Yield-stress materials, which require a sufficiently large forcing to flow, are currently ill-understood theoretically. To gain insight into their yielding transition, here we study numerically the rheology of a suspension of deformable droplets under pressure-driven flow. We show that the suspension displays yield-stress behaviour, with the droplets remaining motionless when the applied body-force is below a critical value. In the non-flowing phase, droplets jam to form an amorphous structure, whereas they order in the flowing phase. Yielding is linked to a percolation transition in the contacts of droplet-droplet overlaps, and requires suitable wetting boundary conditions and strict conservation of the droplet area to exist. Close to the yielding transition, we find strong oscillations in the droplet motion which closely resemble those found experimentally in confined colloidal glasses under flow. We show that even when droplets are static the underlying solvent moves by permeation, so that the viscosity of the composite system is never truly infinite, and, as we discuss, its precise value ceases to be a bulk material property of the system.
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…
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 study the rheology of a suspension of soft deformable droplets subjected to a pressure-driven flow. Through computer simulations, we measure the apparent viscosity as a function of droplet concentration and pressure gradient, and provide evidence of a discontinuous shear thinning behaviour, which occurs at a concentration-dependent value of the forcing. We further show that this response is associated with a nonequilibrium transition between a `hard' (or less deformable) phase, which is nearly jammed and flows very slowly, and a `soft' (or more deformable) phase, which flows much more easil…
We analyze a suspension of deformable particles in a pressure-driven flow. The suspension is composed of neutrally buoyant initially spherical particles and a Newtonian carrier fluid, and the flow is solved by means of direct numerical simulations, using a fully Eulerian method based on a one-continuum formulation. The solid phase is modeled with an incompressible viscous hyperelastic constitutive relation, and the flow is characterized by three main dimensionless parameters, namely the solid volume fraction, the Reynolds and capillary numbers. The dependency of the effective viscosity on thes…
We numerically investigate the morphology and disclination line dynamics of active nematic droplets in three dimensions. Although our model only incorporates the simplest possible form of achiral active stress, active nematic droplets display an unprecedented range of complex morphologies. For extensile activity finger-like protrusions grow at points where disclination lines intersect the droplet surface. For contractile activity, however, the activity field drives cup-shaped droplet invagination, run-and-tumble motion or the formation of surface wrinkles. This diversity of behaviour is explai…
When a droplet is generated, the ligament connecting the drop to the nozzle thins down and eventually pinches off. Adding solid particles to the liquid phase leads to a more complex dynamic, notably by increasing the shear viscosity. Moreover, it introduces an additional length scale to the system, the diameter of the particles, which eventually becomes comparable to the diameter of the ligament. In this paper, we experimentally investigate the thinning and pinch-off of drops of suspensions with two different sizes of particles. We characterize the thinning for different particle size ratios a…
We examine the shape of droplets atop deformable thin elastomeric films prepared with an anisotropic tension. As the droplets generate a deformation in the taut film through capillary forces, they assume a shape that is elongated along the high tension direction. By measuring the contact line profile, the tension in the membrane can be completely determined. Minimal theoretical arguments lead to predictions for the droplet shape and membrane deformation that are in excellent agreement with the data. On the whole, the results demonstrate that droplets can be used as probes to map out the stress…
We analyze fluctuations of particle displacements and stresses in a sheared athermal suspension of elastic capsules (red blood cells). Upon variation of the volume fraction from the dilute up to the highly concentrated regime, our numerical simulations reveal different characteristic power-law regimes of the fluctuation variances and relaxation times. In the jammed phase and at high shear rates, anomalous scaling exponents are found that deviate from pure dimensional predictions. The observed behavior is rationalized via kinetic arguments and a dissipation balance model that takes into account…
We investigate imbibition of a monodisperse emulsion into a low-aspect ratio microfluidic channel with the height h comparable to the droplet diameter d. For confinement ratio d/h = 1.2, the tightly confined disk-like droplets in the channel move more slowly compared to the average suspension velocity. Behind the meniscus that drives the imbibition, there is a droplet-free region, separated from the suspension region by a sharp concentration front. The suspension exhibits strong droplet density and velocity fluctuations, but on average, the suspension domain remains uniform. For weaker confine…
The structural evolution of suspensions upon freezing is studied with optical microscopy in a suspended droplet configuration. Droplets have millimeter size and consist in an aqueous mixture of silica particles while the surroundings phase is hexane. Freeze-thaw cycles are applied to this system and a two-step freezing mechanism evidenced. A fast adiabatic growth of dendrites that invade the full droplets is first observed, and occurs within a few milliseconds. Then a slow process lasts for several seconds and corresponds to the release of solidification latent heat into the hexane phase. The …
We investigate the 3D structure and drying dynamics of complex mixtures of emulsion droplets and colloidal particles, using confocal microscopy. Air invades and rapidly collapses large emulsion droplets, forcing their contents into the surrounding porous particle pack at a rate proportional to the square of the droplet radius. By contrast, small droplets do not collapse, but remain intact and are merely deformed. A simple model coupling the Laplace pressure to Darcy's law correctly estimates both the threshold radius separating these two behaviors, and the rate of large-droplet evacuation. Fin…
We develop a lattice gas model for the drying of droplets of a nanoparticle suspension on a planar surface, using dynamical density functional theory (DDFT) to describe the time evolution of the solvent and nanoparticle density profiles. The DDFT assumes a diffusive dynamics but does not include the advective hydrodynamics of the solvent, so the model is relevant to highly viscous or near to equilibrium systems. Nonetheless, we see an equivalent of the coffee-ring stain effect, but in the present model it occurs for thermodynamic rather the fluid-mechanical reasons. The model incorporates the …
The equilibrium properties of polymer droplets on a soft deformable surface are investigated by molecular dynamics simulations of a bead-spring model. The surface consists of a polymer brush with irreversibly end-tethered linear homopolymer chains onto a flat solid substrate. We tune the softness of the surface by varying the grafting density. Droplets are comprised of bead-spring polymers of various chain lengths. First, both systems, brush and polymer liquid, are studied independently in order to determine their static and dynamic properties. In particular, using a numerical implementation o…
The deposition of particles on a substrate by drying a colloidal suspension droplet is at the core of applications ranging from traditional printing on paper to printable electronics or photovoltaic devices. The self-pinning induced by the accumulation of particles at the contact line plays an important role in the formation of the deposition. In this paper, we investigate both numerically and theoretically, the effect of friction between the particles and the substrate on the deposition pattern. Without friction, the contact line shows a stick-slip behaviour and a dot-like deposit is left aft…
We experimentally investigated the splashing of dense suspension droplets impacting a solid surface, extending prior work to the regime where the viscosity of the suspending liquid becomes a significant parameter. The overall behavior can be described by a combination of two trends. The first one is that the splashing becomes favored when the kinetic energy of individual particles at the surface of a droplet overcomes the confinement produced by surface tension. This is expressed by a particle-based Weber number $We_p$. The second is that splashing is suppressed by increasing the viscosity of …
Exploring the role of hydrodynamic interactions in spherically-confined drying colloidal suspensions
Auburn University（奥本大学）；Leibniz-Institut für Polymerforschung Dresden e.V.（德累斯顿莱布尼茨聚合物研究所）；Technische Universität Dresden（德累斯顿工业大学）；Johannes Gutenberg University Mainz（美因茨约翰内斯·古腾堡大学）
Phase separation can drive spatial organization of multicomponent mixtures. For instance in developing animal embryos, effective phase separation descriptions have been used to account for the spatial organization of different tissue types. Similarly, separation of different tissue types and the emergence of a polar organization is also observed in cell aggregates mimicking early embryonic axis formation. Here, we describe such aggregates as deformable two-phase fluid droplets, which are suspended in a fluid environment (third phase). Using hybrid finite-volume Lattice-Boltzmann simulations, w…
The method of formation of nanoparticle aggregates such as high-coverage spherical shells of microspheres or 3-D micro crystals grown in the geometry unaffected by a substrate is described. In the reported experiment, the evaporation of single levitated water droplet containing 200 nm diameter polystyrene spheres was studied. Successive stages of the drying process were discussed by analyzing the intensity of light elastically scattered by the evaporating droplet. The numerically simulated self-assembly coincides nicely with the observed morphologies resulting from transformation of a droplet …
Young's law fails on soft solid and liquid substrates where there are substantial deformations near the contact line. On liquid substrates, this is captured by Neumann's classic analysis, which provides a geometrical construction for minimising the interfacial free energy. On soft solids, the total free energy includes an additional contribution from elasticity. A linear-elastic model incorporating an out-of-plane restoring force due to solid surface tension was recently shown to accurately predict the equilibrium shape of a thin elastic film due to a large sessile droplet. Here, we extend thi…
Immiscible contaminants are commonly involved in naturally occurring suspensions. The resulting variations of their flow behavior has rarely been evaluated. Here, we investigate the variation of the viscosity of the oil-based two-phase suspension over a period of two years, which is exposed to the ambient air at the production stage. We find that the air's absolute humidity, which strongly varies with the seasons, causes exchanges of water droplets with the suspension, substantially altering its shear-thinning behavior. Only in winter, when the humidity is low, is the latter close to that of i…
During detachment of a viscous fluid extruded from a nozzle a filament linking the droplet to the latter is formed. Under the effect of surface tension the filament thins until pinch off and final detachment of the droplet. In this paper we study the effect of the presence of individual particles trapped in the filament on the detachment dynamics using granular suspensions of small volume fractions (ϕ < 6%). We show that even a single particle strongly modifies the detachment dynamics. The particle perturbs the thinning of the thread and a large droplet of fluid around the particle is formed. …
Using absorbance measurements through a Couette cell containing an emulsion of buoyant droplets, volume fraction profiles are measured at various shear rates. These viscous resuspension experiments allow a direct determination of the normal stress in the vorticity direction in connection with the suspension balance model that has been developed for suspensions of solid particles. The results unambigously show that the normal viscosity responsible for the shear-induced migration of the droplets is independant on the capillary number, implying that particle deformation does not play a great role…
Persistence of Coffee-Ring Deposits in Concentrated Suspensions of Anisotropic Colloids
Department of Physics, Brandeis University（布兰迪斯大学物理系）；Department of Physics and Astronomy, Northwestern University（西北大学物理与天文学系）；Applied Mathematics and Statistics, Colorado School of Mines（科罗拉多矿业大学应用数学与统计学系）
Understanding flow patterns and coupled transport phenomena during evaporation of droplets loaded with colloidal particles is central to design technical applications such as organizing proteins/DNA on a solid surface. We review recent reports on evaporating sessile droplets of colloidal suspensions on a solid surface. Starting from the classical mechanism of formation of a ring-like deposit, we discuss the influence of several problem parameters. Notably, thermal or solutal Marangoni effect, particle size, particle concentration, particle shape, substrate wettability, pH of the suspension etc…
The wetting of solid surfaces can be manoeuvred by altering the energy balance at the interfacial region. While electric field acts favourably to spread a droplet on a rigid surface, this tendency may be significantly suppressed over soft surfaces, considering a part of the interfacial energy being utilized to deform the solid elastically by capillary forces. Here, we bring out a unique mechanism by virtue of which addition of nano-particles to the droplet brings in a favourable recovery of the electro-spreading characteristics of a soft surface, by realizing an alteration in the effective die…
Liquid marbles, which are droplets coated with a hydrophobic powder, were exposed to a uniform electric field. It was established that a threshold value of the electric field, 15 cgse, should be surmounted for deformation of liquid marbles. The shape of the marbles was described as a prolate spheroid. The semi-quantitative theory describing deformation of liquid marbles in a uniform electric field is presented. The scaling law relating the radius of the contact area of the marble to the applied electric field shows a satisfactory agreement with the experimental data.
A convolutional neural network technique for online tracking of the radius evolution of levitating evaporating microdroplets of pure liquids, liquid mixtures and suspensions
We analyse the stability of virus-carrying particles in air at equilibrium after the dissipation of the initial turbulent process produced by sneezing, coughing, breathing or speaking. Because the viruses are expelled mainly attached to small droplets, with diverse sizes and weights, and the external environmental conditions can also be diverse, the subsequent motion spannes different spatial and temporal scales. For droplet sizes larger than $100\,μm$, computing the time of decay to the ground and the distance travelled with a simple free fall model with empirical data extracted from the lite…
In most practical situations, active particles are affected by their environment, for example, by a chemical concentration gradient, light intensity, gravity, or confinement. In particular, the effect of an external flow field is important for particles swimming in a solvent fluid. For deformable active particles such as self-propelled liquid droplets and active vesicles, as well as microorganisms such as euglenas and neutrophils, a general description has been developed by focusing on shape deformation. In this review, we present our recent studies concerning the dynamics of a single active d…
We study suspensions of rigid particles in a plane Couette flow with deformable elastic walls. We find that, in the limit of vanishing inertia, the elastic walls induce shear thinning of the suspension flow such that the effective viscosity decreases as the wall deformability increases. This shear-thinning behavior originates from the interactions between rigid particles, soft wall and carrier fluid; an asymmetric wall deformation induces a net lift force acting on the particles which therefore migrate towards the bulk of the channel. Based on our observations, we provide a closure for the sus…
Suspensions of non-Brownian rods: droplet pinch-off, onset of heterogeneity and effective extensional viscosity
PMMH, CNRS, ESPCI Paris, Sorbonne Université, Université Paris-Cité（PMHH，法国国家科学研究中心，巴黎高等物理化工学院，索邦大学，巴黎 Cité 大学）；Department of Mechanical Engineering, University of California, Santa Barbara（加州大学圣塔芭芭拉分校机械工程系）；Institute of Physics, University of Amsterdam（阿姆斯特丹大学物理研究所）；Department of Mechanical Engineering, University of Maryland（马里兰大学机械工程系）；Department of Chemical and Biomolecular Engineering, University of Maryland（马里兰大学化学与生物分子工程系）
When colloidal suspensions dry, stresses build up and cracks often occur - a phenomenon undesirable for important industries such as paint and ceramics. We demonstrate an effective method which can completely eliminate cracking during drying: by adding emulsion droplets into colloidal suspensions, we can systematically decrease the amount of cracking, and eliminate it completely above a critical droplet concentration. Since the emulsion droplets eventually also evaporate, our technique achieves an effective function while making little changes to the component of final product, and may therefo…
We show how resonant (near-field) coupling affects wave transport in disordered media through ultrasonic experiments in concentrated suspensions. The samples consist of resonant emulsions in which oil droplets are suspended in a liquid gel. By varying the droplet concentration, the limits of the Independent Scattering Approximation are experimentally demonstrated. For the most concentrated samples, the proximity of resonant scatterers induces a renormalization of the surrounding medium, leading to a reducing of scattering strength. We point out an optimal volume fraction of oil droplets for wh…
Interfacially arrested melting in thin films: capillarity-driven suspension of phase transitions
Zhejiang Key Laboratory of Extreme Environment Functional Materials, Yiwu Research Institute of Fudan University（复旦大学义乌研究院极端环境功能材料浙江省重点实验室）；Shanghai Frontiers Science Research Base of Intelligent Optoelectronics and Perception, Institute of Optoelectronics, Fudan University（复旦大学光电研究院上海智能光电子与感知前沿科学基地）；Max Planck Institute of Colloids and Interfaces（马克斯·普朗克胶体与界面研究所）
Discrete simulation methods are efficient tools to investigate the complex behaviors of complex fluids made of either dry granular materials or dilute suspensions. By contrast, materials made of soft and/or concentrated units (emulsions, foams, vesicles, dense suspensions) can exhibit both significant elastic particle deflections (Hertz-like response) and strong viscous forces (squeezed liquid). We point out that the gap between two particles is then not determined solely by the positions of their centers, but rather exhibits its own dynamics. We provide a new discrete numerical method, named …
The motion of a deformable active particle in linear shear flow is explored theoretically. Based on symmetry considerations, in two spatial dimensions, we propose coupled nonlinear dynamical equations for the particle position, velocity, deformation, and rotation. In our model, both, passive rotations induced by the shear flow as well as active spinning motions, are taken into account. Our equations reduce to known models in the two limits of vanishing shear flow and vanishing particle deformability. For varied shear rate and particle propulsion speed, we solve the equations numerically and ob…
Deformability is a central feature of many types of microswimmers, e.g. for artificially generated self-propelled droplets. Here, we analyze deformable bead-spring microswimmers in an externally imposed solvent flow field as simple theoretical model systems. We focus on their behavior in a circular swirl flow in two spatial dimensions. Linear (straight) two-bead swimmers are found to circle around the swirl with a slight drift to the outside with increasing activity. In contrast to that, we observe for triangular three-bead or square-like four-bead swimmers a tendency of being drawn into the s…
Suspensions of spherical active particles often show microphase separation. At a continuum level, coupling their scalar density to fluid flow, there are two distinct explanations. Each involves an effective interfacial tension: the first mechanical (causing flow) and the second diffusive (causing Ostwald ripening). Here we show how the negative mechanical tension of contractile swimmers creates, via a self-shearing instability, a steady-state life cycle of droplet growth interrupted by division whose scaling behavior we predict. When the diffusive tension is also negative, this is replaced by …
The flow of deformable particles, such as droplets, dragged by a fluid, through a network of narrow pores inside rocks or other porous media is key in a range of applications, from enhanced oil recovery and water filtration to lab on a chip sorting of cells. The collective dynamics and its impact on the flow are poorly understood. Here, using droplets as a prototype, we show that collective transport can occur for conditions under which a single particle would get trapped at a pore channel. When a series of droplets gets trapped, the fluids flow is affected significantly, leading to an increas…
Active particles, including swimming microorganisms, autophoretic colloids and droplets, are known to self-organize into ordered structures at fluid-solid boundaries. The entrainment of particles in the attractive parts of their spontaneous flows has been postulated as a possible mechanism underlying this phenomenon. Here, combining experiments, theory and numerical simulations, we demonstrate the validity of this flow-induced ordering mechanism in a suspension of active emulsion droplets. We show that the mechanism can be controlled, with a variety of resultant ordered structures, by simply a…
Jamming is a fundamental transition that governs the mechanical behavior of particulate media, including sand, foam and dense suspensions but also biological tissues: Upon compression, particulate media can change from freely flowing to a disordered solid. Jamming has previously been conceived as a bulk phenomenon involving particle motions in fixed geometries. In a diverse class of soft materials, however, solidification can take place in a deformable geometry, such as on the surface of a fluid droplet or in the formation of a bijel. In these systems the nature and dynamics of jamming remains…
The fragmentation of liquid sheets produces a collection of droplets. The size distribution of the droplets has a considerable impact on the coating efficiency of sprays and the transport of contaminants. Although many processes commonly used particulate suspensions, the influence of the particles on the spreading dynamics of the sheet and its subsequent fragmentation has so far been considered negligible. In this paper, we consider experimentally a transient suspension sheet that expands radially. We characterize the influence of the particles on the dynamics of the liquid sheet and the fragm…
Numerous experimental and computational studies show that continuous hopper flows of granular materials obey the Beverloo equation that relates the volume flow rate $Q$ and the orifice width $w$: $Q \sim (w/σ_{\rm avg}-k)^β$, where $σ_{\rm avg}$ is the average particle diameter, $kσ_{\rm avg}$ is an offset where $Q\sim 0$, the power-law scaling exponent $β=d-1/2$, and $d$ is the spatial dimension. Recent studies of hopper flows of deformable particles in different background fluids suggest that the particle stiffness and dissipation mechanism can also strongly affect the power-law scaling expo…
