arXiv subjects

Christian Diddens

Publications and source records attributed to Christian Diddens.

At least 37 records · Page 2Linked to original sources

arXiv2022

Interfacial aggregation of self-propelled Janus colloids in sessile droplets

Living microorganisms in confined systems typically experience an affinity to populate boundaries. The reason for such affinity to interfaces can be a combination of their directed motion and hydrodynamic interactions at distances larger than their own size. Here we will show that self-propelled Janus particles (polystyrene particles partially coated with platinum) immersed in droplets of water and hydrogen peroxide tend to accumulate in the vicinity of the liquid/gas interface. Interestingly, the interfacial accumulation occurs despite the presence of an evaporation-driven flow caused by a solutal Marangoni flow, which typically tends to redistribute the particles within the droplet's bulk. By performing additional experiments with passive colloids (flow tracers) and comparing with numerical simulations for both particle active motion and the fluid flow, we disentangle the dominating mechanisms behind the observed interfacial particle accumulation. These results allow us to make an analogy between active Janus particles and some biological microswimmers concerning how they interact with their environment.

physics.flu-dyn↗

arXiv2022

Evaporation-driven liquid flow in sessile droplets

The evaporation of a sessile droplet spontaneously induces an internal capillary liquid flow. The surface-tension driven minimisation of surface area and/or surface-tension differences at the liquid-gas interface caused by evaporation-induced temperature or chemical gradients set the liquid into motion. This flow drags along suspended material and is one of the keys to control the material deposition in the stain that is left behind by a drying droplet. Applications of this principle range from the control of stain formation in the printing and coating industry, to the analysis of DNA, to forensic and medical research on blood stains, and to the use of evaporation-driven self-assembly for nanotechnology. Therefore, the evaporation of sessile droplets attracts an enormous interest from not only the fluid dynamics, but also the soft matter, chemistry, biology, engineering, nanotechnology and mathematics communities. As a consequence of this broad interest, knowledge on evaporation-driven flows in drying droplets has remained scattered among the different fields, leading to various misconceptions and misinterpretations. In this review we aim to unify these views, and reflect on the current understanding of evaporation-driven liquid flows in sessile droplets in the light of the most recent experimental and theoretical advances. In addition, we outline open questions and indicate promising directions for future research.

physics.flu-dyn↗

arXiv2022

Evaporation of a sessile colloidal water-glycerol droplet: Marangoni ring formation

The transport and aggregation of particles in suspensions is an important process in many physicochemical and industrial processes. In this work, we study the transport of particles in an evaporating binary droplet. Surprisingly, the accumulation of particles occurs not only at the contact line (due to the coffee-stain effect) or at the solid substrate (due to sedimentation), but also at a particular radial position near the liquid-air interface, forming a "ring", which we term as the Marangoni ring. The formation of this ring is primarily attributed to the solutal Marangoni flow triggered by the evaporation dynamics of the water-glycerol droplet. Experiments and simulations show fair agreement in the volume evolution and the general structure of the solutal Marangoni flow, that is, the Marangoni vortex. Experiments show that the location of the Marangoni ring is strongly correlated with the Marangoni vortex. However, finite element numerical simulations fail to describe the particle distribution seen in the experiments. Interestingly, the particles not only accumulate to form the Marangoni ring but also assemble as colloidal crystals close to the liquid-air interface, yielding iridescence. The formation of the colloidal crystals in the experiments is strong evidence that non-hydrodynamic interactions, which are not represented in the simulations, also play a significant role in our system.

physics.flu-dyn↗

arXiv2022

Physiochemical hydrodynamics of the phase segregation in an evaporating binary microdroplet

Phase segregation triggered by selective evaporation can emerge in multicomponent systems, leading to complex physiochemical hydrodynamics. Recently, Li et al. (Phys. Rev. Lett., vol. 120, 2018, 224501) and Kim & Stone (J. Fluid Mech., vol. 850, 2018, pp. 769-783) reported a segregative behavior (i.e., demixing) in an evaporating binary droplet. In this work, by means of experiments and theoretical analysis, we investigate the flow dynamics after the occurrence of the phase segregation. As example, we take the 1,2-hexanediol-water binary droplet system. First, we experimentally reveal the overall physiochemical hydrodynamics of the evaporation process, including the segregative behavior and the resulting flow structure close to the substrate. By quantifying the evolution of the radial flow, we identify three successive life stages of the evaporation process. At Stage I, a radially outward flow is observed. It is driven by the Marangoni effect. At the transition to Stage II, the radial flow partially reverses, starting from the contact line. This flow breaks the axial symmetry and remarkably is driven by the segregation itself. Finally at Stage III, the flow decays as the evaporation gradually ceases. At this stage the segregation has grown to the entire droplet, and the flow is again controlled by the Marangoni effect. The resulting Marangoni flow homogenizes the distribution of the entrapped volatile water over the whole droplet.

physics.flu-dyn↗

arXiv2022

Droplet dissolution driven by emerging thermal gradients and Marangoni flow

The lifetime $τ$ of an isothermal and purely diffusively dissolving droplet in a host liquid scales as $τ\sim R_0^2$ with its initial radius $R_0$ [Langmuir, Phys. Rev. 12, 368 (1919)]. For a droplet dissolving due to natural convection driven by density differences, its lifetime scales as $τ\sim R_0^{5/4}$ [Dietrich et al., J. Fluid Mech. 794, 45 (2016)]. In this paper we experimentally find and theoretically derive yet another droplet dissolution behavior, resulting in $τ\sim R_0^4$. It occurs when the dissolution dynamics is controlled by local heating of the liquid, leading to a modified solubility and a thermal Marangoni flow around the droplet. The thermal gradient is achieved by plasmonic heating of a gold nanoparticle decorated sample surface, on which a sessile water droplet immersed in water-saturated 1-butanol solution is sitting. The resulting off-wall thermal Marangoni flow and the temperature dependence of the solubility determine the droplet dissolution rate, resulting in a shrinkage $R(t) \sim (τ-t )^{1/4}$ of the droplet radius and thus in $τ\sim R_0^{4}$.

physics.flu-dyn↗

arXiv2022

Oscillatory droplet dissolution from competing Marangoni and gravitational flows

The dissolution or growth of a droplet in a host liquid is an important part for processes like chemical extraction, chromatography or emulsification. In this work we look at the dissolution of a pair of vertically aligned droplets immersed in water, both experimentally and with numerical simulations. The liquids used for the droplets are long chain alcohols with a low but finite solubility in water and a significantly lower density than that of the host liquid. Therefore, a solutal plume is formed above of the bottom droplet and natural convection dominates the dissolution process. We monitor the volume of the droplets and the velocity field around them over time. When the liquids of the two droplets are the same, our previously found scaling laws for the Sherwood and Reynolds numbers as functions of the Rayleigh number (Dietrich et al., 2016, J. Fluid Mech.) can be applied to the lower droplet. However, remarkably, when the liquid of the top droplet is different than that of the bottom droplet the volume as function of time becomes non-monotonic, and an oscillatory Marangoni flow at the top droplet is observed. We identify the competition between solutal Marangoni flow and density driven convection as the origin of the oscillation, and numerically model the process.

physics.flu-dyn↗

arXiv2022

The asymmetric coalescence of two droplets with different surface tensions is caused by capillary waves

When two droplets with different surface tensions collide, the shape evolution of the merging droplets is asymmetric. Using experimental and numerical techniques, we reveal that this asymmetry is caused by asymmetric capillary waves, which are the result of the different surface tensions of the droplets. We show that the asymmetry is enhanced by increasing the surface tension difference, and suppressed by increasing the inertia of the colliding droplets. Furthermore, we study capillary waves in the limit of no inertia. We reveal that the asymmetry is not directly caused by Marangoni forces. In fact, somehow counterintuitive, asymmetry is strongly reduced by the Marangoni effect. Rather, the different intrinsic capillary wave amplitudes and velocities associated with the different surface tensions of the droplets lie at the origin of the asymmetry during droplet coalescence.

physics.flu-dyn↗

arXiv2021

Time-resolved velocity and pressure field quantification in a flow-focusing device for ultrafast microbubble production

Flow-focusing devices have gained great interest in the past decade, due to their capability to produce monodisperse microbubbles for diagnostic and therapeutic medical ultrasound applications. However, up-scaling production to industrial scale requires a paradigm shift from single chip operation to highly parallelized systems. Parallelization gives rise to fluidic interactions between nozzles that, in turn, may lead to a decreased monodispersity. Here, we study the velocity and pressure field fluctuations in a single flow-focusing nozzle during bubble production. We experimentally quantify the velocity field inside the nozzle at 100 ns time resolution, and a numerical model provides insight into both the oscillatory velocity and pressure fields. Our results demonstrate that, at the length scale of the flow focusing channel, the velocity oscillations propagate at fluid dynamical time scale (order of microseconds) whereas the dominant pressure oscillations are linked to the bubble pinch-off and propagate at a much faster time scale (order of nanoseconds).

physics.flu-dyn↗

arXiv2021

Marangoni instability triggered by selective evaporation of a binary liquid inside a Hele-Shaw cell

Interfacial stability is important for many processes involving heat and mass transfer across two immiscible phases. When this transfer takes place in the form of evaporation of a binary solution with one component being more volatile than the other, gradients in surface tension can arise. These gradients can ultimately destabilise the liquid-gas interface. In the present work, we study the evaporation of an ethanol-water solution, for which ethanol has a larger volatility. The solution is contained in a horizontal Hele-Shaw cell which is open from one end to allow for evaporation into air. A Marangoni instability is then triggered at the liquid-air interface. We study the temporal evolution of this instability by observing the effects that it has on the bulk of the liquid. More specifically, the growth of convective cells is visualized with confocal microscopy and the velocity field close to the interface is measured with micro-particle-image-velocimetry. The results of numerical simulations based on quasi 2D equations satisfactorily compare with the experimental observations, even without consideration of evaporative cooling, although this cooling can play an extra role in experiments. Furthermore, a linear stability analysis applied to a simplified version of the quasi 2D equations showed reasonably good agreement with the results from simulations at early times, when the instability has just been triggered and no coarsening has taken place. In particular, we find a critical Marangoni number below which a regime of stability is predicted.

physics.flu-dyn↗

arXiv2021

Periodic bouncing of a plasmonic bubble in a binary liquid by competing solutal and thermal Marangoni forces

The physicochemical hydrodynamics of bubbles and droplets out of equilibrium, in particular with phase transitions, displays surprisingly rich and often counterintuitive phenomena. Here we experimentally and theoretically study the nucleation and early evolution of plasmonic bubbles in a binary liquid consisting of water and ethanol. Remarkably, the submillimeter plasmonic bubble is found to be periodically attracted to and repelled from the nanoparticle-decorated substrate, with frequencies of around a few kHz. We identify the competition between solutal and thermal Marangoni forces as origin of the periodic bouncing. The former arises due to the selective vaporization of ethanol at the substrate's side of the bubble, leading to a solutal Marangoni flow towards the hot substrate, which pushes the bubble away. The latter arises due to the temperature gradient across the bubble, leading to a thermal Marangoni flow away from the substrate which sucks the bubble towards it. We study the dependence of the frequency of the bouncing phenomenon from the control parameters of the system, namely the ethanol fraction and the laser power for the plasmonic heating. Our findings can be generalized to boiling and electrolytically or catalytically generated bubbles in multicomponent liquids.

physics.flu-dyn↗

arXiv2021

Marangoni instability of a drop in a stably stratified liquid

Marangoni instabilities can emerge when a liquid interface is subjected to a concentration or temperature gradient. It is generally believed that for these instabilities bulk effects like buoyancy are negligible as compared to interfacial forces, especially on small scales. Consequently, the effect of a stable stratification on the Marangoni instability has hitherto been ignored. Here we report, for an immiscible drop immersed in a stably stratified ethanol-water mixture, a new type of oscillatory solutal Marangoni instability which is triggered once the stratification has reached a critical value. We experimentally explore the parameter space spanned by the stratification strength and the drop size and theoretically explain the observed crossover from levitating to bouncing by balancing the advection and diffusion around the drop. Finally, the effect of the stable stratification on the Marangoni instability is surprisingly amplified in confined geometries, leading to an earlier onset.

physics.flu-dyn↗

arXiv2020

Competing Marangoni and Rayleigh convection in evaporating binary droplets

For a small sessile or pendant droplet it is generally assumed that gravity does not play any role once the Bond number is small. This is even assumed for evaporating binary sessile or pendant droplets, in which convective flows can be driven due to selective evaporation of one component and the resulting concentration and thus surface tension differences at the air-liquid interface. However, recent studies have shown that in such droplets gravity indeed can play a role and that natural convection can be the dominant driving mechanism for the flow inside evaporating binary droplets (Edwards et al., Phys. Rev. Lett. 121, 184501 (2018); Li et al., Phys. Rev. Lett. 122, 114501 (2019)). In this study, we derive and validate a quasi-stationary model for the flow inside evaporating binary sessile and pendant droplets, which successfully allows to predict the prevalence and the intriguing interaction of Rayleigh and/or Marangoni convection on the basis of a phase diagram for the flow field expressed in terms of the Rayleigh and Marangoni numbers.

physics.flu-dyn↗

arXiv2020

Rayleigh-Taylor instability by segregation in an evaporating multi-component microdroplet

The evaporation of multi-component droplets is relevant to various applications but challenging to study due to the complex physicochemical dynamics. Recently, Li (2018) reported evaporation-triggered segregation in 1,2-hexanediol-water binary droplets. In this present work, we added 0.5 wt% silicone oil into the 1,2-hexanediol-water binary solution. This minute silicone oil concentration dramatically modifies the evaporation process as it triggers an early extraction of the 1,2-hexanediol from the mixture. Surprisingly, we observe that the segregation of 1,2-hexanediol forms plumes, rising up from the rim of the sessile droplet towards the apex during the droplet evaporation. By orientating the droplet upside down, i.e., by studying a pendant droplet, the absence of the plumes indicates that the flow structure is induced by buoyancy, which drives a Rayleigh-Taylor instability (i.e., driven by density differences & gravitational acceleration). From micro-PIV measurement, we further prove that the segregation of the non-volatile component (1,2-hexanediol) hinders the evaporation near the contact line, which leads to a suppression of the Marangoni flow in this region. Hence, on long time scales, gravitational effects play the dominant role in the flow structure, rather than Marangoni flows. We compare the measurement of the evaporation rate with the diffusion model of Popov (2005), coupled with Raoult's law and the activity coefficient. This comparison indeed confirms that the silicone-oil-triggered segregation of the non-volatile 1,2-hexanediol significantly delays the evaporation. With an extended diffusion model, in which the influence of the segregation has been implemented, the evaporation can be well described.

physics.flu-dyn↗

arXiv2019

Gravitational effect in evaporating binary microdroplets

The flow in an evaporating glycerol-water binary sub-millimeter droplet with Bond number Bo $\ll$ 1 is studied both experimentally and numerically. First, we measure the flow fields near the substrate by micro-PIV for both sessile and pendant droplets during the evaporation process, which surprisingly show opposite radial flow directions -- inward and outward, respectively. This observation clearly reveals that in spite of the small droplet size, gravitational effects play a crucial role in controlling the flow fields in the evaporating droplets. We theoretically analyze that this gravity-driven effect is triggered by the lower volatility of glycerol which leads to a preferential evaporation of water then the local concentration difference of the two components leads to a density gradient that drives the convective flow. We show that the Archimedes number Ar is the nondimensional control parameter for the occurrence of the gravitational effects. We confirm our hypothesis by experimentally comparing two evaporating microdroplet systems, namely a glycerol-water droplet and a 1,2-propanediol-water droplet. We obtain different Ar, larger or smaller than a unit by varying a series of droplet heights, which corresponds to cases with or without gravitational effects, respectively. Finally, we simulate the process numerically, finding good agreement with the experimental results and again confirming our interpretation.

physics.flu-dyn↗

arXiv2018

A bouncing oil droplet in a stratified liquid and its sudden death

Droplets can self-propel when immersed in another liquid in which a concentration gradient is present. Here we report the experimental and numerical study of a self-propelling oil droplet in a vertically stratified ethanol/water mixture: At first, the droplet sinks slowly due to gravity, but then, before having reached its density matched position, jumps up suddenly. More remarkably, the droplet bounces repeatedly with an ever increasing jumping distance, until all of a sudden it stops after about 30 min. We identify the Marangoni stress at the droplet/liquid interface as responsible for the jumping: its strength grows exponentially because it pulls down ethanol-rich liquid, which in turn increases its strength even more. The jumping process can repeat because gravity restores the system. Finally, the sudden death of the jumping droplet is also explained. Our findings have demonstrated a type of prominent droplet bouncing inside a continuous medium with no wall or sharp interface.

physics.flu-dyn↗

arXiv2018

Microdroplets nucleation by dissolution of a multicomponent drop in a host liquid

Multicomponent liquid drops in a host liquid are very relevant in various technological applications. Their dissolution or growth dynamics is complex. Differences in solubility between the drop components combined with the solutal Marangoni effect and natural convections contribute to this complexity, which can be even further increased in combination with the ouzo effect, i.e., the spontaneous nucleation of microdroplets due to composition-dependent miscibilities in a ternary system. The quantitive understanding of this combined process is important for applications in industry, particularly for modern liquid-liquid microextraction processes. In this work, as a model system, we experimentally and theoretically explore water/ethanol drops dissolving in anethole oil. During the dissolution, we observed two types of microdroplets nucleation, namely water microdroplet nucleation in the surrounding oil at drop midheight and oil microdroplet nucleation in the aqueous drop, again at midheight. The nucleated oil microdroplets are driven by Marangoni flows inside the aqueous drop and evolve into microdroplets rings. A one-dimensional multiphase and multicomponent diffusion model in combination with thermodynamical equilibrium theory is proposed to predict the behavior of spontaneous emulsification, i.e. the microdroplet nucleation, that is triggered by diffusion. A scale analysis together with experimental investigations of the fluid dynamics of the system reveals that both the solutal Marangoni flow inside the drop and the buoyancy-driven flow in the host liquid influence the diffusion-triggered emulsification process. Our work provides a physical understanding of the microdroplet nucleation by dissolution of a multicomponent drop in a host liquid.

physics.flu-dyn↗

arXiv2018

Evaporation-triggered segregation of sessile binary droplets

Droplet evaporation of multicomponent droplets is essential for various physiochemical applications, e.g. in inkjet printing, spray cooling and microfabrication. In this work, we observe and study phase segregation of an evaporating sessile binary droplet, consisting of a mixture of water and a surfactant-like liquid (1,2-hexanediol). The phase segregation (i.e., demixing) leads to a reduced water evaporation rate of the droplet and eventually the evaporation process ceases due to shielding of the water by the non-volatile 1,2-hexanediol. Visualizations of the flow field by particle image velocimetry and numerical simulations reveal that the timescale of water evaporation at the droplet rim is faster than that of the Marangoni flow, which originates from the surface tension difference between water and 1,2-hexanediol, eventually leading to segregation.

physics.flu-dyn↗

arXiv2017

Evaporating pure, binary and ternary droplets: thermal effects and axial symmetry breaking

The Greek aperitif Ouzo is not only famous for its specific anise-flavored taste, but also for its ability to turn from a transparent miscible liquid to a milky-white colored emulsion when water is added. Recently, it has been shown that this so-called Ouzo effect, i.e. the spontaneous emulsification of oil microdroplets, can also be triggered by the preferential evaporation of ethanol in an evaporating sessile Ouzo drop, leading to an amazingly rich drying process with multiple phase transitions [H. Tan et al., Proc. Natl. Acad. Sci. USA 113(31) (2016) 8642]. Due to the enhanced evaporation near the contact line, the nucleation of oil droplets starts at the rim which results in an oil ring encircling the drop. Furthermore, the oil droplets are advected through the Ouzo drop by a fast solutal Marangoni flow. In this article, we investigate the evaporation of mixture droplets in more detail, by successively increasing the mixture complexity from pure water over a binary water-ethanol mixture to the ternary Ouzo mixture (water, ethanol and anise oil). In particular, axisymmetric and full three-dimensional finite element method simulations have been performed on these droplets to discuss thermal effects and the complicated flow in the droplet driven by an interplay of preferential evaporation, evaporative cooling and solutal and thermal Marangoni flow. By using image analysis techniques and micro-PIV measurements, we are able to compare the numerically predicted volume evolutions and velocity fields with experimental data. The Ouzo droplet is furthermore investigated by confocal microscopy. It is shown that the oil ring predominantly emerges due to coalescence.

physics.flu-dyn↗