Multiple emulsions are a class of soft fluid in which small drops are immersed within a larger one and stabilized over long periods of time by a surfactant. We recently showed that, if a monodisperse multiple emulsion is subject to a pressure-driven flow, a wide variety of nonequilibrium steady states emerges at late times, whose dynamics relies on a complex interplay between hydrodynamic interactions and multibody collisions among internal drops. In this work, we use lattice Boltzmann simulations to study the dynamics of polydisperse double emulsions driven by a Poiseuille flow within a microfluidic channel. Our results show that their behavior is critically affected by multiple factors, such as initial position, polydispersity index, and area fraction occupied within the emulsion. While at low area fraction inner drops may exhibit either a periodic rotational motion (at low polydispersity) or arrange into nonmotile configurations (at high polydispersity) located far from each other, at larger values of area fraction they remain in tight contact and move unidirectionally. This decisively conditions their close-range dynamics, quantitatively assessed through a time-efficiency-like factor. Simulations also unveil the key role played by the capsule, whose shape changes can favor the formation of a selected number of nonequilibrium states in which both motile and nonmotile configurations are found.
We numerically study the dynamics of a polydisperse double emulsion under a symmetric shear flow. We show that both dispersity and shear rate crucially affect the behavior of the innermost drops and of the surrounding shell. While at low/moderate values of shear rates the inner drops rotate periodically around a common center of mass triggered by the fluid vortex formed within the emulsion generally regardless of their polydispersity, at higher values such dynamics occurs only at increasing polydispersity, since monodisperse drops are found to align along the shear flow and become approximatel…
We study dense and highly polydisperse emulsions at droplet volume fractions ϕ>= 0.65. We apply oscillatory shear and observe droplet motion using confocal microscopy. The presence of droplets with sizes several times the mean size dramatically changes the motion of smaller droplets. Both affine and nonaffine droplet motions are observed, with the more nonaffine motion exhibited by the smaller droplets which are pushed around by the larger droplets. Droplet motions are correlated over length scales from one to four times the mean droplet diameter, with larger length scales corresponding to hig…
Ultrasound-vaporizable microdroplets can be exploited for targeted drug delivery. However, it requires customized microfluidic techniques able to produce monodisperse, capillary-sized and biocompatible multiple emulsions. Recent development of microfluidic devices led to the optimization of microdroplet production with high yields, low polydispersity and well-defined diameters. So far, only few were shown to be efficient for simple droplets or multiple emulsions production below 5 microns in diameter, which is required to prevent microembolism after intravenous injection. Here, we present a ve…
Emulsions often act as carriers for water-insoluble solutes that are delivered to a specific target. The molecular transport of solutes in emulsions can be facilitated by surfactants and is often limited by diffusion through the continuous phase. We here investigate this transport on a molecular scale by using a lipophilic molecular rotor as a proxy for solutes. Using fluorescence lifetime microscopy we track the transport of these molecules from the continuous phase towards the dispersed phase in polydisperse oil-in-water emulsions. We show that this transport comprises two timescales, which …
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…
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…
We have discovered the existence of polydisperse High Internal-Phase-Ratio Emulsions (HIPE) in which the internal-phase droplets, present at 95% volume fraction, remain spherical and organize themselves in the available space according to Apollonian packing rules. These polydisperse HIPE are formed during emulsification of surfactant-poor compositions of oil-surfactant-water two-phase systems. Their droplet size-distributions evolve spontaneously towards power laws with the Apollonian exponent. Small-Angle X-Ray Scattering performed on aged HIPEs demonstrated that the droplet packing structure…
We present a deep learning-based object detection and object tracking algorithm to study droplet motion in dense microfluidic emulsions. The deep learning procedure is shown to correctly predict the droplets' shape and track their motion at competitive rates as compared to standard clustering algorithms, even in the presence of significant deformations. The deep learning technique and tool developed in this work could be used for the general study of the dynamics of biological agents in fluid systems, such as moving cells and self-propelled micro organisms in complex biological flows.
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 study the stability of a model Pickering emulsion system. A special counter-flow microfluidics set-up was used to prepare monodisperse Pickering emulsions, with oil droplets in water. The wettability of the monodisperse silica nanoparticles (NPs) could be tuned by surface grafting and the surface coverage of the droplets was controlled using the microfluidics setup. A surface coverage as low as 23$\%$ is enough to stabilize the emulsions and we evidence a new regime of Pickering emulsion stability where the surface coverage of emulsion droplets of constant size increases in time, in coexist…
We have developed Norland Optical Adhesive (NOA) flow focusing devices, making use of the excellent solvent compatibility and surface properties of NOA to generate micron scale oil-in-water emulsions with polydispersities as low as 5%. While current work on microfluidic oil-in-water emulsification largely concerns the production of droplets with sizes on the order of 10s of micrometres, large enough that Brownian motion is negligible, our NOA devices can produce droplets with radii ranging from 2 μm to 12 μm. To demonstrate the utility of these emulsions as colloidal model systems we produce f…
We report the emergence of large-scale hyperuniformity in microfluidic emulsions. Upon periodic driving confined emulsions undergo a first-order transition from a reversible to an irreversible dynamics. We evidence that this dynamical transition is accompanied by structural changes at all scales yielding macroscopic yet finite hyperuniform structures. Numerical simulations are performed to single out the very ingredients responsible for the suppression of density fluctuations. We show that as opposed to equilibrium systems the long-range nature of the hydrodynamic interactions are not required…
In this work, we present two types of microfluidic chips involving magnetic nanoparticles dispersed in cyclohexane with oleic acid. In the first case, the hydrophobically coated nanoparticles are self-assembled with an amphiphilic diblock copolymer by a double-emulsion process in order to prepare giant magnetic vesicles (polymersomes) in one step and at a high throughput. It was shown in literature that such diblock copolymer W/O/W emulsion droplets can evolve into polymersomes made of a thin (nanometric) magnetic membrane through a dewetting transition of the oil phase from the aqueous intern…
Polydisperse fibre networks are the basis of many natural and man-made architectures, ranging from high-performance bio-based materials to components of living cells and tissues. The formation and persistence of such networks are given by fibre properties such as length and stiffness as well as the number density and fibre-fibre interactions. Studies of fibre network behavior, such as connectivity or rigidity thresholds, typically assume fixed fibre length and isotropic fibre orientation distributions, specifically for nanoscale fibres where the methods providing time-resolved measurements are…
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…
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 …
In nature, structural colour generation is based on discriminative light propagation associated with physical structures in the range of the wavelengths of light1. These iridescent structural colours are of immense significance2 but not easy to control experimentally and therefore difficult to exploit for applications. In this work, we employ microfluidics to produce polymerizable double emulsions that can not only induce the already known lensing effect3 but also result in the spectral separation of white light. Here, liquids of varying refractive in-dex that constitute the emulsions resulted…
A robust route for the biased production of single-handed chiral structures has been found in generating non-spherical, multi-component double emulsions using microfluidics. The specific type of handedness is determined by the final packing geometry of four different inner drops inside an ultra-thin sheath of oil. Before three-dimensional chiral structures are formed, the quasi-one-dimensional chain re-arranges in two dimensions into either checkerboard or stripe patterns. We derive an analytical model predicting which pattern is more likely and assembles in the least amount of time. Moreover,…
Understanding the fluid-structure interaction is crucial for an optimal design and manufacturing of soft mesoscale materials. Multi-core emulsions are a class of soft fluids assembled from cluster configurations of deformable oil-water double droplets (cores), often employed as building-blocks for the realisation of devices of interest in bio-technology, such as drug-delivery, tissue engineering and regenerative medicine. Here, we study the physics of multi-core emulsions flowing in microfluidic channels and report numerical evidence of a surprisingly rich variety of driven non-equilibrium sta…
