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 compared to interfacial forces, especially on small scales. Consequently, the effect of a stable stratification on the Marangoni instability has hitherto been ignored. Here, however, we show that they can matter. We report, for an immiscible drop immersed in a stably stratified ethanol-water mixture, a new type of oscillatory solutal Marangoni instability that 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 strongly amplified in confined geometries, leading to an earlier onset.

How ambient conditions affect the Leidenfrost temperature.

By sufficiently heating a solid, a sessile drop can be prevented from contacting the surface by floating on its own vapour. While certain aspects of the dynamics of this so-called Leidenfrost effect are understood, it is still unclear why a minimum temperature (the Leidenfrost temperature TL) is required before the effect manifests itself, what properties affect this temperature, and what physical principles govern it. Here we investigate the dependence of the Leidenfrost temperature on the ambient conditions: first, by increasing (decreasing) the ambient pressure, we find an increase (decrease) in TL. We propose a rescaling of the temperature which allows us to collapse the curves for various organic liquids and water onto a single master curve, which yields a powerful tool to predict TL. Secondly, increasing the ambient temperature stabilizes meta-stable, levitating drops at increasingly lower temperatures below TL. This observation reveals the importance of thermal Marangoni flow in describing the Leidenfrost effect accurately. Our results shed new light on the mechanisms playing a role in the Leidenfrost effect and may help to eventually predict the Leidenfrost temperature and achieve complete understanding of the phenomenon, however, many questions still remain open.

Plasmonic Microbubble Dynamics in Binary Liquids.

The growth of surface plasmonic microbubbles in binary water/ethanol solutions is experimentally studied. The microbubbles are generated by illuminating a gold nanoparticle array with a continuous wave laser. Plasmonic bubbles exhibit ethanol concentration-dependent behaviors. For low ethanol concentrations (fe) of ≲67.5%, bubbles do not exist at the solid-liquid interface. For high fe values of ≳80%, the bubbles behave as in pure ethanol. Only in an intermediate window of 67.5% ≲ fe ≲ 80% do we find sessile plasmonic bubbles with a highly nontrivial temporal evolution, in which as a function of time three phases can be discerned. (1) In the first phase, the microbubbles grow, while wiggling. (2) As soon as the wiggling stops, the microbubbles enter the second phase in which they suddenly shrink, followed by (3) a steady reentrant growth phase. Our experiments reveal that the sudden shrinkage of the microbubbles in the second regime is caused by a depinning event of the three-phase contact line. We systematically vary the ethanol concentration, laser power, and laser spot size to unravel water recondensation as the underlying mechanism of the sudden bubble shrinkage in phase 2.

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.

Dynamics of Formation of a Vapor Nanobubble Around a Heated Nanoparticle.

We study the formation of a nanobubble around a heated nanoparticle in a bulk liquid by using molecular dynamics simulations. The nanoparticle is kept at a temperature above the critical temperature of the surrounding liquid, leading to the formation of a vapor nanobubble attached to it. First, we study the role of both the temperature of the bulk liquid far away from the nanoparticle surface and the temperature of the nanoparticle itself on the formation of a stable vapor nanobubble. We determine the exact conditions under which it can be formed and compare this with the conditions that follow from a macroscopic heat balance argument. Next, we demonstrate the role of dissolved gas on the conditions required for nucleation of a nanobubble and on its growth dynamics. We find that beyond a certain threshold concentration, the dissolved gas dramatically facilitates vapor bubble nucleation due to the formation of gaseous weak spots in the surrounding liquid.

Dynamic Leidenfrost Effect: Relevant Time and Length Scales.

When a liquid droplet impacts a hot solid surface, enough vapor may be generated under it to prevent its contact with the solid. The minimum solid temperature for this so-called Leidenfrost effect to occur is termed the Leidenfrost temperature, or the dynamic Leidenfrost temperature when the droplet velocity is non-negligible. We observe the wetting or drying and the levitation dynamics of the droplet impacting on an (isothermal) smooth sapphire surface using high-speed total internal reflection imaging, which enables us to observe the droplet base up to about 100 nm above the substrate surface. By this method we are able to reveal the processes responsible for the transitional regime between the fully wetting and the fully levitated droplet as the solid temperature increases, thus shedding light on the characteristic time and length scales setting the dynamic Leidenfrost temperature for droplet impact on an isothermal substrate.

The speed of sound in a gas-vapour bubbly liquid.

In addition to the vapour of the liquid, bubbles in cavitating flows usually contain also a certain amount of permanent gas that diffuses out of the liquid as they grow. This paper presents a simplified linear model for the propagation of monochromatic pressure waves in a bubbly liquid with these characteristics. Phase change effects are included in detail, while the gas is assumed to follow a polytropic law. It is shown that even a small amount of permanent gas can have a major effect on the behaviour of the system. Particular attention is paid to the low-frequency range, which is of special concern in flow cavitation. Numerical results for water and liquid oxygen illustrate the implications of the model.

Tribonucleation of bubbles.

We report on the nucleation of bubbles on solids that are gently rubbed against each other in a liquid. The phenomenon is found to depend strongly on the material and roughness of the solid surfaces. For a given surface, temperature, and gas content, a trail of growing bubbles is observed if the rubbing force and velocity exceed a certain threshold. Direct observation through a transparent solid shows that each bubble in the trail results from the early coalescence of several microscopic bubbles, themselves detaching from microscopic gas pockets forming between the solids. From a detailed study of the wear tracks, with atomic force and scanning electron microscopy imaging, we conclude that these microscopic gas pockets originate from a local fracturing of the surface asperities, possibly enhanced by chemical reactions at the freshly created surfaces. Our findings will be useful either for preventing undesired bubble formation or, on the contrary, for "writing with bubbles," i.e., creating controlled patterns of microscopic bubbles.

The Leidenfrost temperature increase for impacting droplets on carbon-nanofiber surfaces.

Droplets impacting on a superheated surface can either exhibit a contact boiling regime, in which they make direct contact with the surface and boil violently, or a film boiling regime, in which they remain separated from the surface by their own vapor. The transition from the contact to the film boiling regime depends not only on the temperature of the surface and the kinetic energy of the droplet, but also on the size of the structures fabricated on the surface. Here we experimentally show that surfaces covered with carbon-nanofibers delay the transition to film boiling to much higher temperatures compared to smooth surfaces. We present physical arguments showing that, because of the small scale of the carbon fibers, they are cooled by the vapor flow just before the liquid impact, thus permitting contact boiling up to much higher temperatures than on smooth surfaces. We also show that as long as the impact is in the film boiling regime, the spreading factor of impacting droplets is consistent with the We(3/10) scaling (with We being the Weber number) as predicted for large We by a scaling analysis.

Effects of particle settling on Rayleigh-Bénard convection.

The effect of particles falling under gravity in a weakly turbulent Rayleigh-Bénard gas flow is studied numerically. The particle Stokes number is varied between 0.01 and 1 and their temperature is held fixed at the temperature of the cold plate, of the hot plate, or the mean between these values. Mechanical, thermal, and combined mechanical and thermal couplings between the particles and the fluid are studied separately. It is shown that the mechanical coupling plays a greater and greater role in the increase of the Nusselt number with increasing particle size. A rather unexpected result is an unusual kind of reverse one-way coupling, in the sense that the fluid is found to be strongly influenced by the particles, while the particles themselves appear to be little affected by the fluid, despite the relative smallness of the Stokes numbers. It is shown that this result derives from the very strong constraint on the fluid behavior imposed by the vanishing of the mean fluid vertical velocity over the cross sections of the cell demanded by continuity.

Growing bubbles in a slightly supersaturated liquid solution.

We have designed and constructed an experimental system to study gas bubble growth in slightly supersaturated liquids. This is achieved by working with carbon dioxide dissolved in water, pressurized at a maximum of 1 MPa and applying a small pressure drop from saturation conditions. Bubbles grow from hydrophobic cavities etched on silicon wafers, which allows us to control their number and position. Hence, the experiment can be used to investigate the interaction among bubbles growing in close proximity when the main mass transfer mechanism is diffusion and there is a limited availability of the dissolved species.

A general derivation of the subharmonic threshold for non-linear bubble oscillations.

The paper describes an approximate but rather general derivation of the acoustic threshold for a subharmonic component to be possible in the sound scattered by an insonified gas bubble. The general result is illustrated with several specific models for the mechanical behavior of the surface coating of bubbles used as acoustic contrast agents. The approximate results are found to be in satisfactory agreement with fully non-linear numerical results in the literature. The amplitude of the first harmonic is also found by the same method. A fundamental feature identified by the analysis is that the subharmonic threshold can be considerably lowered with respect to that of an uncoated free bubble if the mechanical response of the coating varies rapidly in the neighborhood of certain specific values of the bubble radius, e.g., because of buckling.

Heat transport in bubbling turbulent convection.

Boiling is an extremely effective way to promote heat transfer from a hot surface to a liquid due to numerous mechanisms, many of which are not understood in quantitative detail. An important component of the overall process is that the buoyancy of the bubble compounds with that of the liquid to give rise to a much-enhanced natural convection. In this article, we focus specifically on this enhancement and present a numerical study of the resulting two-phase Rayleigh-Bénard convection process in a cylindrical cell with a diameter equal to its height. We make no attempt to model other aspects of the boiling process such as bubble nucleation and detachment. The cell base and top are held at temperatures above and below the boiling point of the liquid, respectively. By keeping this difference constant, we study the effect of the liquid superheat in a Rayleigh number range that, in the absence of boiling, would be between 2 × 10(6) and 5 × 10(9). We find a considerable enhancement of the heat transfer and study its dependence on the number of bubbles, the degree of superheat of the hot cell bottom, and the Rayleigh number. The increased buoyancy provided by the bubbles leads to more energetic hot plumes detaching from the cell bottom, and the strength of the circulation in the cell is significantly increased. Our results are in general agreement with recent experiments on boiling Rayleigh-Bénard convection.

Ultrasound artificially nucleated bubbles and their sonochemical radical production.

We describe the ejection of bubbles from air-filled pits micromachined on a silicon surface when exposed to ultrasound at a frequency of approximately 200 kHz. As the pressure amplitude is increased the bubbles ejected from the micropits tend to be larger and they interact in complex ways. With more than one pit, there is a threshold pressure beyond which the bubbles follow a trajectory parallel to the substrate surface and converge at the center point of the pit array. We have determined the size distribution of bubbles ejected from one, two and three pits, for three different pressure amplitudes and correlated them with sonochemical OH· radical production. Experimental evidence of shock wave emission from the bubble clusters, deformed bubble shapes and jetting events that might lead to surface erosion are presented. We describe numerical simulations of sonochemical conversion using the empirical bubble size distributions, and compare the calculated values with experimental results.

Spatial distribution of heat flux and fluctuations in turbulent Rayleigh-Bénard convection.

We numerically investigate the radial dependence of the velocity and temperature fluctuations and of the time-averaged heat flux j ¯(r) in a cylindrical Rayleigh-Bénard cell with aspect ratio Γ=1 for Rayleigh numbers Ra between 2×10^{6} and 2×10^{9} at a fixed Prandtl number Pr=5.2. The numerical results reveal that the heat flux close to the sidewall is larger than in the center and that, just as the global heat transport, it has an effective power law dependence on the Rayleigh number, j ¯(r)∝Ra{γ{j}(r)}. The scaling exponent γ{j}(r) decreases monotonically from 0.43 near the axis (r≈0) to 0.29 close to the sidewalls (r≈D/2). The effective exponents near the axis and the sidewall agree well with the measurements of Shang et al. [Phys. Rev. Lett. 100, 244503 (2008)] and the predictions of Grossmann and Lohse [Phys. Fluids 16, 1070 (2004)]. Extrapolating our results to large Rayleigh number would imply a crossover at Ra≈10^{15}, where the heat flux near the axis would begin to dominate. In addition, we find that the local heat flux is more than twice as high at the location where warm or cold plumes go up or down than in plume depleted regions.

Drop impact on superheated surfaces.

At the impact of a liquid droplet on a smooth surface heated above the liquid's boiling point, the droplet either immediately boils when it contacts the surface ("contact boiling"), or without any surface contact forms a Leidenfrost vapor layer towards the hot surface and bounces back ("gentle film boiling"), or both forms the Leidenfrost layer and ejects tiny droplets upward ("spraying film boiling"). We experimentally determine conditions under which impact behaviors in each regime can be realized. We show that the dimensionless maximum spreading γ of impacting droplets on the heated surfaces in both gentle and spraying film boiling regimes shows a universal scaling with the Weber number We (γ~We(2/5)), which is much steeper than for the impact on nonheated (hydrophilic or hydrophobic) surfaces (γ~We(1/4)). We also interferometrically measure the vapor thickness under the droplet.

Effect of vapor bubbles on velocity fluctuations and dissipation rates in bubbly Rayleigh-Bénard convection.

Numerical results for kinetic and thermal energy dissipation rates in bubbly Rayleigh-Bénard convection are reported. Bubbles have a twofold effect on the flow: on the one hand, they absorb or release heat to the surrounding liquid phase, thus tending to decrease the temperature differences responsible for the convective motion; but on the other hand, the absorbed heat causes the bubbles to grow, thus increasing their buoyancy and enhancing turbulence (or, more properly, pseudoturbulence) by generating velocity fluctuations. This enhancement depends on the ratio of the sensible heat to the latent heat of the phase change, given by the Jakob number, which determines the dynamics of the bubble growth.

Validation of an approximate model for the thermal behavior in acoustically driven bubbles.

The chemical production of radicals inside acoustically driven bubbles is determined by the local temperature inside the bubbles. Therefore, modeling of chemical reaction rates in bubbles requires an accurate evaluation of the temperature field and the heat exchange with the liquid. The aim of the present work is to compare a detailed partial differential equation model in which the temperature field is spatially resolved with an ordinary differential equation model in which the bubble contents are assumed to have a uniform average temperature and the heat exchanges are modeled by means of a boundary layer approximation. The two models show good agreement in the range of pressure amplitudes in which the bubble is spherically stable.

Dynamics of a disturbed sessile drop measured by atomic force microscopy (AFM).

A new method for studying the dynamics of a sessile drop by atomic force microscopy (AFM) is demonstrated. A hydrophobic microsphere (radius, r ∼ 20-30 µm) is brought into contact with a small sessile water drop resting on a polytetrafluoroethylene (PTFE) surface. When the microsphere touches the liquid surface, the meniscus rises onto it because of capillary forces. Although the microsphere volume is 6 orders of magnitude smaller than the drop, it excites the normal resonance modes of the liquid interface. The sphere is pinned at the interface, whose small (<100 nm) oscillations are readily measured with AFM. Resonance oscillation frequencies were measured for drop volumes between 5 and 200 µL. The results for the two lowest normal modes are quantitatively consistent with continuum calculations for the natural frequency of hemispherical drops with no adjustable parameters. The method may enable sensitive measurements of volume, surface tension, and viscosity of small drops.