arXiv subjects

Christian Diddens

Publications and source records attributed to Christian Diddens.

At least 19 recordsLinked to original sources

arXiv2026

Leidenfrost droplets: The roles of ambient humidity and internal droplet circulation

A volatile droplet gently deposited on a superheated substrate can sit on a thin film of its own vapour, which prevents contact between the drop and surface. This phenomenon is called the Leidenfrost effect. In this paper, through direct numerical simulations, we analyse characteristics of Leidenfrost water droplets with a single computational model over four decades of droplet radius, stitching together previous works in the limit of large and small droplets. Using the model, we show that the ambient humidity, an underappreciated factor in the Leidenfrost system, in combination with the flow in the drop has a significant impact on the geometry and drying kinetics. Our results imply the inadequacies of commonly made assumptions of a pure vapour phase and an isothermal droplet. When modelling large Leidenfrost droplets with an axisymmetric model, large discrepancies between experiments and the computational results occur. Through azimuthal stability analysis, we show that this is due to the unrealistic constraint of axisymmetry. This finding is supported by 3D simulations of a simplified model. Finally, some hypotheses are explored to account for the remaining discrepancies with experimental data.

physics.flu-dyn↗

arXiv2025

Upstream motion of oil droplets in co-axial Ouzo flow due to Marangoni forces

To explore the physicochemical hydrodynamics of phase-separating ternary liquids (Ouzo-type), a binary oil-ethanol mixture is introduced into a co-flowing stream of water. Oil droplets nucleate at the interface between the two liquids, leading to a larger oil droplet interacting with the ethanol-rich jet. Although buoyancy forces and hydrodynamic drag forces push the droplet in downstream direction, we observe an upstream motion. Using computational fluid dynamics simulations of a simplified model system, we identify the nucleation zone for oil droplets and uncover Marangoni forces to be responsible for the upstream motion of the droplet. A semi-analytical model allows us to identify the key parameters governing this effect. A general conclusion is that Marangoni stresses can reverse the motion of droplets through channels, where the surrounding liquid is a multi-component mixture. The insights from this work are not only relevant for channel flow, but more generally, for the physicochemical hydrodynamics of multiphase, multi-component systems.

physics.flu-dyn↗

arXiv2025

Internal flow and concentration in neighbouring evaporating binary droplets and rivulets

In this paper, the evaporation of neighbouring multi-component droplets or rivulets - often found in applications such as inkjet printing, spray cooling, and pesticide delivery - is studied numerically and theoretically. The proximity induces a shielding effect that reduces individual evaporation rates and disrupts the symmetry of both the concentration profile and the flow field in the liquids. We examine how the symmetry of flow and concentration fields is affected by key parameters, namely the contact angle, the inter-droplet (or inter-rivulet) distance, and the magnitude of surface tension gradient forces (i.e. the Marangoni number). We focus on binary mixtures, such as water and 1,2-hexanediol, where only one component evaporates and evaporation is slow, thereby allowing simplifications to the governing equations. To manage the complexity of the full three-dimensional droplet problem, we begin with a two-dimensional model of neighbouring rivulets. Solving the complete transient equations for rivulets with pinned contact lines and fixed inter-rivulet distance reveals that the asymmetry - quantified by the position of the interfacial stagnation point of the flow - diminishes over time. Using a validated quasi-stationary model, we find, with increasing contact angle and inter-rivulet distance, that the stagnation point migrates closer to the centre, yet it remains unaffected by the Marangoni number. A simplified lubrication model applied to droplets shows similar dependencies on contact angle and distance, although here the stagnation point appears to vary with the Marangoni number. We attribute this dependence to the additional azimuthal flow in droplets, leading to a non-linear evolution of the concentration and therefore a non-trivial dependence of the symmetry on the Marangoni number.

physics.flu-dyn↗

arXiv2025

Hidden in plain sight: How evaporation impacts the pendant drop method

The surface tension of a liquid, which drives most free surface flows at small scales, is often measured with the pendant drop method due to its simplicity and reliability. When the drop is suspended in air, controlling the ambient temperature and humidity is usually an afterthought, resulting in evaporation of the drop during the measurement. Here, we investigate the effect of evaporation on the measured surface tension using experiments and numerical simulations. In the experiments, we measured the evolution of the droplet temperature, which can drastically reduce by ($\Delta T \approx 10 \degC$) due to evaporative cooling, and thereby altering the measured surface tension by more than 1 mN/m. This finding can be reproduced by numerical simulations, which additionally allows for controlled investigations of the individual influences of further effects on the pendant drop method, namely shape deformations by evaporation-driven flows in the gas-phase and in the liquid-phase including the resulting Marangoni flow. We provide a simple passive method to control the relative humidity without requiring additional instrumentation. Our findings are particularly pertinent to Marangoni flows which are driven by surface tension gradients, and which are consequently highly sensitive to measurement inaccuracies. We apply our method with different aqueous mixtures of glycerol and various diols. Our results and insights have implications for various applications, ranging from inkjet printing to agricultural sprays. Finally, we have meticulously documented our setup and procedure for future reference.

physics.flu-dyn↗

arXiv2025

A Diffuse-Interface Marangoni Instability

We investigate a novel Marangoni-induced instability that arises exclusively in diffuse fluid interfaces, absent in classical sharp-interface models. Using a validated phase-field Navier-Stokes-Allen-Cahn framework, we linearize the governing equations to analyze the onset and development of interfacial instability driven by solute-induced surface tension gradients. A critical interfacial thickness scaling inversely with the Marangoni number, $\delta_\mathrm{cr} \sim Ma^{-1}$, emerges from the balance between advective and diffusive transport. Unlike sharp-interface scenarios where matched viscosity and diffusivity stabilize the interface, finite thickness induces asymmetric solute distributions and tangential velocity shifts that destabilize the system. We identify universal power-law scalings of velocity and concentration offsets with a modified Marangoni number $Ma^\delta$, independent of capillary number and interfacial mobility. A critical crossover at $Ma^\delta \approx 590$ distinguishes diffusion-dominated stabilization from advection-driven destabilization. These findings highlight the importance of diffuse-interface effects in multiphase flows, with implications for miscible fluids, soft matter, and microfluidics where interfacial thickness and coupled transport phenomena are non-negligible.

physics.flu-dyn↗

arXiv2025

Skin formation in evaporating colloidal droplets

When a droplet containing a concentrated suspension evaporates in a dry environment, a layer often forms at the interface accumulating non-volatile material. Such a "skin layer" experiences strong stresses and eventually turns mechanically unstable at the last stage of evaporation. Predicting the formation of such skin layer or particle shell and its properties is a crucial problem for applications and constitutes a multi-scale problem, from the micro/nanoscopic scale of the particles to the millimetric size of the droplets. Interestingly, its physical description lies at the interface between deterministic macroscopic evaporation models and microscopic stochastic particles interactions and diffusion. In this work we present a general theoretical approach to obtain the time-dependent particle concentration profile in an implicit manner, for the general case of diffusion-limited evaporation of spherical droplets, and more generally to all 1D non linear diffusion-limited cases with particles pressure and mobility terms of rational form. This approach is compared successfully to numerical solutions obtained using a finite element solver in the limit of high P\'eclet numbers, and to 2D Brownian dynamics simulations. Our results show that the concentration profiles and shell formation onset depend nontrivially on the initial packing fraction. By analyzing these profiles, we determine the position where the glassy layer forms, whose formation is expected to play a critical role in shell buckling. This model provides a robust framework for predicting the size and maximum aspect ratio of the resulting clusters.

physics.flu-dyn↗

arXiv2024

Marangoni flow driven hysteresis and azimuthal symmetry breaking in evaporating binary droplets

The non-uniform evaporation rate at the liquid-gas interface of binary droplets induces solutal Marangoni flows. In glycerol-water mixtures (positive Marangoni number, where the more volatile fluid has higher surface tension), these flows stabilise into steady patterns. Conversely, in water-ethanol mixtures (negative Marangoni number, where the less volatile fluid has higher surface tension), Marangoni instabilities emerge, producing seemingly chaotic flows. This behaviour arises from the opposing signs of the Marangoni number. Perturbations locally reducing surface tension at the interface drive Marangoni flows away from the perturbed region. Incompressibility enforces a return flow, drawing fluid from the bulk towards the interface. In mixtures with a negative Marangoni number, preferential evaporation of the lower-surface-tension component leads to a higher concentration of the higher-surface-tension component at the interface as compared to the bulk. The return flow therefore creates a positive feedback loop, further reducing surface tension and enhancing the instability. We investigate bistable quasi-stationary solutions in evaporating binary droplets with negative Marangoni numbers and we examine symmetry breaking across a range of Marangoni number and contact angles. Remarkably, droplets with low contact angle show instabilities at lower critical Marangoni numbers than droplets with larger contact angles. Our numerical simulations reveal that interactions between droplet height profiles and non-uniform evaporation rates trigger azimuthal Marangoni instabilities in flat droplets. This geometrically confined instability can even destabilise mixtures with positive Marangoni numbers, particularly for concave liquid-gas interfaces. Finally, through Lyapunov exponent analysis, we confirm the chaotic nature of flows in droplets with a negative Marangoni number.

physics.flu-dyn↗

arXiv2024

Evaporating sessile droplets: solutal Marangoni effects overwhelm thermal Marangoni flow

When an evaporating water droplet is deposited on a thermally conductive substrate, the minimum temperature will be at the apex due to evaporative cooling. Consequently, density and surface tension gradients emerge within the droplet and at the droplet-gas interface, giving rise to competing flows from, respectively, the apex towards the contact line (thermal-buoyancy-driven flow) and the other way around (thermal Marangoni flow). In small droplets with a diameter below the capillary length, the thermal Marangoni effects are expected to dominate over thermal buoyancy ("thermal Rayleigh") effects. However, contrary to these theoretical predictions, our experiments mostly show a dominant circulation from the apex towards the contact line, indicating a prevailing of thermal Rayleigh convection. Furthermore, our experiments often show an unexpected asymmetric flow that persisted for several minutes. We hypothesise that a tiny amount of contaminants, commonly encountered in experiments with water/air interfaces, act as surfactants and counteract the thermal surface tension gradients at the interface and thereby promote the dominance of Rayleigh convection. Our finite element numerical simulations demonstrate that, under our specified experimental conditions, a mere 0.5% reduction in the static surface tension caused by surfactants leads to a reversal in the flow direction, compared to the theoretical prediction without contaminants. Additionally, we investigate the linear stability of the axisymmetric solutions, revealing that the presence of surfactants also affects the axial symmetry of the flow.

physics.flu-dyn↗

arXiv2024

Symmetry Breaking in Chemical Systems: Engineering Complexity through Self-Organization and Marangoni Flows

Far from equilibrium, chemical and biological systems can form complex patterns and waves through reaction-diffusion coupling. Fluid motion often interferes with these self-organized concentration patterns. In this study, we investigate the influence of Marangoni-driven flows inside a thin layer of fluid ascending the outer surfaces of hydrophilic obstacles on the spatio-temporal dynamics of chemical waves in the modified Belousov-Zhabotinsky reaction. Our observations reveal that circular waves originate nearly simultaneously at the obstacles and propagate outward. In a covered setup, where evaporation is minimal, the wavefronts maintain their circular shape. However, in an uncovered setup with significant evaporation and resulting Marangoni flows, the interplay between surface tension-driven Marangoni flows and gravity destabilizes the wavefronts, creating distinctive flower-like patterns around the obstacles. Our analysis shows that here solutal Marangoni forces are more relevant than thermal ones. Our experiments further show that the number of petals formed increases linearly with the obstacle's diameter, though a minimum diameter is required for these instabilities to appear. These findings demonstrate the potential to 'engineer' specific wave patterns, offering a method to control and direct reaction dynamics. This capability is especially important for developing microfluidic devices requiring precise control over chemical wave propagation.

physics.flu-dyn↗

arXiv2024

Role of surfactants on droplet formation in piezoacoustic inkjet printing across microsecond-to-second timescales

In piezo acoustic drop-on-demand inkjet printing a single droplet is produced for each piezo driving pulse. This droplet is typically multicomponent, including surfactants to control the spreading and drying of the droplet on the substrate. However, the role of these surfactants on the droplet formation process remains rather elusive. Surfactant concentration gradients may manifest across microsecond-to-second timescales, spanning both the rapid ejection of ink from the nozzle exit and the comparatively slower idling timescale governing the firing of successive droplets. In the present work, we study the influence of surfactants on droplet formation across 6 orders of magnitude in time. To this end, we visualize the microsecond droplet formation process using stroboscopic laser-induced fluorescence microscopy while we vary the nozzle idle time. Our results show that increasing the idle time up to O(1) s affects only the break-up dynamics of the inkjet but not its velocity. By contrast, for idle times $>$ O(1) s, both the break-up dynamics are altered and the velocity of the inkjet increases. We show that the increased velocity results from a decreased surface tension of the ejected droplet, which we extracted from the observed shape oscillations of the jetted droplets in flight. The measured decrease in surface tension is surprising as the $\mu$s timescale of droplet formation is much faster than the typical ms-to-s timescale of surfactant adsorption. By varying the bulk surfactant concentration, we show that the fast decrease in surface tension results from a local surfactant concentration increase to more than 200 times the CMC. Our results suggest that a local high concentration of surfactant allows for surfactant adsorption to the interface of an inkjet at the $\mu$s-to-ms timescale, which is much faster than the typical ms-to-s timescale of surfactant adsorption.

physics.flu-dyn↗

arXiv2024

Deforming ice with drops

A uniform solidification front undergoes non-trivial deformations when encountering an insoluble dispersed particle in a melt. For solid particles, the overall deformation characteristics are primarily dictated by heat transfer between the particle and the surroundings, remaining unaffected by the rate of approach of the solidification front. In this Letter, we show that, conversely, when interacting with a droplet or a bubble, the deformation behaviour exhibits entirely different and unexpected behaviour. It arises from an interfacial dynamics which is specific to particles with free interfaces, namely thermal Marangoni forces. Our study employs a combination of experiments, theory, and numerical simulations to investigate the interaction between the droplet and the freezing front and unveils its surprising behaviour. In particular, we quantitatively understand the dependence of the front deformation $Δ$ on the front propagation velocity, which, for large front velocities, can even revert from attraction ($Δ< 0$) to repulsion ($Δ> 0$).

physics.flu-dyn↗

arXiv2024

Non-monotonic surface tension leads to spontaneous symmetry breaking in a binary evaporating drop

The evaporation of water/1,2-hexanediol binary drops shows remarkable segregation dynamics, with hexanediol-rich spots forming at the rim, thus breaking axisymmetry. While the segregation of hexanediol near the rim can be attributed to the preferential evaporation of water, the symmetry-breaking and spot formation could not yet be successfully explained. With three-dimensional simulations and azimuthal stability analysis of a minimal model, we investigate the flow and composition in the drop. We show that a slightly non-monotonic surface tension causes the emergence of a counter-rotating Marangoni vortex in the hexanediol-rich rim region, which subsequently becomes azimuthally unstable and forms the observed spots. Accurate measurements with several different methods reveal that the surface tension is indeed non-monotonic. This work provides valuable insight for applications like inkjet printing or spray cooling.

physics.flu-dyn↗

arXiv2024

Evaporation of acoustically levitated bicomponent droplets: mass and heat transfer characteristics

Evaporation of multicomponent droplets is important in a wide range of applications, albeit complex, and requires a careful investigation. We experimentally and numerically investigate the evaporation characteristics of spherical, ethanol-water droplets with different initial concentration ratios in the acoustic levitation field. Imaging techniques and infrared thermometry are used for acquiring volume and surface temperature variations of droplets, reflecting their mass and heat transfer characteristics. Numerical simulations are conducted using modified parameters based on a theoretical model to consider the effect of the acoustic field. The calculation results show good agreement with the experimental data. The concentration and temperature distribution within the droplet is further investigated based on the numerical results.

physics.flu-dyn↗

arXiv2024

Enhanced bubble growth near an advancing solidification front

Frozen water might appear opaque since gas bubbles can get trapped in the ice during the freezing process. They nucleate and then grow near the advancing solidification front, due to the formation of a gas supersaturation region in its vicinity. A delicate interplay between the rate of mass transfer and the rate of freezing dictates the final shapes and sizes of the entrapped gas bubbles. In this work, we experimentally and numerically investigate the initial growth of such gas bubbles that nucleate and grow near the advancing ice front. We show that the initial growth of these bubbles is governed by diffusion and is enhanced due to a combination of the presence of the background gas concentration gradient and the motion of the approaching front. Additionally, we recast the problem into that of mass transfer to a moving spherical object in a homogeneous concentration field, finding good agreement between our experimental data and the existing scaling relations for that latter problem. Lastly, we address how fluid flow around the bubble might further affect this growth and qualitatively explore this through numerical simulations.

physics.flu-dyn↗

arXiv2023

Bifurcation tracking on moving meshes and with consideration of azimuthal symmetry breaking instabilities

We present a black-box method to numerically investigate the linear stability of arbitrary multi-physics problems. While the user just has to enter the system's residual in weak formulation, i.e. by a finite element method, all required discretized matrices are automatically assembled based on just-in-time generated and compiled highly performant C code. Based on this method, entire phase diagrams in the parameter space can be obtained by bifurcation tracking and continuation within minutes. Particular focus is put on problems with moving domains, e.g. free surface problems in fluid dynamics, since a moving mesh introduces a plethora of complicated nonlinearities to the system. By symbolic differentiation before the code generation, however, these moving mesh problems are made accessible to bifurcation tracking methods. In a second step, our method is generalized to investigate symmetry-breaking instabilities of axisymmetric stationary solutions by effectively utilizing the symmetry of the base state. Each bifurcation type is validated on the basis of results reported in the literature on versatile fluid dynamics problems.

physics.comp-ph↗

arXiv2023

Evaporation of binary liquids from a capillary tube

Evaporation of multi-component liquid mixtures in confined geometries, such as capillaries, is crucial in applications such as microfluidics, two-phase cooling devices, and inkjet printing. Predicting the behaviour of such systems becomes challenging because evaporation triggers complex spatio-temporal changes in the composition of the mixture. These changes in composition, in turn, affect evaporation. In the present work, we study the evaporation of aqueous glycerol solutions contained as a liquid column in a capillary tube. Experiments and direct numerical simulations show three evaporation regimes characterised by different temporal evolutions of the normalised mass transfer rate (or Sherwood number, $Sh$), namely $Sh (\tilde{t}) = 1$, $Sh \sim 1/\sqrt{\tilde{t}}$, and $Sh \sim \exp\left(-\tilde{t}\right)$. Here $\tilde{t}$ is a normalised time. We present a simplistic analytical model which shows that the evaporation dynamics can be expressed by the classical relation $Sh = \exp \left( \tilde{t} \right) \mathrm{erfc} \left( \sqrt{\tilde{t}}\right)$. For small and medium $\tilde{t}$, this expression results in the first and second of the three observed scaling regimes, respectively. This analytical model is formulated in the limit of pure diffusion and when the penetration depth $δ(t)$ of the diffusion front is much smaller than the length $L(t)$ of the liquid column. When $δ\approx L$, finite length effects lead to $Sh \sim \exp\left(-\tilde{t}\right)$, i.e. the third regime. Finally, we extend our analytical model to incorporate the effect of advection and determine the conditions under which this effect is important. Our results provide fundamental insight into the physics of selective evaporation from a multi-component liquid column.

physics.flu-dyn↗

arXiv2023

On the rising and sinking motion of bouncing oil drops in strongly stratified liquids

When an immiscible oil drop is immersed in a stably stratified ethanol-water mixture, the Marangoni flow on the surface of the drop can experience an oscillatory instability, so that the drop undergoes a transition from levitating to bouncing. The onset of the instability and its mechanisms have been studied previously, yet the bouncing motion of the drop itself, which is a completely different problem, has not yet been investigated. Here we study how the bouncing characteristics (jumping height, rising and sinking time) depend on the control parameters (drop radius, stratification strength, drop viscosity). We first record experimentally the bouncing trajectories of drops of different viscosities in different stratifications. Then a simplified dynamical analysis is performed to get the scaling relations of the jumping height and the rising and sinking times. The rising and sinking time scales are found to depend on the drag coefficient of the drop $C_D^S$ in the stratified liquid, which is determined empirically for the current parameter space. For low viscosity (5 cSt) oil drops the results on the drag coefficient match the ones from the literature. For high viscosity (100 cSt) oil drops the parameter space had not been explored and the drag coefficients are not readily available. Numerical simulations are therefore performed to provide external verification for the drag coefficients, which well match with the experimental results.

physics.flu-dyn↗

arXiv2023

Selective evaporation at the nozzle exit in piezoacoustic inkjet printing

In practical applications of inkjet printing the nozzles in a printhead have intermittent idle periods, during which ink can evaporate from the nozzle exit. Inks are usually multicomponent where each component has its own characteristic evaporation rate resulting in concentration gradients within the ink. These gradients may directly and indirectly (via Marangoni flows) alter the jetting process and thereby its reproducibility and the resulting print quality. In the present work, we study selective evaporation from an inkjet nozzle for water-glycerol mixtures. Through experiments, analytical modeling, and numerical simulations, we investigate changes in mixture composition with drying time. By monitoring the acoustics within the printhead, and subsequently modeling the system as a mass-spring-damper system, the composition of the mixture can be obtained as a function of drying time. The results from the analytical model are validated using numerical simulations of the full fluid mechanical equations governing the printhead flows and pressure fields. Furthermore, the numerical simulations reveal that the time independent concentration gradient we observe in the experiments is due to the steady state of water flux through the printhead. Finally, we measure the number of drop formation events required in this system before the mixture concentration within the nozzle attains the initial (pre-drying) value, and find a stronger than exponential trend in the number of drop formations required. These results shed light on the complex physiochemical hydrodynamics associated with the drying of ink at a printhead nozzle, and help in increasing the stability and reproducibility of inkjet printing.

physics.flu-dyn↗