A micron-sized droplet of bromine water immersed in a surfactant-laden oil phase can swim (S. Thutupalli, R. Seemann, S. Herminghaus, New J. Phys. 13 073021 (2011)). The bromine reacts with the surfactant at the droplet interface and generates a surfactant mixture. It can spontaneously phase-separate due to solutocapillary Marangoni flow, which propels the droplet. We model the system by a diffusion-advection-reaction equation for the mixture order parameter at the interface including thermal noise and couple it to fluid flow. Going beyond previous work, we illustrate the coarsening dynamics of the surfactant mixture towards phase separation in the axisymmetric swimming state. Coarsening proceeds in two steps: an initially slow growth of domain size followed by a nearly ballistic regime. On larger time scales thermal fluctuations in the local surfactant composition initiates random changes in the swimming direction and the droplet performs a persistent random walk, as observed in experiments. Numerical solutions show that the rotational correlation time scales with the square of the inverse noise strength. We confirm this scaling by a perturbation theory for the fluctuations in the mixture order parameter and thereby identify the active emulsion droplet as an active Brownian particle.
We consider an emulsion whose droplets contain a trapped species (insoluble in the continuous phase), and study the emulsion's stability against coarsening via Lifshitz-Slyozov dynamics (Ostwald Ripening). Extending an earlier treatment by Kabalnov et al(Colloids and Surfaces, 24,(1987), 19-32), we derive a general condition on the mean initial droplet volume which ensures stability, even when arbitrary polydispersity is present in both size and composition of the initial droplets. We distinguish "nucleated" coarsening, which requires either fluctuations about the mean field equations or a tai…
The field of active matter, and particularly active emulsions, is growing rapidly, with significant progress made recently on both theoretical and experimental fronts. Here, we summarize experimental research progress related to active droplets. The constitution of active droplets, in particular the chemical compositions and structure of interfaces, is critical. We discuss how emulsion properties such as mechanism of motion, speed, trajectory, interaction strength, and lifetime are related to the droplet composition. We consider not only traditional single emulsions but also more complex varia…
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…
The rheological properties of emulsions are of considerable importance in a diverse range of scenarios. Here we describe a superposition of the effects of droplet elasticity and volume fraction on the dynamics of emulsions. The superposition is governed by physical interactions between droplets, and provides a new mechanism for modifying the flow behavior of emulsions, by controlling the elasticity of the dispersed phase. We investigate the properties of suspensions of emulsified wormlike micelles (WLM). Dense suspensions of the emulsified WLM droplets exhibit thermally responsive properties i…
Tissues are subjected to large external forces and undergo global deformations during morphogenesis. We use synthetic analogues of tissues to study the impact of cell-cell adhesion on the response of cohesive cellular assemblies under such stresses. In particular, we use biomimetic emulsions in which the droplets are functionalized in order to exhibit specific droplet-droplet adhesion. We flow these emulsions in microfluidic constrictions and study their response to this forced deformation via confocal microscopy. We find that the distributions of avalanche sizes are conserved between repulsiv…
An important strategy to stabilize emulsions is to arrest coalescence of the constituent droplets with an opposing rheological force. Colloidal particles adsorbed on the surface of emulsion droplets in a Pickering emulsion become increasingly crowded during successive coalescence events because the combined surface area of coalescing droplets is less than that of the constituent droplets. Beyond a critical density, the particles form a rigid shell around the droplet and inhibit both relaxation of the droplet shape and further coalescence. The resulting droplets have a nonuniform distribution o…
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…
We simulate the response of a particle-stabilized emulsion droplet in an external force field, such as gravity, acting equally on all $N$ particles. We show that the field strength required for breakup (at fixed initial area fraction) decreases markedly with droplet size, because the forces act cumulatively, not individually, to detach the interfacial particles. The breakup mode involves the collective destabilization of a solidified particle raft occupying the lower part of the droplet, leading to a critical force per particle that scales approximately as $N^{-1/2}$.
We report a new mechanism for nucleation in a monolayer of hexagonally packed monodisperse droplet arrays. Upon cooling, we observe solidified droplets to nucleate their supercooled neighbors giving rise to an autocatalytic-like mechanism for accelerated crystallization. This collective mode of nucleation depends on the strength and nature of droplet contacts. Intriguingly, the statistical distribution of the solidified droplet clusters is found to be independent of emulsion characteristics except surfactant. In contrast to classical nucleation theory, our work highlights the need to consider …
We demonstrate that emulsion droplets stabilized by interfacial particles become unstable beyond a size threshold set by gravity. This holds not only for colloids but supra-colloidal glass beads, using which we directly observe the ejection of particles near the droplet base. The number of particles acting together in these ejection events decreases with time until a stable acorn-like configuration is reached. Stability occurs when the weight of all remaining particles is less than the interfacial binding force of one particle. We also show the importance of the curvature of the droplet surfac…
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.
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…
When cooled down, emulsion droplets stabilized by a frozen interface of alkane molecules and surfactants have been observed to undergo a spectacular sequence of morphological transformations: from spheres to faceted icosahedra, down to flattened liquid platelets. While generally ascribed to the interplay between the elasticity of the frozen interface and surface tension, the physical mechanisms underpinning these transitions have remained elusive, despite different theoretical pictures having been proposed in recent years. In this article, we introduce a comprehensive mechanical model of morph…
The freeze-thaw cycling of particle-stabilised emulsions can alter the emulsion structure and stability. This could have significant consequences for using particle stabilisation in industrial applications where increased stability is generally desirable. It is therefore important to characterise the behaviour and stability of these composites under the influence of freeze-thaw cycles. Water-in-oil Pickering emulsions stabilised by poly(methyl methacrylate) particles were subjected to freeze-thaw cycles of the continuous phase under two different conditions - uniform and non-uniform freezing. …
We study water-in-oil emulsion droplets, running the Belousov-Zhabotinsky reaction, that form a new type of active matter unit. These droplets, stabilised by surfactants dispersed in the oil medium, are capable of internal chemical oscillations and also self-propulsion due to dynamic interfacial instabilities that result from the chemical reactions. The chemical oscillations can couple via the exchange of activator and inhibitor type of reaction intermediates across the droplets under precise conditions of surfactant bilayer formation between the droplets. Here we present the synchronization b…
Combining high-speed photography with electric current measurement, we investigate the electrocoalescence of Pickering emulsion droplets. Under high enough electric field, the originally-stable droplets coalesce via two distinct approaches: normal coalescence and abnormal coalescence. In the normal coalescence, a liquid bridge grows continuously and merges two droplets together, similar to the classical picture. In the abnormal coalescence, however, the bridge fails to grow indefinitely; instead it breaks up spontaneously due to the geometric constraint from particle shells. Such connecting-th…
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…
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…
To model a nematic emulsion consisting of a surfactant-coated water droplet dispersed in a nematic host, we performed a molecular dynamics simulation of a droplet immersed in a system of 2048 Gay-Berne ellipsoids in a nematic phase. Strong radial anchoring at the surface of the droplet induced a Saturn ring defect configuration, consistent with theoretical predictions for very small droplets. A surface ring configuration was observed for lower radial anchoring strengths, and a pair of point defects was found near the poles of the droplet for tangential anchoring. We also simulated the falling …
Inverse nematic emulsions in which surfactant-coated water droplets are dispersed in a nematic host fluid have distinctive properties that set them apart from dispersions of two isotropic fluids or of nematic droplets in an isotropic fluid. We present a comprehensive theoretical study of the distortions produced in the nematic host by the dispersed droplets and of solvent mediated dipolar interactions between droplets that lead to their experimentally observed chaining. A single droplet in a nematic host acts like a macroscopic hedgehog defect. Global boundary conditions force the nucleation o…
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 …
This work analyzes trajectories obtained by YOLO and DeepSORT algorithms of dense emulsion systems simulated by Lattice Boltzmann methods. The results indicate that the individual droplet's moving direction is influenced more by the droplets immediately behind it than the droplets in front of it. The analysis also provides hints on constraints on writing down a dynamical model of droplets for the dense emulsion in narrow channels.
We study how local rearrangements alter droplet stresses within flowing dense quasi-two-dimensional emulsions at area fractions $ϕ\geq 0.88$. Using microscopy, we measure droplet positions while simultaneously using their deformed shape to measure droplet stresses. We find that rearrangements alter nearby stresses in a quadrupolar pattern: stresses on neighboring droplets tend to either decrease or increase depending on location. The stress redistribution is more anisotropic with increasing $ϕ$. The spatial character of the stress redistribution influences where subsequent rearrangements occur…
In living cells, molecular motors create activity that enhances the diffusion of particles throughout the cytoplasm, and not just ones attached to the motors. We demonstrate initial steps toward creating artificial cells that mimic this phenomenon. Our system consists of active, Pt-coated Janus particles and passive tracers confined to emulsion droplets. We track the motion of both the active particles and passive tracers in a hydrogen peroxide solution, which serves as the fuel to drive the motion. We first show that correcting for bulk translational and rotational motion of the droplets indu…
We have discovered the existence of extremely 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. Such Apollonian emulsions are obtained from dispersing oil dropwise in water in the presence of very little surfactant, and allowing them to evolve at rest for a week. The packing structure of the droplets was confirmed through size distribution measurements that evolved spontaneously towards power laws with the known Apoll…
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…
We study the elasto-plastic behavior of dense attractive emulsions under mechanical perturbation. The attraction is introduced through non-specific depletion interactions between the droplets and is controlled by changing the concentration of surfactant micelles in the continuous phase. We find that such attractive forces are not sufficient to induce any measurable modification on the scalings between the local packing fraction and the deformation of the droplets. However, when the emulsions are flown through 2D microfluidic constrictions, we uncover a measurable effect of attraction on their …
In their Comment [arXiv:2102.03842], Haas et al. advance two hypotheses on the nature of the shape transformations observed in surfactant-stabilized emulsion droplets, as the theoretical models that us [Phys. Rev. Lett. 126, 038001 (2021)] and others [P. A. Haas et al. Phys. Rev. Lett. 118, 088001 (2017), Phys. Rev. Research 1, 023017 (2019)] have introduced to account for these observations. (1) Because of the different surfactants used in experimental studies, the physical mechanisms underpinning the shape transformations may, in fact, differ in spite of the extraordinary resemblance in the …
In this study, we present experimental and theoretical analyses of double emulsion drop evaporation. After the apparent completion of evaporation of the inner phase of a double emulsion drop, surprisingly, a resurfacing of a daughter droplet is observed. We further investigated to hypothesize this phenomenon which allowed us to obtain a prolonged fixed contact line evaporation for a single phase drop along with similar occurrence of resurfacing as of the double emulsion drops.
We propose diagrams representing the equilibrium morphologies of two immiscible liquid droplets brought into contact. We study the dependence of the shape of the droplets on the surface tensions and ratio of volumes. We study theoretically and experimentally the regimes of the parameters corresponding to complete engulfing (one of the droplets completely absorbed by the other one), non-engulfing (in which the droplets remain separated) and partial-engulfing (intermediate configuration in which all three interfaces are present). We specify the values of surface tensions corresponding to a Janus…
The effective capillary interaction potentials for small colloidal particles trapped at the surface of liquid droplets are calculated analytically. Pair potentials between capillary monopoles and dipoles, corresponding to particles floating on a droplet with a fixed center of mass and subjected to external forces and torques, respectively, exhibit a repulsion at large angular separations and an attraction at smaller separations, with the latter resembling the typical behavior for flat interfaces. This change of character is not observed for quadrupoles, corresponding to free particles on a mec…
We experimentally study the shear flow of oil-in-water emulsion droplets in a thin sample chamber with a hopper shape. In this thin chamber, the droplets are quasi-2D in shape. The sample is at an area fraction above jamming and forced to flow with a constant flux rate. Stresses applied to a droplet from its neighbors deform the droplet outline, and this deformation is quantified to provide an ad hoc measure of the stress. As the sample flows through the hopper we see large fluctuations of the stress, similar in character to what has been seen in other flows of complex fluids. Periods of time …
We present a mechanistic model of drug release from a multiple emulsion into an external surrounding fluid. We consider a single multi-layer droplet where the drug kinetics are described by a pure diffusive process through different liquid shells. The multi-layer problem is described by a system of diffusion equations coupled via interlayer conditions imposing continuity of drug concentration and flux. Mass resistance is imposed at the outer boundary through the application of a surfactant at the external surface of the droplet. The two-dimensional problem is solved numerically by finite volum…
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…
Micro- and nanogels are widely used to stabilise emulsions and simultaneously implement their responsiveness to the external stimuli. One of the factors that improves the emulsion stability is the nanogel softness. Here, we study how the softest nanogels that can be synthesised with precipitation polymerisation of N-isopropylacrylamide (NIPAM), the ultra-low crosslinked (ULC) nanogels, stabilise oil-in-water emulsions. We show that ULC nanogels can efficiently stabilise emulsions already at low mass concentrations. These emulsions are resistant to droplet flocculation, stable against coalescen…
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…
Many industrial soft materials often include oil-in-water (O/W) emulsions at the core of their formulations. By using tuneable interface stabilizing agents, such emulsions can self-assemble into complex structures. DNA has been used for decades as a thermoresponsive highly specific binding agent between hard and, recently, soft colloids. Up until now, emulsion droplets functionalized with DNA had relatively low coating densities and were expensive to scale up. Here a general O/W DNA-coating method using functional non-ionic amphiphilic block copolymers, both diblock and triblock, is presented.…
Separating petroleum hydrocarbons from water is an important problem to address in order to mitigate the disastrous effects of hydrocarbons on aquatic ecosystems. A rational approach to address the problem of marine oil water separation is to disperse the oil with the aid of surfactants in order to minimize the formation of large slicks at the water surface and to maximize the oil-water interfacial area. Here we investigate the fundamental wetting and transport behavior of such surfactant-stabilized droplets and the flow conditions necessary to perform sieving and separation of these stabilize…
There is a large debate on the destabilization mechanism of emulsions. We present a simple technique using mechanical compression to destabilize oil-in-water emulsions. Upon compression of the emulsion, the continuous aqueous phase is squeezed out, while the dispersed oil phase progressively deforms from circular to honeycomb-like shapes. The films that separate the oil droplets are observed to thin and break at a critical oil/water ratio, leading to coalescence events. Electrostatic interactions and local droplet rearrangements do not determine film rupture. Instead, the destabilization occur…
We numerically study the Rayleigh-Bénard (RB) convection in two-dimensional model emulsions confined between two parallel walls at fixed temperatures. The systems under study are heterogeneous, with finite-size droplets dispersed in a continuous phase. The droplet concentration is chosen to explore the convective heat transfer of both Newtonian (low droplet concentration) and non-Newtonian (high droplet concentration) emulsions, the latter exhibiting shear-thinning rheology, with a noticeable increase of viscosity at low shear rates. It is well known that the transition to convection of a homo…
Emulsion droplets trapped in an ultrasonic levitator behave in two ways that solid spheres do not: (1) Individual droplets spin rapidly about an axis parallel to the trapping plane, and (2) coaxially spinning droplets form long chains aligned with their common axis of rotation. Acoustically-organized chains interact hydrodynamically, either to merge into longer chains or to form three-dimensional bundles of chains. Solid spheres, by contrast, form close-packed planar crystals drawn together by the sound-mediated secondary Bjerknes interaction. We demonstrate the chain-to-crystal transition wit…
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…
We experimentally and computationally study the flow of a quasi-two-dimensional emulsion through a constricting hopper shape. Our area fractions are above jamming such that the droplets are always in contact with one another and are in many cases highly deformed. At the lowest flow rates, the droplets exit the hopper via intermittent avalanches. At the highest flow rates, the droplets exit continuously. The transition between these two types of behaviors is a fairly smooth function of the mean strain rate. The avalanches are characterized by a power law distribution of the time interval betwee…
Molecular chirality controls droplet division and helical fiber formation in liquid crystal emulsions
Faculty of Mathematics and Physics, University of Ljubljana(卢布尔雅那大学数学与物理学院);Condensed Matter Physics Department, Jožef Stefan Institute(约热·斯蒂芬研究所凝聚态物理系);Dynamics of Complex Fluids, Max Planck Institute for Dynamics and Self-Organization(马克斯·普朗克动力学与自组织研究所复杂流体动力学);Department of Chemistry, Faculty of Science, Tokyo University of Science(东京理科大学理学部化学系)
By varying the oil volume fraction, the microscopic droplet size and the macroscopic rheology of emulsions are investigated in a Taylor-Couette (TC) turbulent shear flow. Although here oil and water in the emulsions have almost the same physical properties (density and viscosity), unexpectedly, we find that oil-in-water (O/W) and water-in-oil (W/O) emulsions have very distinct hydrodynamic behaviors, i.e., the system is clearly asymmetric. By looking at the micro-scales, the average droplet diameter hardly changes with the oil volume fraction neither for O/W nor for W/O. However, for W/O it is…
We study long range density fluctuations (hyperuniformity) in two-dimensional jammed packings of bidisperse droplets. Taking advantage of microfluidics, we systematically span a large range of size and concentration ratios of the two droplet populations. We identify various defects increasing long range density fluctuations mainly due to organization of local particle environment. By choosing an appropriate bidispersity, we fabricate materials with a high level of hyperuniformity. Interesting transparency properties of these optimized materials are established based on numerical simulations.
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…
Here we study theoretically the dynamics of a 2D and a 3D isotropic droplet in a nematic liquid crystal under a shear flow. We find a large repertoire of possible nonequilibrium steady states as a function of the shear rate and of the anchoring of the nematic director field at the droplet surface. We first discuss homeotropic anchoring. For weak anchoring, we recover the typical behaviour of a sheared isotropic droplet in a binary fluid, which rotates, stretches and can be broken by the applied flow. For intermediate anchoring, new possibilities arise due to elastic effects in the nematic flui…
We propose an improved viscosity model accounting for experiments of emulsions of two immiscible liquids at arbitrary volume fractions and low shear rates. The model is based on a recursive-differential method formulated in terms of the appropriate scaling variable which emerges from an analysis of excluded volume effects in the system. This variable, called the effective filling fraction, incorporates the geometrical information of the system which determines the maximum packing and reduces to the bare filling fraction for infinitely diluted emulsions. The agreement of our model for the visco…
Double emulsions, due to their compartmental structures, are essential in food, agricultural, and pharmaceutical applications. Traditionally, double emulsifications rely on the presence of both oil-soluble and water-soluble surfactants or external stimuli responsive materials and require sequential droplet formation settings or unique fluidic designs. We report on unusual phenomenon where double emulsions are spontaneously formed as soon an aqueous nanoparticle dispersion is placed in contact with an oleic micellar solution. Nanoscale water droplets nucleate in oil in the form of swollen micel…
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…
We propose here a new mechanism of droplet coarsening in phase-separating fluid mixtures. In contrast to the conventional understanding that there are no interactions between droplets in the late stage of spinodal decomposition, we demonstrate the existence of interactions between droplets that is caused by the coupling between diffuse concentration change around droplets. We show the possibility that this mechanism plays an important role in droplet phase separation together with Brownian-coagulation mechanism. We also discuss the coupling between hydrodynamic and diffusion modes, namely, "co…