In the Leidenfrost effect, liquid drops deposited on a hot surface levitate on a thin vapor cushion fed by evaporation of the liquid. This vapor layer forms a concave depression in the drop interface. Using laser-light interference coupled to high-speed imaging, we measured the radius, curvature, and height of the vapor pocket, as well as non-axisymmetric fluctuations of the interface for water drops at different temperatures. The geometry of the vapor pocket depends primarily on the drop size and not on the substrate temperature.
Above a critical temperature known as the Leidenfrost point (LFP), a heated surface can suspend a liquid droplet above a film of its own vapor. The insulating vapor film can be highly detrimental in metallurgical quenching and thermal control of electronic devices, but may also be harnessed to reduce drag and generate power. Manipulation of the LFP has occurred mostly through experiment, giving rise to a variety of semi-empirical models that account for the Rayleigh-Taylor instability, nucleation rates, and superheat limits. However, a truly comprehensive model has been difficult given that th…
We show that thermal creep is at the origin of the recently discovered Leidenfrost ratchet, where liquid droplets float on a vapor layer along a heated sawtooth surface and accelerate to velocities of up to 40 cm=s. As the active element, the asymmetric temperature profile at each ratchet summit rectifies the vapor flow in the boundary layer. This mechanism works at low Reynolds number and provides a novel tool for controlling gas flow at nanostructured surfaces.
We report on the collision-coalescence dynamics of drops in Leidenfrost state using liquids with different physicochemical properties. Drops of the same liquid deposited on a hot concave surface coalesce practically at contact, but when drops of different liquids collide, they can bounce several times before finally coalescing when the one that evaporates faster reaches a critical size, of the order of the capillary length. The bouncing dynamics is produced because the drops are not only in Leidenfrost state with the substrate, they also experience Leidenfrost effect between them at the moment…
The mobility of Leidenfrost drop has been exploited for the manipulation of drop motions. In the classical model, the Leidenfrost drop was levitated by a vapor cushion, in the absence of touch to the surface. Here we report a standing Leidenfrost state on a heated hydrophobic surface where drop stands on the surface with partial adhesion and further self-rotates like Sufi-whirling. To elucidate this new phenomenon, we imaged the evolution of the partial adhesion, the inner circulation, and the ellipsoidal rotation of the drop. The stable partial adhesion is accompanied by thermal and mechanica…
We experimentally investigate the effect of an electric field applied between a Leidenfrost droplet and the heated substrate on which it is levitating. We quantify the electro-Leidenfrost effect by imaging the interference fringes between the liquid-vapour and vapour-substrate interfaces. The increase of the voltage induces a decrease of the vapour layer thickness. Above a certain critical voltage the Leidenfrost effect is suppressed and the drop starts boiling. Our study characterizes this way to control and/or to avoid the Leidenfrost effect that is undesirable in many domains such as metall…
We experimentally investigate the Leidenfrost effect at pressures ranging from 1 to 0.05 atmospheric pressure. As a direct consequence of the Clausius-Clapeyron phase diagram of water, the droplet temperature can be at ambient temperature in a non-sophisticated lab environment. Furthermore, the lifetime of the Leidenfrost droplet is significantly increased in this low pressure environment. The temperature and pressure dependance of the evaporation rate are successfully tested against a recently proposed model. These results may pave a way to reach efficient Leidenfrost micro-fluidic and milli-…
The Leidenfrost effect describes liquid drops under gravity levitating on a vapour cushion, which is sourced at the liquid-vapour interface from evaporation caused by the hot substrate below. It has been experimentally observed that when two or more Leidenfrost drops approach one another, there is a short-range repulsion that can prevent coalescence. In the present work, we investigate the coalescence process of initially momentum-less Leidenfrost drops. This is carried out by numerically simulating two-dimensional systems of liquid and vapour using the recently developed dynamic van der Waals…
When a liquid droplet impacts a hot solid surface, enough vapor may be generated under it as 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/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 surfac…
We consider the flotation of deformable, non-wetting drops on a liquid interface. We consider the deflection of both the liquid interface and the droplet itself in response to the buoyancy forces, density difference and the various surface tensions within the system. Our results suggest new insight into a range of phenomena in which such drops occur, including Leidenfrost droplets and floating liquid marbles. In particular, we show that the floating state of liquid marbles is very sensitive to the tension of the particle-covered interface and suggest that this sensitivity may make such experim…
We show that a volatile liquid drop placed at the surface of a non-volatile liquid pool warmer than the boiling point of the drop can experience a Leidenfrost effect even for vanishingly small superheats. Such an observation points to the importance of the substrate roughness, negligible in the case considered here, in determining the threshold Leidenfrost temperature. A theoretical model based on the one proposed by Sobac et al. [Phys. Rev. E 90, 053011 (2014)] is developed in order to rationalize the experimental data. The shapes of the drop and of the substrate are analyzed. The model notab…
Drops deposited on an evaporating liquid bath can be maintained in an inverse Leidenfrost state by the vapor emanating from the bath, making them levitate and hover almost without friction. These perfectly non-wetting droplets create a depression in the liquid interface that sustains their weight, which generates repellent forces when they approach a meniscus rising against a wall. Here, we study this reflection in detail, and show that frictionless Leidenfrost drops are a simple and efficient tool to probe the shape of an unknown interface. We then use the menisci to control the motion of the…
The Leidenfrost effect-prolonged evaporation of droplets on a superheated surface-happens only when the surface temperature is above a certain transitional value. Here, we show that specially engineered droplets - liquid marbles - can exhibit similar effect at any superheated temperatures (up to 465 oC tested in our experiment) without a transition. Very possibly, this phenomenon is due to the fact that liquid marbles are droplets coated with microparticles and these microparticles help levitate the liquid core and maintain an insulation layer between the liquid and the superheated surface.
When deposited on a hot bath, volatile drops are observed to stay in levitation: the so-called Leidenfrost effect. Here, we discuss drop dynamics in an inverse Leidenfrost situation where room-temperature drops are deposited on a liquid nitrogen pool, and levitate on a vapor film generated by evaporation of the bath. In the seconds following deposition, we observe that the droplets start to glide on the bath along a straight path, only disrupted by elastic bouncing close to the edges of the container. Initially at rest, these self-propelled drops accelerate within a few seconds and reach veloc…
The present article highlights the role of non-Newtonian (elastic) effects on the droplet impact phenomenology at temperatures considerably higher than the boiling point, especially at or above the Leidenfrost regime. The Leidenfrost point (LFP) was found to decrease with increase in the impact Weber number (based on velocity just before the impact) for fixed polymer (Polyacrylamide, PAAM) concentrations. Water droplets fragmented at very low Weber numbers (~22), whereas the polymer droplets resisted fragmentation at much higher Weber numbers (~155). We also varied the polymer concentration an…
It is demonstrated that non-coalescent droplets of acetone can be formed on liquid substrates. The fluid flows around and in an acetone droplet hovering on water are recorded to shed light on the mechanisms which might lead to non-coalescence. For sufficiently low impact velocities, droplets undergo a damped oscillation on the surface of the liquid substrate but at higher velocities clean bounce-off occurs. Comparisons of experimentally observed static configurations of floating droplets to predictions from a theoretical model for a small non-wetting rigid sphere resting on a liquid substrate …
We investigate the different boiling régimes around a single continuously laser-heated 80 nm gold nanoparticle and draw parallels to the classical picture of boiling. Initially, nanoscale boiling takes the form of transient, inertia-driven, unsustainable boiling events characteristic of a nanoscale boiling crisis. At higher heating power, nanoscale boiling is continuous, with a vapor film being sustained during heating for at least up to 20 $μ$s. Only at high heating powers does a substantial stable vapour nanobubble form. At intermediate heating powers, unstable boiling sometimes takes the fo…
The Leidenfrost effect occurs when an object near a hot surface vaporizes rapidly enough to lift itself up and hover. Although well-understood for liquids and stiff sublimable solids, nothing is known about the effect with materials whose stiffness lies between these extremes. Here we introduce a new phenomenon that occurs with vaporizable soft solids: the elastic Leidenfrost effect. By dropping hydrogel spheres onto hot surfaces we find that, rather than hovering, they energetically bounce several times their diameter for minutes at a time. With high-speed video during a single impact, we unc…
Droplet vaporization has a great impact on combustion of liquid fuels and might greatly affects the engine performance. Physical understanding and theoretical interpretation of the droplet vaporization behavior are decisive to constitute appropriate models for spray combustion. In this work, we proposed a fully transient formulation for the droplet vaporization at wide ranges of temperature and pressure. The governing equations are solved analytically by means of suitable coordinate transformations. The droplet surface temperature and mass fraction of fuel vapor are determined by the matching …
Evaporation of a liquid drop surrounded by either vapor of the same fluid, or vapor and air, is usually attributed to vapor diffusion -- which, however, does not apply to the former setting, as pure fluids do not diffuse. The present paper puts forward an additional mechanism, one that applies to both settings. It is shown that disparities between the drop and vapor in terms of their pressure and chemical potential give rise to a flow. Its direction depends on the vapor density and the drop's size. In undersaturated or saturated vapor, all drops evaporate -- but in oversaturated (yet thermodyn…
It is well-known that liquid and saturated vapor, separated by a flat interface in an unbounded space, are in equilibrium. One would similarly expect a liquid drop, sitting on a flat substrate, to be in equilibrium with the vapor surrounding it. Yet, it is not: as shown in this work, the drop evaporates. Mathematically, this conclusion is deduced using the diffuse-interface model, but it can also be reformulated in terms of the maximum-entropy principle, suggesting model independence. Physically, evaporation of drops is due to the so-called Kelvin effect, which gives rise to a liquid-to-vapor …
We investigate freely expanding sheets formed by ultrasoft gel beads, and liquid and viscoelastic drops, produced by the impact of the bead or drop on a silicon wafer covered with a thin layer of liquid nitrogen that suppresses viscous dissipation thanks to an inverse Leidenfrost effect. Our experiments show a unified behaviour for the impact dynamics that holds for solids, liquids, and viscoelastic fluids and that we rationalize by properly taking into account elastocapillary effects. In this framework, the classical impact dynamics of solids and liquids as far as viscous dissipation is negli…
Evaporating droplets are known to show complex motion that has conventionally been explained by the Marangoni effect (flow induced by the gradient of surface tension). Here, we show that the droplet motion can be induced even in the absence of the Marangoni effect due to the gradient of evaporation rate. We derive an equation for the velocity of a droplet subject to non-uniform evaporation rate and non-uniform surface tension placed on an inert substrate where the wettability is uniform and unchanged. The equation explains the previously observed attraction-repulsion- chasing behaviors of evap…
When a liquid drop impacts on a heated substrate, it can remain deposited, or violently boil in contact, or lift off with or without ever touching the surface. The latter is known as the Leidenfrost effect. The duration and area of the liquid--substrate contact is highly relevant for the heat transfer, as well as other effects such as corrosion. However, most experimental studies rely on side view imaging to determine contact times, and those are often mixed with the time until the drop lifts off from the substrate. Here, we develop and validate a reliable method of contact time determination …
The multivariable theory of nucleation [N. V. Alekseechkin, J. Chem. Phys. 124, 124512 (2006)] is applied to the droplet nucleation in a supersaturated single-component vapor; the droplet volume V, temperature T, and volume change rate U=V_dot are the variables of the theory. A new approach based on macroscopic kinetics is developed for the droplet evolution and results in the derived equations for U_dot, V_dot, and T_dot. It is shown that there is no the viscosity effect in the employed ideal gas approximation, so the variable U can be omitted. The nonisothermal effect (the discrepancy betwee…
Patterning the wettability of solid surfaces is a successful strategy to control the dropwise condensation of vapor onto partially wetting solid surfaces. We followed the condensation of water vapor onto electrowetting-functionalized surfaces with structured co-planar electrodes. A detailed analysis of the experimental distribution of millions of drops reveals that despite the presence of contact angle hysteresis and the occurrence of random drop coalescence events, the preferential drop position closely follows the evolution of the local minima of the numerically calculated drop size-dependen…
Results for the kinetics of vapor-liquid transitions, following temperature quenches with different densities, are presented from the molecular dynamics simulations of a Lennard-Jones system. For critical density, bicontinuous liquid and vapor domains are observed which grow with time obeying the prediction of hydrodynamic mechanism. On the other hand, for quenches with density significantly below the critical one, phase separation progresses via nucleation and growth of liquid droplets. In the latter case, Brownian diffusion and collision mechanism for the droplet growth is confirmed. We also…
In 1897 Ostwald formulated his step rule for formation of the most stable crystal state for a system with crystal polymorphism. The rule describes the irreversible way a system converts to the crystal with lowest free energy. But in fact the irreversible way a supercooled gas below the triple point temperature $T_{tr.p.}$ crystallizes via a liquid droplet is an example of Ostwald's step rule. The homogeneous nucleation in the supersaturated gas is not to a crystal, but to a liquid-like critical nucleus. We have for the first time performed constant energy (NVE) Molecular Dynamics (MD) of homog…
The impact of nanometer sized drops on solid surfaces is studied using molecular dynamics simulations. Equilibrated floating drops consisting of short chains of Lennard-Jones liquids with adjustable volatility are directed normally onto an atomistic solid surface where they are observed to bounce, stick, splash or disintegrate, depending on the initial velocity and the nature of the materials involved. Drops impacting at low velocity bounce from non-wetting surfaces but stick and subsequently spread slowly on wetting surfaces. Higher velocity impacts produce an prompt splash followed by disint…
Molecular dynamics simulations of miscible and partially miscible binary Lennard--Jones mixtures are used to study the dynamics and thermodynamics of vapor condensation onto a non-volatile liquid drop in the canonical ensemble. When the system volume is large, the driving force for condensation is low and only a submonolayer of the solvent is adsorbed onto the liquid drop. A small degree of mixing of the solvent phase into the core of the particles occurs for the miscible system. At smaller volumes complete film formation is observed and the dynamics of film growth are dominated by cluster-clu…
Results for the kinetics of vapor-liquid phase transition have been presented from the molecular dynamics simulations of a single component two-dimensional Lennard-Jones fluid. The phase diagram for the model, primary prerequisite for this purpose, has been obtained via the Monte Carlo simulations. Our focus is on the region very close to the vapor branch of the coexistence curve. Quenches to such region provide morphology that consists of disconnected circular liquid clusters in the vapor background. We identified that these clusters exhibit diffusive motion and grow via sticky collisions amo…
Subject of this work is to investigate the kinetics of mass transfer of volatile amphiphiles from their vapors to aqueous drops, and from the saturated aqueous drop solutions to air. The used amphiphiles are benzyl acetate, linalool, and citronellol. The adequate theoretical processing of the equilibrium surface tension isotherms is applied to construct the two-dimensional equation of state, which relates the surface tension to the adsorption at the interface. The measured surface tension relaxations with time in the regimes of adsorption from vapor and evaporation from drop combined with the …
We investigate freely expanding viscoelastic sheets. The sheets are produced by the impact of drops on a quartz plate covered with a thin layer of liquid nitrogen that suppresses shear viscous dissipation as a result of the cold Leidenfrost effect. The time evolution of the sheet is simultaneously recorded from top and side views using high-speed cameras. The investigated viscoelastic fluids are Maxwell fluids, which are characterized by low elastic moduli, and relaxation times that vary over almost two orders of magnitude, thus giving access to a large spectrum of viscoelastic and elastocapil…
Marangoni self-contracted droplets are formed by a mixture of two liquids, one of larger surface tension and larger evaporation rate than the other. Due to evaporation, the droplets contract to a stable contact angle instead of spreading on a wetting substrate. This gives them unique properties, including absence of pinning force and ability to move under vapor gradients, self- and externally imposed. We first model the dynamics of attraction in an unconfined geometry and then study the effects of confinement on the attraction range and dynamics, going from minimal confinement (vertical bounda…
A method of simulating the drying process of a soft matter solution with an implicit solvent model by moving the liquid-vapor interface is applied to various solution films and droplets. For a solution of a polymer and nanoparticles, we observe "polymer-on-top" stratification, similar to that found previously with an explicit solvent model. Furthermore, "polymer-on-top" is found even when the nanoparticle size is smaller than the radius of gyration of the polymer chains. For a suspension droplet of a bidisperse mixture of nanoparticles, we show that core-shell clusters of nanoparticles can be …
We study the interaction of a liquid drop with an elastic beam in the case where bending effects dominate. We use a variational approach to derive equilibrium equations for the system in the presence of gravity and in the presence or absence of contact line pinning. We show that the derived equilibrium equations for the beam subsystem reveal the external forces applied on the beam by the liquid and vapor phases. Among these, the force applied at the triple line (the curve where the three phases meet) is found to lie along the liquid-vapor interface.
We present a multi-phase-field model to describe quantitatively nanowire growth by the vapor-liquid-solid (VLS) process. The free-energy functional of this model depends on three non-conserved order parameters that distinguish the vapor, liquid, and solid phases. The evolution equations for those order parameters describe basic kinetic processes including the rapid (quasi-instantaneous) equilibration of the liquid catalyst to a droplet shape with constant mean curvature, the slow incorporation of growth atoms at the droplet surface, and crystallization within the droplet. The standard constrai…
Saliva is primarily composed of water, but additionally includes a variety of organic and inorganic substances such as salt, proteins, peptides, mucins, virions, etc. The presence of such solutes affects the evaporation time of respiratory droplets that are sedimenting in air, and thereby the airborne transmission of infections. From solutions of the coupled heat-conduction and water-diffusion equations within the droplet and in the ambient vapor phase, we find that the solute-induced water vapor-pressure reduction considerably slows down the evaporation process and dominates the solute-concen…
Results from the state-of-the-art molecular dynamics simulations are presented for both equilibrium and nonequilibrium dynamics following vapor-liquid transition in a single component Lennard-Jones system. We have fixed the overall density close to the vapor-branch of the coexistence curve so that the liquid phase forms droplet structure in the background of vapor phase. In the equilibrium case, the motion of a single droplet is studied in both microcanonical and canonical ensembles, in the latter case a hydrodynamics preserving Nosé-Hoover thermostat was used to control the temperature. The d…
We study liquid-vapor phase separation under shear via the Shan-Chen lattice Boltzmann model. Besides the rheological characteristics, we analyze the Kelvin-Helmholtz(K-H) instability resulting from the tangential velocity difference of the fluids on two sides of the interface. We discuss also the growth behavior of droplets. The domains being close to the walls are lamellar-ordered, where the hydrodynamic effects dominate. The patterns in the bulk of the system are nearly isotropic, where the domain growth results mainly from the diffusion mechanism. Both the interfacial tension and the K-H i…
Recent advances in nano-rheology require that new methods and models be developed to describe the equilibrium and non-equilibrium properties of entangled polymeric materials and their interfaces at a molecular level of detail. In this work we present a Slip-Spring (SLSP) model capable of describing the dynamics of entangled polymers at interfaces, including explicit liquid-vapor and liquid-solid interfaces. The highly coarse-grained approach adopted with this model enables simulation of entire nano-rheological characterization systems within a particle-level base description. Many-body dissipa…
In spite of significant advances in replication technologies, methods to produce well-defined three dimensional structures are still at its infancy. Such a limitation would be evident if we were to produce a large array of simple and, especially, compound convex lenses, also guaranteeing that their surfaces would be molecularly smooth. Here, we report a novel method to produce such structures by cloning the 3D shape of nectar drops, found widely in nature, using conventional soft lithography.The elementary process involves transfer of a thin patch of the sugar solution coated on a glass slide …
Close to the triple point, the surface of ice is covered by a thin liquid layer (so-called quasi-liquid layer) which crucially impacts growth and melting rates. Experimental probes cannot observe the growth processes below this layer, and classical models of growth by vapor deposition do not account for the formation of premelting films. Here, we develop a mesoscopic model of liquid-film mediated ice growth, and identify the various resulting growth regimes. At low saturation, freezing proceeds by terrace spreading, but the motion of the buried solid is conveyed through the liquid to the outer…
The role of metastable liquid phases in vapor-crystal nucleation is studied using Density Functional Theory(DFT). The model gives a semi-quantitatively accurate description of both the vapor-liquid-solid phase diagram for both simple fluids (Lennard-Jones interactions) and of the low-density/high-density/crystal phase diagram for model globular proteins (ten Wolde-Frenkel interaction). The density profile is characterized by two local order parameters, the average density and the crystallinity. The bulk free energy model is supplemented by squared-derivative terms in these order parameters to …
The process of nucleation of vapor bubbles from a superheated liquid and of liquid droplets from a supersaturated vapor is investigated using the Modified-Core van der Waals model Density Functional Theory (Lutsko, JCP 128, 184711 (2008)). A novel approach is developed whereby nucleation is viewed as a transition from a metastable state to a stable state via the minimum free energy path which is identified using the nudged elastic-band method for exploring free energy surfaces. This allows for the unbiased calculation of the properties of sub- and super-critical clusters, as well as of the cri…
