We numerically study the dynamic behavior under a symmetric shear flow of selected examples of concentrated phase emulsions with multi-core morphology confined within a microfluidic channel. A variety of new nonequilibrium steady states is reported. Under low shear rates, the emulsion is found to exhibit a solid-like behavior, in which cores display a periodic planetary-like motion with approximately equal angular velocity. At higher shear rates two steady states emerge, one in which all inner cores align along the flow and become essentially motionless and a further one in which some cores accumulate near the outer interface and produce a dynamical elliptical-shaped ring chain, reminiscent of a treadmilling-like structure, while others occupy the center of the emulsion. A quantitative description in terms of i) motion of the cores, ii) rate of deformation of the emulsion and iii) structure of the fluid flow within the channel is also provided.
We present mesoscale numerical simulations of Rayleigh-Bénard convection in a two-dimensional concentrated emulsion, confined between two parallel walls, heated from below and cooled from above, under the effect of buoyancy forces. The systems under study comprise finite-size droplets, whose concentration $Φ_0$ is varied, ranging from the dilute limit up to the point where the emulsion starts to be packed and exhibits non-Newtonian rheology. We focus on the characterisation of the convective heat transfer properties close to the transition from conductive to convective states. The convective f…
The nonlinear rheological response of soft glassy materials is addressed experimentally by focusing on concentrated emulsions where interdroplet attraction is tuned through varying the surfactant content. Velocity profiles are recorded using ultrasonic velocimetry simultaneously to global rheological data in the Couette geometry. Our data show that non-adhesive and adhesive emulsions have radically different flow behaviors in the vicinity of yielding: while the flow remains homogeneous in the non-adhesive emulsion and the Herschel-Bulkley model for a yield stress fluid describes the data very …
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…
Droplet microfluidics, in which micro-droplets serve as individual reactors, has enabled a wide range of high-throughput biochemical processes. Unlike solid wells typically used in current biochemical assays, droplets are subject to instability and can undergo breakup, especially under fast flow conditions. Although the physics of single drops has been studied extensively, the flow of crowded drops or concentrated emulsions, where droplet volume fraction exceeds 80 percent, is relatively unexplored in microfluidics. In this article and the related invited lecture from the 74th Annual Meeting o…
In the absence of coalescence, coarsening of emulsions (and foams) is controlled by molecular diffusion of dispersed phase between droplets/bubbles. Studies of dilute emulsions have shown how the osmotic pressure of a trapped species within droplets can ``osmotically stabilise'' the emulsion. Webster and Cates (Langmuir, 1998, 14, 2068-2079) gave rigorous criteria for osmotic stabilisation of mono- and polydisperse emulsions, in the dilute regime. We consider here whether analogous criteria exist for the osmotic stabilisation of mono- and polydisperse concentrated emulsions and foams, and sugg…
We use a custom shear cell coupled to an optical microscope to investigate at the particle level the yielding transition in concentrated emulsions subjected to an oscillatory shear deformation. By performing experiments lasting thousands of cycles on samples at several volume fractions and for a variety of applied strain amplitudes, we obtain a comprehensive, microscopic picture of the yielding transition. We find that irreversible particle motion sharply increases beyond a volume-fraction dependent critical strain, which is found to be in close agreement with the strain beyond which the stres…
The study of the formation of bands of drops along the direction of the vorticity in a concentrated emulsion is presented. That is, the observed anisotropic structures are characterized by regions of high concentration of drops interspaced with regions of about equal width where hardly any particles are present. These particle distributions are a clear departure to what has previously reported for this emulsion. These patterns are induced by the effect of a simple flow in circular parallel plate geometry (CSS450-Linkam), but only after a prolonged time after the inception of the flow. That is,…
We investigate numerically, by a hybrid lattice Boltzmann method, the morphology and the dynamics of an emulsion made of a polar active gel, contractile or extensile, and an isotropic passive fluid. We focus on the case of a highly off-symmetric ratio between the active and passive components. In absence of any activity we observe an hexatic-ordered droplets phase, with some defects in the layout. We study how the morphology of the system is affected by activity both in the contractile and extensile case. In the extensile case a small amount of activity favors the elimination of defects in the…
In a recent letter (Denkov et al., Phys. Rev. Lett., vol. 100 (2008) p. 138301) we calculated theoretically the macroscopic viscous stress of steadily sheared foam/emulsion from the energy dissipated inside the transient planar films, formed between neighboring bubbles/drops in the shear flow. The model predicts that the viscous stress in these systems should be a proportional to Ca^1/2, where Ca is the capillary number and n = 1/2 is the power-law index. In the current paper we explain in detail our model and develop it further in several aspects: First, we extend the model to account for the…
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…
Yield stress fluids are widely used in industrial application to arrest dense solid particles, which can be studied by using a concentrated emulsion as a model fluid. We show in experiments that particle sedimentation in emulsions cannot be predicted by the classical criterion for spheres embedded in a yield stress fluid. Phase separation processes take place, where a liquid layer forms and particle sedimentation is enhanced by the emulsion drainage. In addition, emulsion drainage can be arrested or enhanced by the amount of particles embedded in the emulsion. A minimal mathematical model is d…
The mechanisms for phase separation in highly concentrated emulsions when subjected to a thermal phase transition remain to be elucidated. Here, we create a hexagonally close-packed monodisperse emulsion in 2D and show that during a cool-heat cycle, the emulsion fully destabilizes akin to phase separation. The mechanism for this catastrophic destabilization is found to be spontaneous coalescence initiation that synchronously occurs between every solidified droplet and its neighbors. This synchronous coalescence initiation establishes system-wide network connectivity in the emulsion causing lar…
We study the rheology of a two-fluid emulsion in semi-concentrated conditions; the solute is Newtonian while the solvent an inelastic power law fluid. The problem at hand is tackled by means of direct numerical simulations using the volume of fluid method. The analysis is performed for different volume fractions and viscosity ratios under the assumption of negligible inertia and zero buoyancy force. Several carrier fluids are considered encompassing both the shear-thinning and thickening behaviors. We show that the effective viscosity of the system increases for shear-thickening fluids and dec…
The morphology of a mixture made of a polar active gel immersed in an isotropic passive fluid is studied numerically. Lattice Boltzmann method is adopted to solve the Navier-Stokes equation and coupled to a finite-difference scheme used to integrate the dynamic equations of the concentration and of the polarization of the active component. By varying the relative amounts of the mixture phases, different structures can be observed. In the contractile case, at moderate values of activity, elongated structures are formed when the active component is less abundant, while a dynamic emulsion of pass…
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…
We investigate numerically the behaviour of a phase-separating mixture of a blue phase I liquid crystal with an isotropic fluid. The resulting morphology is primarily controlled by an inverse capillary number, $χ$, setting the balance between interfacial and elastic forces. When $χ$ and the concentration of the isotropic component are both low, the blue phase disclination lattice templates a cubic array of fluid cylinders. For larger $χ$, the isotropic phase arranges primarily into liquid emulsion droplets which coarsen very slowly, rewiring the blue phase disclination lines into an amorphous …
We use computer simulations to study the morphology and rheological properties of a bidimensional emulsion resulting from a mixture of a passive isotropic fluid and an active contractile polar gel, in the presence of a surfactant that favours the emulsification of the two phases. By varying the intensity of the contractile activity and of an externally imposed shear flow, we find three possible morphologies. For low shear rates, a simple lamellar state is obtained. For intermediate activity and shear rate, an asymmetric state emerges, which is characterized by shear and concentration banding a…
The yielding of foams, concentrated emulsions, pastes and other soft materials under applied strain is often characterized by measuring the complex shear modulus as a function of strain amplitude at low frequency. Results obtained for materials of different physico-chemical constitution are strikingly similar, suggesting the presence of a generic mechanism as pointed out in several previous theoretical studies. We show that the observed strain dependence of the complex shear modulus can be interpreted as the consequence of elasto-plastic response.
Shear thickening is a type of non-Newtonian behavior in which the stress required to shear a fluid increases faster than linearly with shear rate. Many concentrated suspensions of particles exhibit an especially dramatic version, known as Discontinuous Shear Thickening (DST), in which the stress suddenly jumps with increasing shear rate and produces solid-like behavior. The best known example of such counter-intuitive response to applied stresses occurs in mixtures of cornstarch in water. Over the last several years, this shear-induced solid-like behavior together with a variety of other unusu…
Amorphous glassy materials of diverse nature -- concentrated emulsions, granular materials, pastes, molecular glasses -- display complex flow properties, intermediate between solid and liquid, which are at the root of their use in many applications. A classical feature, well documented yet not really understood, is the very non-linear nature of the flow rule relating stresses and strain rates. Using a microfluidic velocimetry technique, we characterize the flow of thin layers of concentrated emulsions, confined in gaps of different thicknesses by surfaces of different roughness. Beyond the cla…
Dispersions of immiscible liquids, such as emulsions and polymer blends, are at the core of many industrial applications which makes the understanding of their properties (morphology, stability, etc.) of great interest. A wide range of these properties depend on interfacial phenomena, whose understanding is therefore of particular importance. The behaviour of interfacial tension in emulsions and polymer blends is well-understood -both theoretically and experimentally -in the case of non-reactive stabilization processes using pre-made surfactants. However, this description of the interfacial te…
Nanocarriers are nanosized materials commonly used for targeted-oriented delivery of active compounds, including antimicrobials and small-molecular drugs. They equally represent fundamental and engineering challenges since sophisticated nanocarriers must show adequate structure, stability, and function in complex ambients. Here, we report on the computational design of a distinctive class of nanocarriers, built from buckled armored nanodroplets, able to selectively encapsulate or release a probe load under specific flow conditions. Mesoscopic simulations offer detailed insight into the interpl…
The behaviour in simple shear of two concentrated and strongly cohesive mineral suspensions showing highly non-monotonic flow curves is described. Two rheometric test modes were employed, controlled stress and controlled shear-rate. In controlled stress mode the materials showed runaway flow above a yield stress, which, for one of the suspensions, varied substantially in value and seemingly at random from one run to the next, such that the up flow-curve appeared to be quite irreproducible. The down-curve was not though, as neither was the curve obtained in controlled rate mode, which turned ou…
Materials such as foams, concentrated emulsions, dense suspensions or colloidal gels, are yield stress fluids. Their steady flow behavior, characterized by standard rheometric techniques, is usually modeled by a Herschel-Bulkley law. The emergence of techniques that allow the measurement of their local flow properties (velocity and volume fraction fields) has led to observe new complex behaviors. It was shown that many of these materials exhibit shear banding in a homogeneous shear stress field, which cannot be accounted for by the standard steady-state constitutive laws of simple yield stress…
Microscopic dynamics reveal the origin of the bulk rheological response in complex fluids. In model systems particle motion can be tracked, but for industrially relevant samples this is often impossible. Here we adapt differential dynamic microscopy (DDM) to study flowing highly-concentrated samples without particle resolution. By combining an investigation of oscillatory flow, using a novel "echo-DDM" analysis, and steady shear, through flow-DDM, we characterise the yielding of a silicone oil emulsion on both the microscopic and bulk level. Through measuring the rate of shear-induced droplet …
Gas-generating reactive flows in bicontinuous catalyst support structures
Helmholtz Institute Erlangen-Nürnberg für Erneuerbare Energien（埃尔朗根-纽伦堡亥姆霍兹可再生能源研究所）；Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡弗里德里希·亚历山大大学）
The volume phase transition of microgels is one of the most paradigmatic examples of stimuli-responsiveness, enabling a collapse from a highly swollen microgel state into a densely coiled state by an external stimulus. Although well characterized in bulk, it remains unclear how the phase transition is affected by the presence of a confining interface. Here, we demonstrate that the temperature-induced volume phase transition of poly(N-isopropylacrylamide) microgels, conventionally considered an intrinsic molecular property of the polymer, is in fact largely suppressed when the microgel is adsor…
The occurence of shear bands in a complex fluid is generally understood as resulting from a structural evolution of the material under shear, which leads (from a theoretical perspective) to a non-monotonic stationnary flow curve related to the coexistence of different states of the material under shear. In this paper we present a scenario for shear-banding in a particular class of complex fluids, namely foams and concentrated emulsions, which differs from other scenarii in two important ways. First, the appearance of shear bands is shown to be possible both without any intrinsic physical evolu…
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…
