The coalescence of droplets plays a crucial role in nature and modern technology. Various experimental and theoretical studies explored droplet dynamics in 3D and on 2D solid or liquid substrates. In this paper, we demonstrate the coalescence of isotropic droplets confined in thin quasi-2D liquids -- overheated smectic films. We observe the merging of micrometer-sized flat droplets using high-speed-imaging and analyse the shape transformations of the droplets on the timescale of milliseconds. Our studies reveal the scaling laws of the coalescence time, which exhibits a different dependence on the droplet geometry than in case of droplets on a solid substrate. A theoretical model is proposed to explain the difference in behaviour.
This fluid dynamics video shows the different interaction mechanisms of coalescence-induced droplet jumping during condensation on a nanostructured superhydrophobic surface. High speed imaging was used to show jumping behavior on superhydrophobic copper oxide and carbon nanotube surfaces. Videos demonstrating multi-jumping droplets, jumping droplet return to the surface, and droplet-droplet electrostatic repulsions were analyzed. Experiments using external electric fields in conjunction with high speed imaging in a custom built experimental chamber were used to show that all coalescence-induce…
Coalescence of micrometer-scale droplets is impacted by several parameters, including droplet size, viscosities of the two phases, droplet velocity and angle of approach, as well as interfacial tension and surfactant coverage. The dynamics and thinning of films between coalescing droplets can be particularly complex in the presence of surfactants, due to the generation of Marangoni stresses and reduced film mobility. In this work, a microfluidic hydrodynamic Stokes trap is used to gently steer and trap surfactant-laden micrometer-sized droplets at the center of a cross-slot. Incoming droplets …
Recent investigations on the coalescence of polymeric droplets on a solid substrate have reported strong disagreements; the heart of the issue is whether coalescence of polymeric drops is similar to that of Newtonian fluid and is independent of molecular relaxation, or whether the role of entanglement of polymeric chains leads to a transition kinetics different from that of Newtonian fluid. Via this report, we resolve the disagreements through a discussion on the effects of merging method on the dominant forces governing the coalescence process, i.e., inertia, dissipation, and relaxation. Our …
Coalescence-induced alignment of anisotropic particles in drying sessile droplets
Forschungszentrum Jülich（于利希研究中心）；Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IET-2)（亥姆霍兹埃尔朗根-纽伦堡可再生能源研究所（IET-2））；Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡弗里德里希·亚历山大大学）
This paper considers the interaction between two droplets placed on a substrate in immediate vicinity. We show here that when the two droplets are of different fluids and especially when one of the droplet is highly volatile, a wealth of fascinating phenomena can be observed. In particular, the interaction may result in the actuation of the droplet system, i.e. its displacement over a finite length. In order to control this displacement, we consider droplets confined on a hydrophilic stripe created by plasma-treating a PDMS substrate. This controlled actuation opens up unexplored opportunities…
For the first time we observed formation of small satellite droplets from the bridge at droplet coalescence. Investigations were made using a Hele-Shaw cell in the two-phase region at nematic-isotropic phase transition. In previous works on coalescence it was considered that before start of coalescence there exists a bridge between the outer fluid connecting regions on the two sides of the droplets (outer bridge). After start of coalescence a bridge connecting the two droplets appears (droplet bridge) and the outer bridge is broken. For the first time we have shown that there are coalescence p…
The dynamics of droplets on substrates has a strong impact on microfluidic systems ranging from commercially available lab-on-chip systems to state of the art developments in open microfluidics. Coalescence of micro and nano droplets on a substrate has been studied extensively, but in previous studies the focus has been on the interface movement. Here, we use computer simulations to investigate coalescence of droplets immersed in another liquid, in an inertia-dominated regime and also investigate the droplet's internal flow field. It is found that qualitatively the dynamics is similar to coale…
The coalescence between growing droplets is important for the surface coverage and spatial arrangements of droplets on surfaces. In this work, total internal reflection fluorescence (TIRF) microscopy is utilized to in-situ investigate the formation of nanodroplets around the rim of a polymer microcap, with sub-micron spatial and millisecond temporal resolution. We observe that the coalescence among droplets occurs frequently during their growth by solvent exchange. Our experimental results show that the position of the droplet from two merged droplets is related to the size of the parent dropl…
Coalescence of droplets is an ubiquitous phenomenon in chemical, physical and biolog-ical systems. The process of merging of liquid objects has been studied during the pastyears experimentally and theoretically in different geometries. We introduce a uniquesystem that allows a quasi two-dimensional description of the coalescence process,micrometer-sized flat droplets in freely suspended smectic liquid-crystal films. We findthat the bridge connecting the droplets grows linearly in time during the initial stage ofcoalescence, both with respect to its height and lateral width. We also verify self…
The coalescence of two resting liquid droplets in a saturated vapor phase is investigated by Lattice Boltzmann simulations in two and three dimensions. We find that, in the viscous regime, the bridge radius obeys a t^{1/2}-scaling law in time with the characteristic time scale given by the viscous time. Our results differ significantly from the predictions of existing analytical theories of viscous coalescence as well as from experimental observations. While the underlying reason for these deviations is presently unknown, a simple scaling argument is given that describes our results well.
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…
Moving contact lines of more than two phases dictate a large number of interfacial phenomena. Despite its significance to fundamental and applied processes, the contact lines at a junction of four-phases (two immiscible liquids, solid and gas) have been addressed only in a few investigations. Here, we report an intriguing phenomenon that follows after the four phases of oil, water, solid and gas make contact through the coalescence of two different three-phase contact lines. We combine experimental study and theoretical analysis to reveal and rationalize the dynamics exhibited upon the coalesc…
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…
Dynamics of the pendant drop coalescing with a sessile drop to form a single daughter droplet is known to form a bridge. The bridge evolution begins with a point contact between the two drops leading to a liquid neck of size comparable to the diameter of the drops. To probe this phenomenon in polymeric fluids, we quantify the neck radius growth during coalescence using high speed imaging. In the current study, we unveil the existence of three regimes on basis of concentration ratio $c/c^*$ namely, inertio-elastic $c/c^*<c_e/c^*$, viscoelastic $c_e/c^*<c/c^*<20$ and elasticity dominated regimes…
The stability of shapes formed by three viscoelastic droplets during their arrested coalescence has been investigated using micromanipulation experiments. Addition of a third droplet to arrested droplet doublets is shown to be controlled by the balance between interfacial pressures driving coalescence and internal elasticity that resists total consolidation. The free fluid available within the droplets controls the transmission of stress during droplet combination and allows connections to occur via formation of a neck between the droplets. The anisotropy of three-droplet systems adds complexi…
Using molecular dynamics simulations and scaling arguments, we investigate the coalescence preference dynamics of liquid droplets in a phase-segregating off-critical, single-component fluid. It is observed that the preferential distance of the product drop from its larger parent, during a coalescence event, gets smaller for large parent size inequality. The relative coalescence position exhibits a power-law dependence on the parent size ratio with an exponent $q \simeq 3.1$. This value of $q$ is in strong contrast with earlier reports $2.02$ and $5.01$ in the literature. The dissimilarity is e…
Droplets coalescing on flat surfaces tend to end up with the smaller droplet migrating into the larger one. We report a counter-intuitive droplet coalescence pattern on a superhydrophilic cylindrical wire, where the larger droplet is pulled toward the smaller one. Consequently, the center of the combined mass significantly moves toward, often beyond, the original location of the smaller droplet. This phenomenon occurs primarily because the viscous friction that a droplet experiences on a cylindrical wire is not positively correlated with the size of the droplet, unlike the droplets coalescing …
The analysis of the size distribution of droplets condensing on a substrate (breath figures) is a test ground for scaling theories. Here, we show that a faithful description of these distributions must explicitly deal with the growth mechanisms of the droplets. This finding establishes a gateway connecting nucleation and growth of the smallest droplets on surfaces to gross features of the evolution of the droplet size distribution.
The stable configurations formed by two viscoelastic, ellipsoid-shaped droplets during their arrested coalescence has been investigated using micromanipulation experiments. Ellipsoidal droplets are produced by millifluidic emulsification of petrolatum into a yield stress fluid that preserves their elongated shape. The liquid meniscus between droplets can transmit stress and instigate movement of the droplets, from their initial relative position, in order to minimize doublet surface energy. The action of the liquid meniscus causes the ellipsoidal droplets to undergo rolling and restructuring e…
The expected universal dynamics associated with the initial stage of droplet coalescence are difficult to study visually due to the rapid motion of the liquid and the awkward viewing geometry. Here we employ an electrical method to study the coalescence of two inviscid droplets at early times. We measure the growth dynamics of the bridge connecting the two droplets and observe a new asymptotic regime inconsistent with previous theoretical predictions. The measurements are consistent with a model in which the two liquids coalesce with a slightly deformed interface.
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 numerically study the coalescence dynamics of two sessile droplets with radii $R_0$. The droplets are placed on top of a rigid substrate with a contact angle of $θ_{eq.} = π/9$. Having a highly wettable substrate ($θ_{eq} \ll π/2$) theory predicts that the bridge height ($h_0$) scales according to $h_0(t) \sim t^{2/3}.$ This behavior can be altered with e.g. surface tension gradients ($\partial_xγ\neq 0$). These gradients appear for example with heat transfer, surfactants or having different but miscible liquids. Instead of coalescence, these gradients can lead to a stable two droplet state…
Coalescence of sessile polymeric fluid drops on a partially wettable substrate exhibits a transition from inertial to viscoelastic regime at concentration ratio $c/c^* \sim 1$. Our findings unveil that the temporal evolution of the growing bridge height follows a power-law behaviour $t^b$, such that the coefficient $b$ continuously decreases from 2/3 in the inertial regime ($c/c^*<1$) to an asymptotic value of 1/2 in the visco-elastic regime ($c/c^*>1$). To account for fluid elasticity and characteristic time-scale in the viscoelastic regime, a modified thin film equation under lubrication app…
When two liquid drops touch, a microscopic connecting liquid bridge forms and rapidly grows as the two drops merge into one. Whereas coalescence has been thoroughly studied when drops coalesce in vacuum or air, many important situations involve coalescence in a dense surrounding fluid, such as oil coalescence in brine. Here we study the merging of gas bubbles and liquid drops in an external fluid. Our data indicate that the flows occur over much larger length scales in the outer fluid than inside the drops themselves. Thus we find that the asymptotic early regime is always dominated by the vis…
Solvent exchange is a simple method to produce surface nanodroplets on a substrate for a wide range of applications by displacing a solution of good solvent, poor solvent and oil (Solution A) by a poor solvent (Solution B). In this work, we show that the growth and coalescence of nanodroplets on a homogeneous surface is mediated by the viscosity of the solvent. We show that at high flow rates of viscous Solution B, the final droplet volume deviates from the scaling law that correlates final droplet volume to the flow rate of non-viscous Solution B, reported in previous work. We attribute this …
The behavior of a microdrop of dielectric liquid suspended in a magnetic fluid and exposed to the action of electric and magnetic fields is studied experimentally. With increasing electric field, the deformation of droplets into oblate ellipsoid, toroid and curved toroid was observed. At the further increase in the electric field, the bursting of droplets was also revealed. The electrorotation of deformed droplets was observed and investigated. The influence of an additional magnetic field on the droplet dynamics was studied. The main features of the droplet dynamics were interpreted and theor…
We present a theoretical framework for capturing the coalescence of a pendant drop with a sessile drop in polymeric fluids. The framework is based on the unification of various constitutive laws under high Weissenberg creeping flow limit. Our results suggests that the phenomenon comes under a new regime namely, the sub-Newtonian regime followed by the limiting case of arrested coalescence with the arrest angle $θ_{arrest}\propto Ec^{-1/2}$, where $Ec$ is the Elasto-capillary number. Further, we propose a new time scale $T^*$ integrating the continuum variable $Ec$ and the macromolecular parame…
We explore the interfacial instability that results when a Newtonian fluid (a glycerol-water mixture, inner fluid) displaces a viscoelastic fluid (a dense cornstarch suspension, outer fluid) in a radial Hele-Shaw cell. As the ratio of viscosities of the inner and outer fluids is increased, side branched interfacial patterns are replaced by more stable interfaces that display proportionate growth and finger coalescence. We correlate the average finger spacing with the most dominant wavelength of interfacial instability, computed using a mathematical model that accounts for viscous fingering in …
Coalescence of liquid droplets involves an interplay between capillary forces, viscous forces and inertial forces. Here, we unveil a universal temporal evolution of the neck radius during the coalescence of two polymeric drops. Through high speed imaging we demonstrate that drops of polyacrylamide (PAM), poly-vinyl alcohol (PVA), polyethylene oxide (PEO), polyethylene glycol (PEG) and xanthan gum (XG) depict a universal behavior $R/\sqrt(ν_0λ) \sim (t/λ)^{0.36}(C/C^{*})^{-0.83}$ over a dilute, semi-dilute and non-dilute range of concentrations. A linear Phan-Thein-Tanner viscoelastic model cap…
The late-stage phase ordering, in $d=2$ dimensions, of symmetric fluid mixtures violates dynamical scaling. We show however that, even at 50/50 volume fractions, if an asymmetric droplet morphology is initially present then this sustains itself, throughout the viscous hydrodynamic regime, by a `coalescence-induced coalescence' mechanism. Scaling is recovered (with length scale $l \sim t$, as in $d=3$). The crossover to the inertial hydrodynamic regime is delayed even longer than in $d=3$; on entering it, full symmetry is finally restored and we find $l\sim t^{2/3}$, regardless of the initial s…
We present an extensive direct numerical simulation of statistically steady, homogeneous, isotropic turbulence in two-dimensional, binary-fluid mixtures with air-drag-induced friction by using the Cahn-Hilliard-Navier-Stokes equations. We choose parameters, e.g., the surface tension, such that we have a droplet of the minority phase moving inside a turbulent background of the majority phase. We characterize the deformation of the droplet and show that it displays multifractal dynamics. The probability distribution functions of the components of the acceleration of the center of mass of the dro…
When a droplet impacts a fabric mesh at a sufficiently high impact velocity, it not only spreads over the fabric but also penetrate its pores. To determine the influence of this liquid penetration of the fabric on droplet spreading on thin fabric meshes, we measured the droplet spreading ratio on fabric with and without an underlying substrate using a high-speed camera. For fabrics without a substrate, the droplet spreading ratio is reduced as the fabric penetration by the liquid reduces the droplet volume spreading on top of the fabric. Using entropic lattice Boltzmann simulations, we find th…
A finite element model was developed to compute the fluid flow inside a sessile evaporating droplet on hydrophilic substrate in ambient conditions. The evaporation is assumed as quasi-steady and the flow is considered as axisymmetric with a pinned contact line. The Navier-Stokes equations in cylindrical coordinates were solved inside the droplet. Galerkin weight residual approach and velocity pressure formulation was used to discretise the governing equations. Six node triangular mesh and quadratic shape functions were used to obtain higher accuracy solutions. Radial velocity profiles in axial…
Tip-streaming generates micron- and submicron- sized droplets when a thin thread pulled from the pointy end of a drop disintegrates. Here, we report streaming from the equator of a drop placed in a uniform electric field. The instability generates concentric fluid rings encircling the drop, which break up to form an array of microdroplets in the equatorial plane. We show that the streaming results from an interfacial instability at the stagnation line of the electrohydrodynamic flow, which creates a sharp rim. The flow draws from the rim a thin sheet which destabilizes and sheds fluid cylinder…
Coalescence event in pendant and sessile drop is distinguished by the formation and evolution of the liquid bridge created upon singular contact. The bridge radius, $R$, is known to evolve as $R\sim t^b$, with power-law exponent, $b$, signifying the dominant governing forces. In this work, we experimentally explore the phenomenon in sub-classes of complex fluids namely, colloidal and non-colloidal suspensions that have particle hydrodynamic interactions as origin of viscoelasticity. Our observations suggest that such fluids have flow dependent thinning response with finite elasticity in shear …
In our daily lives, after shaking a salad dressing, we see the coarsening of oil droplets suspended in vinegar. Such a demixing process is observed everywhere in nature and also of technological importance. For a case of high droplet density, domain coarsening proceeds with interdroplet collisions and the resulting coalescence. This phenomenon has been explained primarily by the so-called Brownian coagulation mechanism: stochastic thermal forces exerted by molecules induce random motion of individual droplets, causing accidental collisions and subsequent interface-tension driven coalescence. C…
This paper outlines a numerical algorithm that could be used for simulating full 3D dynamics of magnetic fluid droplet shapes in external magnetic fields, by solving boundary integral equations. The algorithm works with arbitrary droplet and carrier fluid viscosity ratios. It is validated with known theoretical relationships. Thus it may be used to evaluate various approximations often used in description of ellipsoidal droplets by comparing droplet dynamics calculated from them to the results obtained numerically from first principles here. The algorithm may be used for investigations of drop…
The Marangoni effect refers to fluid flow induced by a gradient in surface tension at a fluid-fluid interface. We determine the full three-dimensional Marangoni flow generated by a non-uniform surface tension profile at the interface of a self-propelled spherical emulsion droplet. For all flow fields inside, outside, and at the interface of the droplet, we give analytical formulas. We also calculate the droplet velocity vector $\mathbf{v}^D$, which describes the swimming kinematics of the droplet, and generalize the squirmer parameter $β$, which distinguishes between different swimmer types ca…
We study self-propelled dynamics of a droplet due to a Marangoni effect and chemical reactions in a binary fluid with a dilute third component of chemical product which affects the interfacial energy of a droplet. The equation for the migration velocity of the center of mass of a droplet is derived in the limit of an infinitesimally thin inter- face. We found that there is a bifurcation from a motionless state to a propagating state of droplet by changing the strength of the Marangoni effect.
Active fluid droplets surrounded by oil can spontaneously develop circulatory flows. However, the dynamics of the surrounding oil and their influence on the active fluid remain poorly understood. To investigate interactions between the active fluid and the passive oil across their interface, kinesin-driven microtubule-based active fluid droplets were immersed in oil and compressed into a cylinder-like shape. The droplet geometry supported intradroplet circulatory flows, but the circulation was suppressed when the thickness of the oil layer surrounding the droplet decreased. Experiments with tr…
We consider two minimal models of active fluid droplets that exhibit complex dynamics including steady motion, deformation, rotation and oscillating motion. First we consider a droplet with a concentration of active contractile matter adsorbed to its boundary. We analytically predict activity driven instabilities in the concentration profile, and compare them to the dynamics we find from simulations. Secondly, we consider a droplet of active polar fluid of constant concentration. In this system we predict, motion and deformation of the droplets in certain activity ranges due to instabilities i…
