We study the rheology of monodisperse and bidisperse emulsions with various droplet sizes (1 $μ$m -- 2 $μ$m diameter). Above a critical volume fraction $ϕ_c$, these systems exhibit solid-like behavior and a yield stress can be detected. Previous experiments suggest that for small thermal particles, rheology will see a glass transition at $ϕ_c = ϕ_g =0.58$; for large athermal systems, rheology will see a jamming transition at $ϕ_c = ϕ_J =0.64$. However, simulations point out that at the crossover of thermal and athermal regimes, the glass and jamming transitions may both be observed in the same sample. Here we conduct an experiment by shearing four oil-in-water emulsions with a rheometer. We observe both a glass and a jamming transition for our smaller diameter droplets, and only a jamming transition for our larger diameter droplets. The bidisperse sample behaves similarly to the small droplet sample, with two transitions observed. Our rheology data are well-fit by both the Herschel-Bulkley model and the Three Component model. Based on the fitting parameters, our raw rheological data would not collapse onto a master curve. Our results suggest that liquid-solid transitions in dispersions may not be universal, but depend on particle type.
A generalized boundary integral method is developed to investigate the rheology of multiple emulsions with orderly structures up to n layers and up to mi droplets in the i-th layer in microchannels with various geometries. Recently, as fine templates to prepare microcapsules for targeted drug delivery, multiple emulsions with complex structures have been generated through microfluidics. The deformation and breakup of multiple emulsions are critical to the transport and release of their inclusion. However, the numerical investigation of the rheology of multiple emulsions is only limited to a si…
As fine templates to prepare microcapsules, multiple emulsions with complex internal structures have been generated through microfluidics. To study effects of layers, inner droplets and asymmetry of internal structures on rheology of multiple emulsions, a generalized boundary integral method is developed to investigate multiple emulsions with orderly structures up to n layers and up to mi droplets in the i-th layer. Under a modest extensional flow, the complication of internal structures and the collision among inner droplets will subject the particle to stronger shears. However, the particle …
Phenomenon of foam and emulsion jamming at low shear rates is explained by considering the dynamics of thinning in the transient film, formed between the neighboring bubbles and drops. After gradually thinning down to a critical thickness, these films undergo instability transition and thin stepwise, forming the so-called "black films", which are only several nanometers thick and, thereby, lead to stronger adhesion between the dispersed particles. Theoretical analysis shows that such film thickness instability occurs only if the contact time between the bubbles/drops in sheared foam/emulsion i…
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.
We numerically study by lattice Boltzmann simulations the rheological properties of an active emulsion made of a suspension of an active polar gel embedded in an isotropic passive background. We find that the hexatic equilibrium configuration of polar droplets is highly sensitive to both active injection and external forcing and may either lead to asymmetric unidirectional states which break top-bottom symmetry or symmetric ones. In this latter case, for large enough activity, the system develops a shear-thickening regime at low shear rates. Importantly, for larger external forcing a regime wi…
The rheological behaviour of an emulsion made of an active polar component and an isotropic passive fluid is studied by lattice Boltzmann methods. Different flow regimes are found by varying the values of shear rate and extensile activity (occurring, e.g., in microtubule-motor suspensions). By increasing activity, a first transition occurs from linear flow regime to spontaneous persistent unidirectional macro-scale flow, followed by another transition either to (low shear) intermittent flow regime with coexistence of states with positive, negative, and vanishing apparent viscosity, or to (high…
Using confocal microscopy we investigate the effect of attraction on the packing of polydisperse emulsions under gravity. We find that the distributions of neighbors, coordination number, and local packing fraction as a function of attraction are captured by recently proposed geometrical modeling and statistical mechanics approaches to granular matter. This extends the range of applicability of these tools to polydisperse, attractive jammed packings. Furthermore, the dependence of packing density and average coordination number on the strength of attraction provides the first experimental test…
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 show how attractive interactions dramatically influence emulsion rheology. Unlike the repulsive case, attractive emulsions below random close packing, RCP, can form soft gel-like elastic solids. However, above RCP, attractive and repulsive emulsions have similar elasticities. Such compressed attractive emulsions undergo an additional shear-driven relaxation process during yielding. Our results suggest that attractive emulsions begin to yield at weak points through the breakage of bonds, and, above RCP, also undergo droplet configurational rearrangements.
We present local velocity measurements in emulsions under shear using heterodyne Dynamic Light Scattering. Two emulsions are studied: a dilute system of volume fraction $ϕ=20$ % and a concentrated system with $ϕ=75$ %. Velocity profiles in both systems clearly show the presence of wall slip. We investigate the evolution of slip velocities as a function of shear stress and discuss the validity of the corrections for wall slip classically used in rheology. Focussing on the bulk flow, we show that the dilute system is Newtonian and that the concentrated emulsion is shear-thinning. In the latter c…
The aggregation of protein-stabilised emulsions leads to the formation of emulsion gels. These soft solids are classically envisioned as droplet-filled matrices. Here however, it is assumed that protein-coated sub-micron droplets contribute to the network formation in a similar way to proteins. Emulsion gels are thus envisioned as composite networks made of proteins and droplets. Emulsion gels with a wide range of composition are prepared and their viscoelasticity and frequency dependence are measured. Their rheological behaviours are then analysed and compared with the properties of pure gels…
Rheological properties of a dense granular material consisting of frictionless spheres are investigated. It is found that the shear stress, the pressure, and the kinetic temperature obey critical scaling near the jamming transition point, which is considered as a critical point. These scaling laws have some peculiar properties in view of conventional critical phenomena because the exponents depend on the interparticle force models so that they are not universal. It is also found that these scaling laws imply the relation between the exponents that describe the growing correlation length.
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…
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…
We investigate the rheological properties of an assembly of inelastic (but frictionless) particles close to the jamming density using numerical simulation, in which uniform steady states with a constant shear rate $\dotγ$ is realized. The system behaves as a power-law fluid and the relevant exponents are estimated; e.g., the shear stress is proportional to $\dotγ^{1/δ_S}$, where $1/δ_S=0.64(2)$. It is also found that the relaxation time $τ$ and the correlation length $ξ$ of the velocity increase obeying power laws: $τ\sim\dotγ^{-β}$ and $ξ\sim\dotγ^{-α}$, where $β=0.27(3)$ and $α=0.23(3)$.
We investigate the jamming transition in packings of emulsions and granular materials via molecular dynamics simulations. The emulsion model is composed of frictionless droplets interacting via nonlinear normal forces obtained using experimental data acquired by confocal microscopy of compressed emulsions systems. Granular materials are modeled by Hertz-Mindlin deformable spherical grains with Coulomb friction. In both cases, we find power-law scaling for the vanishing of pressure and excess number of contacts as the system approaches the jamming transition from high volume fractions. We find …
We experimentally study the jamming of quasi-two-dimensional emulsions. Our experiments consist of oil-in-water emulsion droplets confined between two parallel plates. From the droplet outlines, we can determine the forces between every droplet pair to within 8% over a wide range of area fractions $ϕ$. We study three bidisperse samples that jam at area fractions $ϕ_c \approx 0.86$. Our data show that for $ϕ> ϕ_c$, the contact numbers and pressure have power-law dependence on $ϕ-ϕ_c$ in agreement with the critical scaling found in numerical simulations. Furthermore, we see a link between the in…
We perform numerical simulations to determine the shear stress and pressure of steady-state shear flow in a soft-disk model in two dimensions at zero temperature in the vicinity of the jamming transition ϕ_J. We use critical point scaling analyses to determine the critical behavior at jamming, and we find that it is crucial to include corrections to scaling for a reliable analysis. We find that the relative size of these corrections are much smaller for pressure than for shear stress. We furthermore find a superlinear behavior for pressure and shear stress above ϕ_J, both from the scaling anal…
The shear-jamming of dense suspensions can be strongly affected by molecular-scale interactions between particles, e.g. by chemically controlling their propensity for hydrogen bonding. However, hydrogen bonding not only enhances interparticle friction, a critical parameter for shear jamming, but also introduces (reversible) adhesion, whose interplay with friction in shear-jamming systems has so far remained unclear. Here, we present atomic force microscopy studies to assess interparticle adhesion, its relationship to friction, and how these attributes are influenced by urea, a molecule that in…
We establish that the rheological curve of dry granular media is non-monotonic, both in the presence and absence of external mechanical agitations. In the presence of weak vibrations, the non-monotonic flow curves govern a hysteretic transition between slow but steady and fast, inertial flows. In the absence of vibrations, the non-monotonic flow curve governs the yielding behavior of granular media. Finally, we show that non-monotonic flow curves can be seen in at least two different flow geometries and for several granular materials.
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…
We investigate the rheology of sheared granular materials near the jamming transition point. We numerically determine the values of the critical fraction and the exponents for the jamming transition using a finite size scaling and the nonlinear minimization method known as the Levenberg-Marquardt algorithm. The exponents are close to our previous theoretical prediction, but there is a small discrepancy, if the critical point is independently determined.
We study granular suspensions under a variety of extensional deformations and simple shear using numerical simulations. The viscosity and Trouton's ratio (the ratio of extensional to shear viscosity) are computed as functions of solids volume fraction $ϕ$ close to the limit of zero inertia. Suspensions of frictionless particles follow a Newtonian Trouton's ratio for $ϕ$ all the way up to $ϕ_0$, a universal jamming point that is independent of deformation type. In contrast, frictional particles lead to a deformation-type-dependent jamming fraction $ϕ_m$, which is largest for shear flows. Trouto…
Amorphous materials as diverse as foams, emulsions, colloidal suspensions and granular media can {\em jam} into a rigid, disordered state where they withstand finite shear stresses before yielding. The jamming transition has been studied extensively, in particular in computer simulations of frictionless, soft, purely repulsive spheres. Foams and emulsions are the closest realizations of this model, and in foams, the (un)jamming point corresponds to the wet limit, where the bubbles become spherical and just form contacts. Here we sketch the relevance of the jamming perspective for the geometry …
We study, by computer simulations, the role of different dissipation forces on the rheological properties of highly-dense particle-laden flows. In particular, we are interested in the close-packing limit (jamming) and the question if "universal" observables can be identified that do not depend on the details of the dissipation model. To this end, we define a simplified lubrication force and systematically vary the range $h_c$ of this interaction. For fixed $h_c$ a cross-over is seen from a Newtonian flow regime at small strain rates to inertia-dominated flow at larger strain rates. The same cr…
We consider the rheology of soft-core frictionless disks in two dimensions in the neighborhood of the athermal jamming transition. From numerical simulations of bidisperse, overdamped, particles, we argue that the divergence of the viscosity below jamming is characteristic of the hard-core limit, independent of the particular soft-core interaction. We develop a mapping from soft-core to hard-core particles that recovers all the critical behavior found in earlier scaling analyses. Using this mapping we derive a duality relation that gives the exponent of the non-linear Herschel-Bulkley rheology…
We present a numerical study of the rheology of a two-fluid emulsion in dilute and semidilute conditions. The analysis is performed for different capillary numbers, volume fraction and viscosity ratio under the assumption of negligible inertia and zero buoyancy force. The effective viscosity of the system increases for low values of the volume fraction and decreases for higher values, with a maximum for about 20 % concentration of the disperse phase. When the dispersed fluid has lower viscosity, the normalised effective viscosity becomes smaller than 1 for high enough volume fractions. To sing…
We study relaxation and rheology of dense athermal suspensions of frictionless particles close below the jamming density. Our key quantity, the relaxation time---determined from the exponential decay of the energy after the shearing has suddenly been switched off---is argued to be a determining factor behind the algebraic divergence of various quantities as the jamming density is approached from below. We also define and measure the ``dissipation time'', which is obtained directly in shearing simulations and find that it behaves similarly to the relaxation time. Comparing shear viscosity with …
We determine the form of the complex shear modulus $G^*$ in soft sphere packings near jamming. Viscoelastic response at finite frequency is closely tied to a packing's intrinsic relaxational modes, which are distinct from the vibrational modes of undamped packings. We demonstrate and explain the appearance of an anomalous excess of slowly relaxing modes near jamming, reflected in a diverging relaxational density of states. From the density of states, we derive the dependence of $G^*$ on frequency and distance to the jamming transition, which is confirmed by numerics.
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…
The effect of a spatially uniform magnetic field on the shear rheology of a dilute emulsion of monodispersed ferrofluid droplets, immersed in a non-magnetizable immiscible fluid, is investigated using direct numerical simulations. The direction of the applied magnetic field is normal to the shear flow direction. The droplets extra stress tensor arising from the presence of interfacial forces of magnetic nature is modeled on the basis of the seminal work of G. K. Batchelor, J. Fluid Mech., 41.3 (1970) under the assumptions of a linearly magnetizable ferrofluid phase and negligible inertia. The …
We investigate the rheology of granular materials via molecular dynamics simulations of homogeneous, simple shear flows of soft, frictional, noncohesive spheres. In agreement with previous results for frictionless particles, we observe three flow regimes existing in different domains of particle volume fraction and shear rate, with all stress data collapsing upon scaling by powers of the distance to the jamming point. Though this jamming point is a function of the interparticle friction coefficient, the relation between pressure and strain rate at this point is found to be independent of frict…
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 …
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 demonstrate that a highly frustrated anisotropic Josephson junction array(JJA) on a square lattice exhibits a zero-temperature jamming transition, which shares much in common with those in granular systems. Anisotropy of the Josephson couplings along the horizontal and vertical directions plays roles similar to normal load or density in granular systems. We studied numerically static and dynamic response of the system against shear, i. e. injection of external electric current at zero temperature. Current-voltage curves at various strength of the anisotropy exhibit universal scaling feature…
We carry out constant volume simulations of steady-state, shear driven, rheology in a simple model of bidisperse, soft-core, frictionless disks in two dimensions, using a dissipation law that gives rise to Bagnoldian rheology. We carry out a detailed critical scaling analysis of our resulting data for pressure $p$ and shear stress $σ$, in order to determine the critical exponent $β$ that describes the algebraic divergence of the Bagnold transport coefficients, as the jamming transition is approached from below. We show that it is necessary, for the strain rates considered in this work, to cons…
The connection between friction and jamming in granular media, molecular glasses, and complex fluids is explored. The paper first reviews the way friction is measured, the types of results that are observed, and what is known about the geometry of contacts between macroscopic surfaces. Then simple models for the origin of static friction are described. These are unable to explain the universal observation of static friction between macroscopic objects. The effects of surface roughness and chemical heterogeneity are discussed, and shown to yield exponentially weak static friction in our three d…
A systematic microscopic theory for the rheology of dense non-Brownian suspensions characterized by the volume fraction $φ$ is developed. The theory successfully derives the critical behavior in the vicinity of the jamming point (volume fraction $φ_{J}$), for both the pressure $P$ and the shear stress $σ_{xy}$, i.e. $P \sim σ_{xy} \sim \dotγη_0 δφ^{-2}$, where $\dotγ$ is the shear rate, $η_0$ is the shear viscosity of the solvent, and $δφ= φ_J - φ> 0$ is the distance from the jamming point. It also successfully describes the behavior of the stress ratio $μ= σ_{xy}/P$ with respect to the viscou…
We attribute similarities in the rheology of many soft materials (foams, emulsions, slurries, etc.) to the shared features of structural disorder and metastability. A generic model for the mesoscopic dynamics of ``soft glassy matter'' is introduced, with interactions represented by a mean-field noise temperature x. We find power law fluid behavior either with (x<1) or without (1<x<2) a yield stress. For 1<x<2, both storage and loss modulus vary with frequency as $ω^{x-1}$, becoming flat near a glass transition (x=1). Values of $x\approx 1$ may result from marginal dynamics as seen in some spin…
Pressure-imposed rheometry is used to examine the influence of surface roughness on the rheology of immersed and dry frictional spheres in the dense regime. The quasi-static value of the effective friction coefficient is not significantly affected by particle roughness while the critical volume fraction at jamming decreases with increasing roughness. These values are found to be similar in immersed and dry conditions. Rescaling the volume fraction by the maximum volume fraction leads to collapses of rheological data on master curves. The asymptotic behaviors are examined close to the jamming t…
Recent advances in shear-thickening suspension rheology suggest a relation between (wet) suspension flow below jamming and (dry) granular physics. To probe this connection, we simulated the contact force networks in suspensions of non-Brownian spheres using the discrete element method (DEM), varying the particle friction coefficient and volume fraction. We find that force networks in these suspensions show quantitative similarities to those in jammed dry grains. As suspensions approach the jamming point, the extrapolated volume fraction and coordination number at jamming are similar to critica…
We study the shearing rheology of dense suspensions of elastic capsules, taking aggregation-free red blood cells as a physiologically relevant example. Particles are non-Brownian and interact only via hydrodynamics and short-range repulsive forces. An analysis of the different stress mechanisms in the suspension shows that the viscosity is governed by the shear elasticity of the capsules, whereas the repulsive forces are subdominant. Evidence for a dynamic yield stress above a critical volume fraction is provided and related to the elastic properties of the capsules. The shear stress is found …
Oscillatory shear has been widely used to study the rheological properties of suspensions under unsteady shear. Furthermore, recent works have shown that oscillatory flows can improve the flowability of dense suspensions. While most studies have been done under constant volume we here study oscillatory shear flows of a two-dimensional suspensions using a normal pressure-controlled set-up. To characterise the rheology, we introduce both a complex macroscopic friction coefficient $μ^{*}$, following the convention of the complex viscosity $η^{*}$, and a shear-rate averaged viscous number $J'$. Th…
Emulsions are a central component of many modern formulations in food, pharmaceuticals, agrichemicals and personal care products. The droplets in these formulations are limited to being spherical as a consequence of the interfacial tension between the dispersed phase and continuous phase. The ability to control emulsion droplet morphology and stabilise non-spherical droplets would enable the modification of emulsion properties such as stability, substrate binding, delivery rate and rheology. One way of controlling droplet microstructure is to apply an elastic film around the droplet to prevent…
