of semi-dilute solutions of a viscoelastic gel are studied. For a 1.4 wt.% solution of the surfactant CTAT, a peak in the zero shear rate viscosity $η_{\circ}$ is observed at approximately equal weight percents of silica and CTAT. This peak shifts to lower silica concentrations on increasing either the CTAT concentration or the surface charge on silica and disappears when the CTAT concentration is increased to 2.6wt%. The increases in $η_{\circ}$ and the high frequency plateau modu…
Using a combination of theory, experiment and simulation we investigate the nonlinear response of dense colloidal suspensions to large amplitude oscillatory shear flow. The time-dependent stress response is calculated using a recently developed schematic mode-coupling-type theory describing colloidal suspensions under externally applied flow. For finite strain amplitudes the theory generates a nonlinear response, characterized by significant higher harmonic contributions. An important feature of the theory is the prediction of an ideal glass transition at sufficiently strong coupling, which is…
A discussion on the viscoelastic properties of weakly attractive colloids and the relation to a newly developed percolation theory is presented. The need for taking into account the particle-particle bond lifetime in order to compare rheological and percolation estimates of the sol-gel transition is stressed. Recent molecular dynamics simulations and generalised percolation theory that use a bond lifetime criterion in the definition of aggregates show that the percolation transition can be reconciled with the rheological sol-gel transition. The percolation concept is used here as a "measuring"…
Long-range hydrodynamics between colloidal particles or fibers is modelled by the Fluid Particle Model. Two methods are considered to impose the fluid boundary conditions at colloidal surfaces. In the first method radial and transverse friction forces between particle and solvent are applied such that the correct friction and torque follows for moving or rotating particles. The force coefficients are calculated analytically and checked by numerical simulation. In the second method a collision rule is used between colloidal particle and solvent particle that imposes the stick boundary condition…
We provide a detailed derivation of a recently developed first-principles approach to calculating averages in systems of interacting, spherical Brownian particles under time-dependent flow. Although we restrict ourselves to flows which are both homogeneous and incompressible, the time-dependence and geometry (e.g. shear, extension) are arbitrary. The approximations formulated within mode-coupling theory are particularly suited to dense colloidal suspensions and capture the slow relaxation arising from particle interactions and the resulting glass transition to an amorphous solid. The delicate …
A comprehensive study is presented on the short-time dynamics in suspensions of charged colloidal spheres. The explored parameter space covers the major part of the fluid-state regime, with colloid concentrations extending up to the freezing transition. The particles are assumed to interact directly by a hard-core plus screened Coulomb potential, and indirectly by solvent-mediated hydrodynamic interactions (HIs). By comparison with accurate accelerated Stokesian Dynamics (ASD) simulations of the hydrodynamic function H(q), and the high-frequency viscosity, we investigate the accuracy of two fa…
The rheology of suspensions of Brownian, or colloidal, particles (diameter $d \lesssim 1$ $μ$m) differs markedly from that of larger grains ($d \gtrsim 50$ $μ$m). Each of these two regimes has been separately studied, but the flow of suspensions with intermediate particle sizes (1 $μ\textrm{m} \lesssim d \lesssim 50$ $μ$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 intermedia…
We present an experimental study of the rheology and structure of a confined suspension of deformable particles flowing in a quasi-two-dimensional Poiseuille flow. Thanks to a precise microfluidic viscosimetry technique combined with measurements of concentration profiles, our study provides the first experimental confirmation {with three-dimensional particles} of a strong relationship between structuring effects and rheology, previously only reported in numerical simulations of purely two-dimensional systems. In conditions where strong structuring effects take place due to confinement, the ev…
We introduce a class of simple models for shear thickening and/ or `jamming' in colloidal suspensions. These are based on schematic mode coupling theory (MCT) of the glass transition, having a memory term that depends on a density variable, and on both the shear stress and the shear rate. (Tensorial aspects of the rheology, such as normal stresses, are ignored for simplicity.) We calculate steady-state flow curves and correlation functions. Depending on model parameters, we find a range of rheological behaviours, including `S-shaped' flow curves, indicating discontinuous shear thickening, and …
Mode coupling theory (MCT) has had notable successes in addressing the rheology of hard-sphere colloidal glasses, and also soft colloidal glasses such as star-polymers. Here, we explore the properties of a recently developed MCT-based schematic constitutive equation under idealized experimental protocols involving single and then double step strains. We find strong deviations from expectations based on factorable, BKZ-type constitutive models. Specifically, a nonvanishing stress remains long after the application of two equal and opposite step strains; this residual stress is a signature of pl…
In the vicinity of their glass transition, dense colloidal suspensions acquire elastic properties over experimental timescales. We investigate the possibility of a visco-elastic flow instability in curved geometry for such materials. To this end, we first present a general strategy extending a first-principles approach based on projections onto slow variables (so far restricted to strictly homogeneous flow) in order to handle inhomogeneities. In particular, we separate the advection of the microstructure by the flow, at the origin of a fluctuation advection term, from the intrinsic dynamics. O…
Dense suspensions of soft colloidal particles display a broad range of physical and rheological properties which are still far from being fully understood. To elucidate the role of deformability on colloidal flow, we employ computer simulations to measure the apparent viscosity of a system of droplets of variable surface tension subjected to a pressure-driven flow. We confirm that our suspension generically undergoes discontinuous shear thinning, and determine the dependence of the onset of the discontinuity on surface tension. We find that the effective viscosity of the suspension is mainly d…
We report studies of the frequency dependent shear modulus, $G^*(ω)=G'(ω)+iG''(ω)$, 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, $G^*(ω) \sim ω^α$, with exponent $α$ that approaches zero with increasing gel density. The amplitude of $G'$ and its variation with temperature and gel density indicate that the l…
Mechanical properties of the cell are important biomarkers for probing its architectural changes caused by cellular processes and/or pathologies. The development of microfluidic technologies have enabled measuring cell mechanics at high-throughput, so that mechanical phenotyping can be applied to large samples in reasonable time-scales. These studies typically measure the stiffness of the cell as the only mechanical biomarker, and cannot disentangle the rheological contribution of different structural components of the cell, including the cell cortex, the interior cytoplasm and its immersed cy…
When a rigid object approaches a soft material in a viscous fluid, hydrodynamic stresses arise in the lubricated contact region and deform the soft material. The elastic deformation modifies in turn the flow, hence generating a soft-lubrication coupling. Moreover, soft elastomers and gels are often porous. These materials may be filled with solvent or uncrosslinked polymer chains, and might be permeable to the surrounding fluid, which complexifies further the description. Here, we derive the point-force response of a semi-infinite and permeable poroelastic substrate. Then, we use this fundamen…
Magnetic fields and magnetic materials have promising microfluidic applications. For example, magnetic micro-convection can enhance mixing considerably. However, previous studies have not explained increased effective diffusion during this phenomenon. Here we show that enhanced interface smearing comes from a gravity induced convective motion within a thin microfluidic channel, caused by a small density difference between miscible magnetic and non-magnetic fluids. This motion resembles diffusive behavior and can be described with an effective diffusion coefficient. We explain this with a theor…
Using mode-coupling theory, we derive a constitutive equation for the nonlinear rheology of dense colloidal suspensions under arbitrary time-dependent homogeneous flow. Generalizing previous results for simple shear, this allows the full tensorial structure of the theory to be identified. Macroscopic deformation measures, such as the Cauchy-Green tensors, thereby emerge. So does a direct relation between the stress and the distorted microstructure, illuminating the interplay of slow structural relaxation and arbitrary imposed flow. We present flow curves for steady planar and uniaxial elongati…
Extensional rheometry of mobile fluids. Part II: Comparison between the uniaxial, planar and biaxial extensional rheology of dilute polymer solutions using numerically-optimized stagnation point microfluidic devices
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…
The phase behaviour of soft colloids has attracted great attention due to the large variety of new phenomenologies emerging from their ability to pack at very high volume fractions. Here we report rheological measurements on interpenetrated polymer network microgels composed of poly(Nisopropylacrylamide) (PNIPAM) and polyacrylic acid (PAAc) at fixed PAAc content as a function of weight concentration. We found three different rheological regimes characteristic of three different states: a Newtonian shear-thinning fluid, an attractive glass characterized by a yield stress, and a jamming state. W…
There is now convincing evidence that inter-particle frictional contacts are essential for observing shear-thickening in concentrated suspensions of compact particles. While this has inspired many strategies to tailor the rheology in these systems, in the more general case, viz-a-viz suspensions of anisotropic particles, the mechanism of shear-thickening remains unclear. Here through simultaneous measurements of the bulk viscosity and the first Normal stress difference, we show that strong shear thickening in suspensions of colloidal rods is accompanied by large positive normal stresses, indic…
We study the steady-state response to applied stress in a simple scalar model of sheared colloids. Our model is based on a schematic (F2) model of the glass transition, with a memory term that depends on both stress and shear rate. For suitable parameters, we find transitions from a fluid to a nonergodic, jammed state, showing zero flow rate in an interval of applied stress. Although the jammed state is a glass, we predict that jamming transitions have an analytical structure distinct from that of the conventional mode coupling glass transition. The static jamming transition we discuss is also…
We explore numerically the shear rheology of soft repulsive particles at large volume fraction. The interplay between viscous dissipation and thermal motion results in multiple rheological regimes encompassing Newtonian, shear-thinning and yield stress regimes near the `colloidal' glass transition when thermal fluctuations are important, crossing over to qualitatively similar regimes near the `jamming' transition when dissipation dominates. In the crossover regime, glass and jamming sectors coexist and give complex flow curves. Although glass and jamming limits are characterized by similar mac…
We construct colloidal ``sticky'' rods from the semi-flexible filamentous fd virus and temperature-sensitive polymers poly(N-isopropylacrylamide) (PNIPAM). The phase diagram of fd-PNIPAM system becomes independent of ionic strength at high salt concentration and low temperature, i.e. the rods are sterically stabilized by the polymer. However, the network of sticky rods undergoes a sol-gel transition as the temperature is raised. The viscoelastic moduli of fd and fd-PNIPAM suspensions are compared as a function of temperature, and the effect of ionic strength on the gelling behavior of fd-PNIPA…
The shear rheology of soft particles systems becomes complex at large density because crowding effects may induce a glass transition for Brownian particles, or a jamming transition for non-Brownian systems. Here we successfully explore the hypothesis that the shear stress contributions from glass and jamming physics are `additive'. We show that the experimental flow curves measured in a large variety of soft materials (colloidal hard spheres, microgel suspensions, emulsions, aqueous foams) as well as numerical flow curves obtained for soft repulsive particles in both thermal and athermal limit…
We investigate the nonlinear rheological behavior of colloidal suspensions of Laponite, a synthetic clay, driven by a steady and homogeneous shear strain. We show that the external drive leads to a drastic slowing down of the aging dynamics or even, in some cases, in the rejuvenation of the system. Under shear, after a surprisingly long time, the spontaneous aging process observed at rest is suppressed. The system then reaches a non-equilibrium stationary state, characterised by a complex viscosity depending on the applied shear rate. In addition, the glass exhibits a non-Newtonian shear-thinn…
Concentrated particulate suspensions, commonplace in the pharmaceutical, cosmetic and food industries, display intriguing rheology. In particular, the dramatic increase in viscosity with strain rate (shear thickening and jamming) which is often observed at high volume fractions, is of strong practical and fundamental importance. Yet manufacture of these products and their subsequent dispensing often involves flow geometries substantially different from that of simple shear flow experiments. Here we show that the elongation and breakage of a filament of a colloidal fluid under tensile loading i…
We report on experiments that consist in deforming a collection of monodisperse droplets produced by a microfluidic chip through a flow-focusing device. We show that a proper numerical modelling of the flow is necessary to access the stress applied by the latter on the droplet along its trajectory through the chip. This crucial step enables the full integration of the differential equation governing the dynamical deformation, and consequently the robust measurement of the interfacial tension by fitting the experiments with the calculated deformation. Our study thus demonstrates the feasibility…
We report contactless measurements of the viscoelastic rheological properties of soft gels. The experiments are performed using a colloidal-probe Atomic Force Microscope (AFM) in a liquid environment and in dynamic mode. The mechanical response is measured as a function of the liquid gap thickness for different oscillation frequencies. Our measurements reveal an elastohydrodynamic (EHD) coupling between the flow induced by the probe oscillation and the viscoelastic deformation of the gels. The data are quantitatively described by a viscoelastic lubrication model. The frequency-dependent storag…
We explore the influence of particle softness and internal structure on both the bulk and interfacial rheological properties of colloidal suspensions. We probe bulk stresses by conventional rheology, by measuring the flow curves, shear stress vs strain rate, for suspensions of soft, deformable microgel particles and suspensions of near hard-sphere-like silica particles. A similar behavior is seen for both kind of particles in suspensions at concentrations up to the random close packing volume fraction, in agreement with recent theoretical predictions for sub-micron colloids. Transient interfac…
We investigate the dynamics of kinetically frozen block copolymer micelles of different softness across a wide range of particle concentrations, from the fluid to the onset of glassy behavior, through a combination of rheology, dynamic light scattering and pulsed field gradient NMR spectroscopy. We additionally perform Brownian dynamics simulations based on an ultrasoft coarse-grained potential, which are found to be in quantitative agreement with experiments, capturing even the very details of dynamic structure factors S(Q, t) on approaching the glass transition. We provide evidence that for …
We discuss the linear and non-linear rheology of concentrated (sub)microscale emulsions, amorphous disordered solids composed of repulsive and deformable soft colloidal spheres. Based on recent results from simulation and theory, we derive quantitative predictions for the dependences of the elastic shear modulus and the yield stress on the droplet volume fraction. The remarkable agreement with experiments we observe supports the scenario that the repulsive glass and the jammed state can be clearly identified in the rheology of soft spheres at finite temperature while crossing continuously from…
Colloidal suspensions have a rich rheology and can exhibit shear-thinning as well as shear-thickening. Numerical simulations recently suggested that shear-thickening may be attributed to the inertia of the colloids, besides the hydrodynamic interactions between them. Here, we consider the ideal limit of a dense bath of soft colloids following an underdamped Langevin dynamics. We use a mean-field equation for the colloidal density to get an analytical expression of the drag force felt by a probe pulled at constant velocity through the suspension. Our results show that inertia can indeed induce …
As a paradigmatic model of active fluids, bacterial suspensions show intriguing rheological responses drastically different from their counterpart colloidal suspensions. Although the flow of bulk bacterial suspensions has been extensively studied, the rheology of bacterial suspensions under confinement has not been experimentally explored. Here, using a microfluidic viscometer, we systematically measure the rheology of dilute E. coli suspensions under different degrees of confinement. Our study reveals a strong confinement effect: the viscosity of bacterial suspensions decreases substantially …
We present a comprehensive study of the slip and flow of concentrated colloidal suspensions using cone-plate rheometry and simultaneous confocal imaging. In the colloidal glass regime, for smooth, non-stick walls, the solid nature of the suspension causes a transition in the rheology from Herschel-Bulkley (HB) bulk flow behavior at large stress to a Bingham-like slip behavior at low stress, which is suppressed for sufficient colloid-wall attraction or colloid-scale wall roughness. Visualization shows how the slip-shear transition depends on gap size and the boundary conditions at both walls an…
