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The effect of confining walls on the fluctuation of a nanoscale thin film's free surface is studied using stochastic thin-film equations (STFEs). Two canonical boundary conditions are employed to reveal the influence of the confinement: (1) an imposed contact angle and (2) a pinned contact line. A linear stability analysis provides the wave eigenmodes, after which thermal-capillary-wave theory predicts the wave fluctuation amplitudes. Molecular dynamics (MD) simulations are performed to test the predictions, and a Langevin diffusion model is proposed to capture oscillations of the contact lines observed in MD simulations. Good agreement between the theoretical predictions and the MD simulation results is recovered, and it is discovered that confinement can influence the entire film. Notably, a constraint on the length scale of wave modes is found to affect fluctuation amplitudes from our theoretical model, especially for 3D films. This opens up challenges and future lines of inquiry.

The relaxation dynamics of thermal capillary waves for nanoscale liquid films on anisotropic-slip substrates are investigated using both molecular dynamics (MD) simulations and a Langevin model. The anisotropy of slip on substrates is achieved using a specific lattice plane of a face-centered cubic lattice. This surface’s anisotropy breaks the simple scalar proportionality between slip velocity and wall shear stress and requires the introduction of a slip-coefficient tensor. The Langevin equation can describe both the growth of capillary wave spectra and the relaxation of capillary wave correlations, with the former providing a time scale for the surface to reach thermal equilibrium. Temporal correlations of interfacial Fourier modes, measured at thermal equilibrium in MD, demonstrate that (i) larger slip lengths lead to a faster decay in wave correlations and (ii) unlike isotropic-slip substrates, the time correlations of waves on anisotropic-slip substrates are wave-direction-dependent. These findings emerge naturally from the proposed Langevin equation, which becomes wave-direction-dependent, agrees well with MD results, and allows us to produce experimentally verifiable predictions.\ud \ud

In immiscible liquid–liquid Newtonian flow through a porous medium, one phase often becomes trapped in corners or narrow regions by capillary forces as blobs (e.g. oil ganglia) deep within the matrix, whilst the second flow exhibits a steady and laminar flow (e.g. of water) that has negligible influence on the trapped liquid–liquid interfaces. However, recent microfluidic experiments have shown the situation radically changes when using a viscoelastic liquid, which is capable of exhibiting pore-scale unsteady flow that can deform such interfaces. Here, a computational model is developed which allows us to capture the forces that cause this behaviour and provide a framework for future investigations of this system. In this paper, the forces on trapped interfaces are investigated for the first time. Notably, when the viscoelastic flow becomes unsteady the forces on the trapped interfaces not only fluctuate but also become amplified, thus supporting experimental findings showing they can be used to free such interfaces. At Weissenberg values of 1.5 and above the fluctuations become important and the mean values of the forces on the interfaces decrease as the fluctuations grow.

The Leidenfrost effect, where a drop levitates on a vapour film above a hot solid, is simulated using an efficient computational model that captures the internal flow within the droplet, models the vapour flow in a lubrication framework and is capable of resolving the dynamics of the process. The initial focus is on quasi-static droplets and the associated geometry of the vapour film formed beneath the drop, where we are able to compare with experimental analyses and assess the range of validity of the theoretical model developed in Sobac et al. (Phys. Rev. E, vol. 103, 2021, 039901). The computational model also allows us to explore parameter space, varying both the drop size and viscosity of the liquid, with computational results in excellent agreement with the theoretical model for high-viscosity liquids. Interestingly, for large water drops, discrepancies between the computational model and experiments occur, and possible reasons for this observation are provided. Our predictions reveal features including a regime with a dimpleless bottom surface of the drop and a minimum in the vapour layer thickness as a function of the drop size. Finally, the capability to simulate dynamics is revealed by computations that predict and track the vapour ‘chimney’ instability for large drops.

Thin-film-based nanoporous membrane technologies exploit evaporation to efficiently cool microscale and nanoscale electronic devices. At these scales, when domain sizes become comparable to the mean free path in the vapour, traditional macroscopic approaches such as the Navier-Stokes-Fourier (NSF) equations become less accurate, and the use of higher-order moment methods is called for. Two higher-order moment equations are considered; the linearised versions of the Grad 13 and Regularised 13 equations. These are applied to the problem of nanoporous evaporation, and results are compared to the NSF method and the method of direct simulation Monte Carlo (i.e. solutions to the Boltzmann equations). Linear and non-linear versions of the boundary conditions are examined, with the latter providing improved results, at little additional computational expense, compared to the linear form. The outcome is a simultaneously accurate and computationally efficient method, which can provide simulation-for-design capabilities at the nanoscale.\ud \ud

The effects of thermal fluctuations on nanoscale flows are captured by a numerical scheme that is underpinned by fluctuating hydrodynamics. A stochastic lubrication equation (SLE) is solved on non-uniform adaptive grids to study a series of nanoscale thin-film flows. The Fornberg scheme is used for high-resolution spatial discretisation and a fully-implicit time-marching scheme is designed for numerical stability. The accuracy of the numerical method is verified against theoretical results for thermal capillary waves during the linear stage of their development. The framework is then used to study the nonlinear behaviour of three bounded thin-film flows: (i) droplet spreading, where new power laws are derived; (ii) droplet coalescence, where molecular dynamics results are reproduced by the SLE at a fraction of the computational cost and it is discovered that thermal fluctuations decelerate the process, in contrast to previously investigated phenomena; and (iii) thin-film rupture, where, in the regime considered, disjoining pressure dominates the final stages of rupture.

The formation of deformed liquid marbles via impact of drops onto powder beds is analyzed using experimental and computational modeling approaches. Experimentally, particular attention is paid to determining a relationship between the maximum contact area of the spreading drops, which determines how much powder the drop's surface is able to harvest, and the drop's surface area when the powder (potentially) encapsulates and then immobilises (“freezes”) the surface of the drop to form a liquid marble. Comparisons between impacts on powder beds to those on rigid and impermeable superhydrophobic substrates show good agreement for a range of parameters and motivate the development of the first mathematical model for the process of liquid marble formation via drop impact. The model utilizes experimentally determined functions to capture encapsulation and freezing thresholds and accounts for the powder's influence on the drop via a surface viscous mechanism. Simulations in the volume-of-fluid framework qualitatively recover many features of the experiments and highlight physical effects that should be incorporated into future analyses.

In this paper we compute the linear stability of similarity solutions of the breakup of viscous liquid threads, in which the viscosity and inertia of the liquid are in balance with the surface tension. The stability of the similarity solution is determined using numerical continuation to find the dominant eigenvalues. Stability of the first two solutions (those with largest minimum radius) is considered. We find that the first similarity solution, which is the one seen in experiments and simulations, is linearly stable with a complex nontrivial eigenvalue, which could explain the phenomenon of break-up producing sequences of small satellite droplets of decreasing radius near a main pinch-off point. The second solution is seen to be linearly unstable. These linear stability results compare favorably to numerical simulations for the stable similarity solution, while a profile starting near the unstable similarity solution is shown to very rapidly leave the linear regime., 14 pages, 8 figures. Accepted version

Classical continuum-based liquid–vapour phase-change models typically assume continuity of temperature at phase interfaces along with a relation which describes the rate of evaporation at the interface (Hertz–Knudsen–Schrage, for example). However, for phase-transition processes at small scales, such as the evaporation of nanodroplets, the assumption that the temperature is continuous across the liquid–vapour interface leads to significant inaccuracies (McGaughey et al., J. Appl. Phys., vol. 91, issue 10, pp. 6406–6415; Rana et al., Phys. Rev. Lett., vol. 123, 154501), as might the adoption of classical constitutive relations that lead to the Navier–Stokes–Fourier (NSF) equations. In this paper, to capture the notable effects of rarefaction at small scales, we adopt an extended continuum-based approach utilising the coupled constitutive relations (CCRs). In CCR theory, additional terms are invoked in the constitutive relations of the NSF equations originating from the arguments of irreversible thermodynamics as well as being consistent with the kinetic theory of gases. The modelling approach allows us to derive new fundamental solutions for the linearised CCR model, to develop a numerical framework based upon the method of fundamental solutions (MFS) and enables three-dimensional multiphase micro-flow simulations to be performed at remarkably low computational cost. The new framework is benchmarked against classical results and then explored as an efficient tool for solving three-dimensional phase-change events involving droplets.

The well-known thermal capillary wave theory, which describes the capillary spectrum of the free surface of a liquid film, does not reveal the transient dynamics of surface waves, e.g. the process through which a smooth surface becomes rough. Here, a Langevin model is proposed that can capture this dynamics, goes beyond the long-wave paradigm which can be inaccurate at the nanoscale, and is validated using molecular dynamics simulations for nanoscale films on both planar and cylindrical substrates. We show that a scaling relation exists for surface roughening of a planar film and the scaling exponents belong to a specific universality class. The capillary spectra of planar films are found to advance towards a static spectrum, with the roughness of the surface $W$ increasing as a power law of time $W\sim t^{1/8}$ before saturation. However, the spectra of an annular film (with outer radius $h_0$ ) are unbounded for dimensionless wavenumber $qh_0 due to the Rayleigh–Plateau instability.

We develop a novel boundary integral formulation for the steady linearized form of Grad's 13-moment (G13) equations applied to a uniform flow of rarefied gas past solid objects at low Mach numbers. Changing variables leads to a system of boundary integral equations that combines integral equations from Stokes flow and potential theory. The strong coupling between the stress deviator and heat flux featured by the G13 equations demands adding a boundary integral equation for the pressure. We specialize the integral equations for an axisymmetric flow with no swirl and derive the axisymmetric fundamental solutions for the pressure equation, seemingly absent in the Stokes-flow literature. Using the boundary element method to achieve a numerical solution, we apply this formulation to streaming flow of rarefied gas past prolate or oblate spheroids with their axis of symmetry parallel to the free stream, considering various aspect ratios and Knudsen numbers—the ratio of the molecules' mean free path to the macroscopic length scale. After validating the method, we obtain the surface profiles of the deviations from the unperturbed state of the traction, heat flux, pressure, temperature, and slip velocity, as well as the drag on the spheroid, observing convergence with the number of elements. Rarefaction phenomena, such as temperature jump and polarization, Knudsen effects in the drag, and velocity slippage, are predicted. This method opens a new path for investigating other gas non-equilibrium phenomena that can be modeled by the same set of equations, such as thermophoresis, and has application in nano- and microfluidics.

Determining physically admissible boundary conditions for higher moments in an extended continuum model is recognised as a major obstacle. Boundary conditions for the regularised 26-moment (R26) equations obtained using Maxwell's accommodation model do exist in the literature; however, we show in this article that these boundary conditions violate the second law of thermodynamics and the Onsager reciprocity relations for certain boundary value problems, and, hence, are not physically admissible. We further prove that the linearised R26 (LR26) equations possess a proper $H$-theorem (second-law inequality) by determining a quadratic form without cross-product terms for the entropy density. The establishment of the $H$-theorem for the LR26 equations in turn leads to a complete set of boundary conditions that are physically admissible for all processes and comply with the Onsager reciprocity relations. As an application, the problem of a slow rarefied gas flow past a spherical droplet with and without evaporation is considered and solved analytically. The results are compared with the numerical solution of the linearised Boltzmann equation, experimental results from the literature and/or other macroscopic theories to show that the LR26 theory with the physically admissible boundary conditions provides an excellent prediction up to Knudsen number $\,\lesssim 1$ and, consequently, provides transpicuous insights into intriguing effects, such as thermal polarisation. In particular, the analytic results for the drag force obtained in the present work are in an excellent agreement with experimental results even for very large values of the Knudsen number., Comment: 40 pages, 12 figures

The combined effects of thermal fluctuations and liquid-solid slip on nanoscale thin-film flows are investigated using stochastic lubrication equations (SLEs). The previous no-slip SLE for films on plates is extended to consider slip effects and a new SLE for films on fibers is derived, using a long-wave approximation to fluctuating hydrodynamics. Analytically derived capillary spectra, which evolve in time, are found from the new SLEs and compared to molecular dynamics simulations. It is shown that thermal fluctuations lead to the generation and growth of surface waves, and slip accelerates this growth. SLEs developed here provide useful tools to study nanoscale film dewetting, nanofiber coating, and liquid transport using nanofibers.

Numerical solutions of the Enskog-Vlasov (EV) equation are used to determine the velocity distribution function of atoms spontaneously evaporating into near-vacuum conditions. It is found that an accurate approximation is provided by a half-Maxwellian including a drift velocity combined with different characteristic temperatures for the velocity components normal and parallel to the liquid-vapor interface. The drift velocity and the temperature anisotropy reduce as the liquid bulk temperature decreases but persist for relatively low temperatures corresponding to a vapor behaviour which is only slightly non-ideal. Deviations from the undrifted isotropic half-Maxwellian are shown to be consequences of collisions in the liquid-vapor interface which preferentially backscatter atoms with lower normal-velocity component., Comment: 28 pages, 9 figures

Most of our understanding of moving contact lines relies on the limit of small capillary number Ca . This means the contact line speed is small compared to the capillary speed γ/η , where γ is the surface tension and η the viscosity, so that the interface is only weakly curved. The majority of recent analytical work has assumed in addition that the angle between the free surface and the substrate is also small, so that lubrication theory can be used. Here, we calculate the shape of the interface near a slip surface for arbitrary angles, and for two phases of arbitrary viscosities, thereby removing a key restriction in being able to apply small capillary number theory. Comparing with full numerical simulations of the viscous flow equation, we show that the resulting theory provides an accurate description up to Ca≈0.1 in the dip coating geometry, and a major improvement over theories proposed previously.

Next-generation processor-chip cooling devices and self-cleaning surfaces can be enhanced by a passive process that require little to no electrical input, through coalescence-induced nanodroplet jumping. Here, we describe the crucial impact thermal capillary waves and ambient gas rarefaction have on enhancing/limiting the jumping speeds of nanodroplets on low adhesion surfaces. By using high-fidelity non-equilibrium molecular dynamics simulations in conjunction with well-resolved volume-of-fluid continuum calculations, we are able to quantify the different dissipation mechanisms that govern nanodroplet jumping at length scales that are currently difficult to access experimentally. We find that interfacial thermal capillary waves contribute to a large statistical spread of nanodroplet jumping speeds that range from 0 - 30 m/s, where the typical jumping speeds of micro/millimeter sized droplets are only up to a few m/s. As the gas surrounding these liquid droplets is no longer in thermodynamic equilibrium, we also show how the reduced external drag leads to increased jumping speeds. This work demonstrates that, in the viscous-dominated regime, the Ohnesorge number and viscosity ratio between the two phases alone are not sufficient, but that the thermal fluctuation number (Th) and the Knudsen Number (Kn) are both needed to recover the relevant molecular physics at nanoscales. Our results and analysis suggest that these dimensionless parameters would be relevant for many other free-surface flow processes and applications that operate at the nanoscale.\ud \ud

We study air entrainment by a solid plate plunging into a viscous liquid, theoretically and numerically. At dimensionless speeds $Ca=U\unicode[STIX]{x1D702}/\unicode[STIX]{x1D6FE}$ of order unity, a near-cusp forms due to the presence of a moving contact line. The radius of curvature of the cusp’s tip scales with the slip length multiplied by an exponential of $-Ca$. The pressure from the air flow drawn inside the cusp leads to a bifurcation, at which air is entrained, i.e. there is ‘wetting failure’. We develop an analytical theory of the threshold to air entrainment, which predicts the critical capillary number to depend logarithmically on the viscosity ratio, with corrections coming from the slip in the gas phase.

The instability and rupture of nanoscale liquid threads is shown to strongly depend on thermal fluctuations. These fluctuations are naturally occurring within molecular dynamics (MD) simulations and can be incorporated via fluctuating hydrodynamics into a stochastic lubrication equation (SLE). A simple and robust numerical scheme is developed for the SLE that is validated against MD for both the initial (linear) instability and the nonlinear rupture process. Particular attention is paid to the rupture process and its statistics, where the `double-cone’ profile reported by Moseler & Landmann [Science, 2000, 289(5482): 1165-1169] is observed, as well as other distinct profile forms depending on the flow conditions. Comparison to the Eggers’ similarity solution [Physical Review Letters, 2002, 89(8): 084502], a power law of the minimum thread radius against time to rupture, shows agreement only at low surface tension; indicating that surface tension cannot generally be neglected when considering rupture dynamics.\ud \ud

A model is developed for liquid drop impact on a solid surface that captures the thin film gas flow beneath the drop, even when the film's thickness is below the mean free path in the gas so that gas kinetic effects (GKE) are important. Simulation results agree with experiments, with the impact speed threshold between bouncing and wetting reproduced to within 5%, while a model without GKE overpredicts this value by at least 50%. To isolate GKE, the pressure dependence of the threshold is mapped and provides experimentally verifiable predictions. There are two principal modes of contact leading to wetting and both are associated with a van der Waals driven instability of the film.

A transition from a ${d}^{2}$ to a $d$ law is observed in molecular dynamics (MD) simulations when the diameter ($d$) of an evaporating droplet reduces to the order of the vapor's mean free path; this cannot be explained by classical theory. This Letter shows that the $d$ law can be predicted within the Navier-Stokes-Fourier (NSF) paradigm if a temperature-jump boundary condition derived from kinetic theory is utilized. The results from this model agree with those from MD in terms of the total lifetime, droplet radius, and temperature, while the classical ${d}^{2}$ law underpredicts the lifetime of the droplet by a factor of 2. Theories beyond NSF are also employed in order to investigate vapor rarefaction effects within the Knudsen layer adjacent to the interface.

We consider the linearized form of the regularized 13-moment equations (R13) to model the slow, steady gas dynamics surrounding a rigid, heat-conducting sphere when a uniform temperature gradient is imposed far from the sphere and the gas is in a state of rarefaction. Under these conditions, the phenomenon of thermophoresis, characterized by forces on the solid surfaces, occurs. The R13 equations, derived from the Boltzmann equation using the moment method, provide closure to the mass, momentum and energy conservation laws in the form of constitutive, transport equations for the stress and heat flux that extend the Navier–Stokes–Fourier model to include non-equilibrium effects. We obtain analytical solutions for the field variables that characterize the gas dynamics and a closed-form expression for the thermophoretic force on the sphere. We also consider the slow, streaming flow of gas past a sphere using the same model resulting in a drag force on the body. The thermophoretic velocity of the sphere is then determined from the balance between thermophoretic force and drag. The thermophoretic force is compared with predictions from other theories, including Grad’s 13-moment equations (G13), variants of the Boltzmann equation commonly used in kinetic theory, and with recently published experimental data. The new results from R13 agree well with results from kinetic theory up to a Knudsen number (based on the sphere’s radius) of approximately 0.1 for the values of solid-to-gas heat conductivity ratios considered. However, in this range of Knudsen numbers, where for a very high thermal conductivity of the solid the experiments show reversed thermophoretic forces, the R13 solution, which does result in a reversal of the force, as well as the other theories predict significantly smaller forces than the experimental values. For Knudsen numbers between 0.1 and 1 approximately, the R13 model of thermophoretic force qualitatively shows the trend exhibited by the measurements and, among the various models considered, results in the least discrepancy.

The instability of a thin liquid film on a solid surface is studied both by molecular dynamics simulations (MD) and a stochastic thin-film equation (STF), which models thermal fluctuations with white noise. A linear stability analysis of the STF allows us to derive a power spectrum for the surface fluctuations, which is quantitatively validated against the spectrum observed in MD. Thermal fluctuations are shown to be critical to the dynamics of nanoscale films. Compared to the classical instability mechanism, which is driven by disjoining pressure, fluctuations (a) can massively amplify the instability, (b) cause the fluctuation wavelength that is dominant to evolve in time (a single fastest-growing mode does not exist), and (c) decrease the critical wavelength so that classically stable films can be ruptured.\ud \ud

The theoretical framework developed by Rayleigh and Plateau in the 19th century has been remarkably accurate in describing macroscale experiments of liquid cylinder instability. Here we re-evaluate and revise the Rayleigh–Plateau instability for the nanoscale, where molecular dynamics experiments demonstrate its inadequacy. A new framework based on the stochastic lubrication equation is developed that captures nanoscale flow features and highlights the critical role of thermal fluctuations at small scales. Remarkably, the model indicates that classically stable (i.e. ‘fat’) liquid cylinders can be broken at the nanoscale, and this is confirmed by molecular dynamics.

Thin-film evaporation from nanoporous membranes is a promising cooling technology employed for the thermal management of modern electronic devices. We propose an effective one-dimensional analytical approach that can accurately predict the temperature and density jump relations, and evaporation rates, for arbitrary nanoporous membrane configurations. This is accomplished through the specification of an effective evaporation coefficient that encompasses the influence of different system parameters, such as porosity, meniscus shape, evaporation coefficient, and receding height. Our proposed approach can accurately predict all the typical output evaporation parameters of interest like mass flux, and temperature and density jumps, without the need to carry out computationally demanding numerical simulations. Several exemplar cases comprising of nanoporous configurations with a wide range of parameters have been considered to demonstrate the feasibility and accuracy of this analytic approach. This work thus enables a quick, efficient, and accurate means of aiding the design and engineering analysis of nanoporous membrane-based cooling devices.\ud

The classical notion of the coalescence of two droplets of the same radius R is that surface tension drives an initially singular flow. In this Letter we show, using molecular dynamics simulations of coalescing water nanodroplets, that after single or multiple bridges form due to the presence of thermal capillary waves, the bridge growth commences in a thermal regime. Here, the bridges expand linearly in time much faster than the viscous-capillary speed due to collective molecular jumps near the bridge fronts. Transition to the classical hydrodynamic regime only occurs once the bridge radius exceeds a thermal length scale l_{T}∼sqrt[R].

Evaporation of a binary liquid into near vacuum conditions has been studied using numerical solutions of a system of two coupled Enskog-Vlasov equations. Liquidvapor coexistence curves have been mapped out for different liquid compositions. The evaporation process has been investigated at a range of liquid temperatures sufficiently lower than the critical one for the vapor not to significantly deviate from the ideal behaviour. It is found that the shape of the distribution functions of evaporating atoms is well approximated by an anisotropic Maxwellian distribution with different characteristic temperatures for velocity components normal and parallel to the liquid-vapor interface. The anisotropy reduces as the evaporation temperature decreases. Evaporation coefficients are computed based on the separation temperature and the maximum concentration of the less volatile component close to the liquid-vapor interface. This choice leads to values which are almost constant in the simulation conditions.

Fundamental solutions (Green’s functions) are derived for the regularised 13-moment system (R13) of rarefied gas dynamics, for small departures from equilibrium; these solutions show the presence of Knudsen layers, associated with exponential decay terms, that do not feature in the solution of lower-order systems (e.g. the Navier–Stokes–Fourier equations). Incorporation of these new fundamental solutions into a numerical framework based on the method of fundamental solutions (MFS) allows for efficient computation of three-dimensional gas microflows at remarkably low computational cost. The R13-MFS approach accurately recovers analytic solutions for low-speed flow around a stationary sphere and heat transfer from a hot sphere (for which a new analytic solution has been derived), capturing non-equilibrium flow phenomena missing from lower-order solutions. To demonstrate the potential of the new approach, the influence of kinetic effects on the hydrodynamic interaction between approaching solid microparticles is calculated. Finally, a programme of future work based on the initial steps taken in this article is outlined.

The interface formation model is applied to describe the initial stages of the coalescence of two liquid drops in the presence of a viscous ambient fluid whose dynamics is fully accounted for. Our focus is on understanding (a) how this model's predictions differ from those of the conventionally used one, (b) what influence the ambient fluid has on the evolution of the shape of the coalescing drops and (c) the coupling of the intrinsic dynamics of coalescence and that of the ambient fluid. The key feature of the interface formation model in its application to the coalescence phenomenon is that it removes the singularity inherent in the conventional model at the onset of coalescence and describes the part of the free surface `trapped' between the coalescing volumes as they are pressed against each other as a rapidly disappearing `internal interface'. Considering the simplest possible formulation of this model, we find experimentally-verifiable differences with the predictions of the conventional model showing, in particular, the effect of drop size on the coalescence process. According to the new model, for small drops a non-monotone time-dependence of the bridge expansion speed is a feature that could be looked for in further experimental studies. Finally, the results of both models are compared to recently available experimental data on the evolution of the liquid bridge connecting the coalescing drops, and the interface formation model is seen to give a better agreement with the data., Comment: Accepted for publication in the Journal of Fluid Mechanics

The maximum speed at which a liquid can wet a solid is limited by the need to displace gas lubrication films in front of the moving contact line. The characteristic height of these films is often comparable to the mean free path in the gas so that hydrodynamic models do not adequately describe the flow physics. This Letter develops a model which incorporates kinetic effects in the gas, via the Boltzmann equation, and can predict experimentally-observed increases in the maximum speed of wetting when (a) the liquid's viscosity is varied, (b) the ambient gas pressure is reduced or (c) the meniscus is confined., Comment: Accepted for publication in Physical Review Letters

We report studies of the coalescence of pairs of picolitre aerosol droplets manipulated with holographic optical tweezers, probing the shape relaxation dynamics following coalescence by simultaneously monitoring the intensity of elastic backscattered light (EBL) from the trapping laser beam (time resolution on the order of 100 ns) while recording high frame rate camera images (time resolution µs). The goals of this work are to: resolve the dynamics of droplet coalescence in holographic optical traps; assign the origin of key features in the time-dependent EBL intensity; and validate the use of the EBL alone to precisely determine droplet surface tension and viscosity. For low viscosity droplets, two sequential processes are evident: binary coalescence first results from the overlap of the optical traps on the time scale of microseconds followed by the recapture of the composite droplet in an optical trap on the time scale of milliseconds. As droplet viscosity increases, the relaxation in droplet shape eventually occurs on the same time scale as recapture, resulting in a convoluted evolution of the EBL intensity that inhibits quantitative determination of the relaxation time scale. Droplet coalescence was simulated using a computational framework to validate both experimental approaches. The results indicate that time-dependent monitoring of droplet shape from the EBL intensity allows for robust determination of properties such as surface tension and viscosity. Finally, the potential of high frame rate imaging to examine the coalescence of dissimilar viscosity droplets is discussed.

Numerical issues arising in computations of viscous flows in corners formed by a liquid-fluid free surface and a solid boundary are considered. It is shown that on the solid a Dirichlet boundary condition, which removes multivaluedness of velocity in the `moving contact-line problem' and gives rise to a logarithmic singularity of pressure, requires a certain modification of the standard finite-element method. This modification appears to be insufficient above a certain critical value of the corner angle where the numerical solution becomes mesh-dependent. As shown, this is due to an eigensolution, which exists for all angles and becomes dominant for the supercritical ones. A method of incorporating the eigensolution into the numerical method is described that makes numerical results mesh-independent again. Some implications of the unavoidable finiteness of the mesh size in practical applications of the finite element method in the context of the present problem are discussed., Submitted to the International Journal for Numerical Methods in Fluids

A new approach to the modelling of wetting fronts in porous media on the Darcy scale is developed, based on considering the types (modes) of motion the menisci go through on the pore scale. This approach is illustrated using a simple model case of imbibition of a viscous incompressible liquid into an isotropic porous matrix with two modes of motion for the menisci, the wetting mode and the threshold mode. The latter makes it necessary to introduce an essentially new technique of conjugate problems that allows one to link threshold phenomena on the pore scale with the motion on the Darcy scale. The developed approach (a) makes room for incorporating the actual physics of wetting on the pore scale, (b) brings in the physics associated with pore-scale thresholds, which determine when sections of the wetting front will be brought to a halt (pinned), and, importantly, (c) provides a regular framework for constructing models of increasing complexity.

We present results from an experimental study of the impact of liquid drops onto powder beds which are pre-wetted with the impacting liquid. Using high-speed video imaging, we study both the dynamics of the initial spreading regime and drainage times once the drop has reached its maximum spread on the surface. During the initial spreading stage, we compare our experimental data to a previously developed model which incorporates imbibition into the spreading dynamics and observe reasonable agreement. We find that the maximum spread is a strong function of the moisture content in the powder bed and that the total time from impact to complete drainage is always shorter than that for dry powder. Our results indicate that there is an optimum moisture content (or saturation) which leads to the fastest penetration. We use simple scaling arguments which also identify an optimum moisture content for fastest penetration, which agrees very well with the experimental result. © 2013 Elsevier B.V.

The finite element simulation of dynamic wetting phenomena, requiring the computation of flow in a domain confined by intersecting a liquid–fluid free surface and a liquid–solid interface, with the three-phase contact line moving across the solid, is considered. For this class of flows, different finite element method (FEM) implementations have been used in the literature, and in some cases, these produced apparently contradictory results. In the present paper, a robust framework for the FEM simulation of dynamic wetting flows is developed, which, by consistently adhering to the FEM methodology, leaves no room for ad hoc ‘optional’ variations in the numerical handling of these flows. The developed approach makes it possible to conduct a convergence study, assess the spatial resolution required to achieve a preset accuracy and provide the corresponding benchmark calculations. This analysis allows one to identify numerical artefacts, which had previously been interpreted as physical effects, and demonstrates that suppressing numerical errors using a ‘strong’ implementation of a boundary condition creates bigger and less detectable errors elsewhere in the computational domain. We provide practical recommendations on the spatial resolution required by a numerical scheme for a given set of non-dimensional similarity parameters and give a user-friendly step-by-step guide specifying the entire implementation, which allows the reader to easily reproduce all presented results including the benchmark calculations. It is also shown how the developed framework accommodates generalizations of the mathematical model accounting for additional physical effects, such as gradients in surface tensions.

Computations of the breakup of a liquid bridge are used to establish the limits of applicability of similarity solutions derived for different breakup regimes. These regimes are based on particular viscous-inertial balances, that is different limits of the Ohnesorge number $Oh$. To accurately establish the transitions between regimes, the minimum bridge radius is resolved through four orders of magnitude using a purpose-built multiscale finite element method. This allows us to construct a quantitative phase diagram for the breakup phenomenon which includes the appearance of a recently discovered low-$Oh$ viscous regime. The method used to quantify the accuracy of the similarity solutions allows us to identify a number of previously unobserved features of the breakup, most notably an oscillatory convergence towards the viscous-inertial similarity solution. Finally, we discuss how the new findings open up a number of challenges for both theoretical and experimental analysis., Comment: Accepted for publication in the Journal of Fluid Mechanics

Recent experiments on coating flows and liquid drop impact both demonstrate that wetting failures caused by air entrainment can be suppressed by reducing the ambient gas pressure. Here, it is shown that non-equilibrium effects in the gas can account for this behaviour, with ambient pressure reductions increasing the gas' mean free path and hence the Knudsen number $Kn$. These effects first manifest themselves through Maxwell slip at the gas' boundaries so that for sufficiently small $Kn$ they can be incorporated into a continuum model for dynamic wetting flows. The resulting mathematical model contains flow structures on the nano-, micro- and milli-metre scales and is implemented into a computational platform developed specifically for such multiscale phenomena. The coating flow geometry is used to show that for a fixed gas-liquid-solid system (a) the increased Maxwell slip at reduced pressures can substantially delay air entrainment, i.e. increase the `maximum speed of wetting', (b) unbounded maximum speeds are obtained as the pressure is reduced only when slip at the gas-liquid interface is allowed for and (c) the observed behaviour can be rationalised by studying the dynamics of the gas film in front of the moving contact line. A direct comparison to experimental results obtained in the dip-coating process shows that the model recovers most trends but does not accurately predict some of the high viscosity data at reduced pressures. This discrepancy occurs because the gas flow enters the `transition regime', so that more complex descriptions of its non-equilibrium nature are required. Finally, by collapsing onto a master curve experimental data obtained for drop impact in a reduced pressure gas, it is shown that the same physical mechanisms are also likely to govern splash suppression phenomena., Accepted for publication in the Journal of Fluid Mechanics

The formation of a single bubble from an orifice in a solid surface, submerged in an in- compressible, viscous Newtonian liquid, is simulated. The finite element method is used to capture the multiscale physics associated with the problem and to track the evolution of the free surface explicitly. The results are compared to a recent experimental analysis and then used to obtain the global characteristics of the process, the formation time and volume of the bubble, for a range of orifice radii; Ohnesorge numbers, which combine the material parameters of the liquid; and volumetric gas flow rates. These benchmark calculations, for the parameter space of interest, are then utilised to validate a selection of scaling laws found in the literature for two regimes of bubble formation, the regimes of low and high gas flow rates., Comment: Accepted for publication in the European Journal of Mechanics B/Fluids

Surface engineering at the nanoscale is a rapidly developing field that promises to impact a range of applications including energy production, water desalination, self-cleaning and anti-icing surfaces, thermal management of electronics, microfluidic platforms, and environmental pollution control. As the area advances, more detailed insights of dynamic wetting interactions on these surfaces are needed. In particular, the coalescence of two or more droplets on ultra-low adhesion surfaces leads to droplet jumping. Here we show, through detailed measurements of jumping droplets during water condensation coupled with numerical simulations of binary droplet coalescence, that this process is fundamentally inefficient with only a small fraction of the available excess surface energy (≲ 6%) convertible into translational kinetic energy. These findings clarify the role of internal fluid dynamics during the jumping droplet coalescence process and underpin the development of systems that can harness jumping droplets for a wide range of applications.

The coalescence of two liquid drops surrounded by a viscous gas is considered in the framework of the conventional model. The problem is solved numerically with particular attention to resolving the very initial stage of the process which only recently has become accessible both experimentally and computationally. A systematic study of the parameter space of practical interest allows the influence of the governing parameters in the system to be identified and the role of viscous gas to be determined. In particular, it is shown that the viscosity of the gas suppresses the formation of toroidal bubble predicted in some cases by early computations where the gas' dynamics was neglected. Focussing computations on the very initial stages of coalescence and considering the large parameter space allows us to examine the accuracy and limits of applicability of various `scaling laws' proposed for different `regimes' and, in doing so, reveal certain inconsistencies in recent works. A comparison to experimental data shows that the conventional model is able to reproduce many qualitative features of the initial stages of coalescence, such as a collapse of calculations onto a `master curve' but, quantitatively, overpredicts the observed speed of coalescence and there are no free parameters to improve the fit. Finally, a phase diagram of parameter space, differing from previously published ones, is used to illustrate the key findings., Comment: Accepted for publication in the Journal of Fluid Mechanics

We examine the dynamics of two coalescing liquid drops in the `inertial regime', where the effects of viscosity are negligible and the propagation of the bridge front connecting the drops can be considered as `local'. The solution fully computed in the framework of classical fluid-mechanics allows this regime to be identified and the accuracy of the approximating scaling laws proposed to describe the propagation of the bridge to be established. It is shown that the scaling law known for this regime has a very limited region of accuracy and, as a result, in describing experimental data it has frequently been applied outside its limits of applicability. The origin of the scaling law's shortcoming appears to be the fact that it accounts for the capillary pressure due only to the longitudinal curvature of the free surface as the driving force for the process. To address this deficiency, the scaling law is extended to account for both the longitudinal and azimuthal curvatures at the bridge front which, fortuitously, still results in an explicit analytic expression for the front's propagation speed. This new expression is then shown to offer an excellent approximation for both the fully-computed solution and for experimental data from a range of flow configurations for a remarkably large proportion of the coalescence process. The derived formula allows one to predict the speed at which drops coalesce for the duration of the inertial regime which should be useful for the analysis of experimental data., Accepted for publication in Physical Review E

The anomalous dynamics of capillary rise in a porous medium discovered experimentally more than a decade ago [T. Delker et al., Phys. Rev. Lett. 76, 2902 (1996)] is described. The developed theory is based on considering the principal modes of motion of the menisci that collectively form the wetting front on the Darcy scale. These modes, which include (i) dynamic wetting mode, (ii) threshold mode, and (iii) interface depinning process, are incorporated into the boundary conditions for the bulk equations formulated in the regular framework of continuum mechanics of porous media, thus allowing one to consider a general case of three-dimensional flows. The developed theory makes it possible to describe all regimes observed in the experiment, with the time spanning more than four orders of magnitude, and highlights the dominant physical mechanisms at different stages of the process.

The spreading of an incompressible viscous liquid over an isotropic homogeneous unsaturated porous substrate is considered. It is shown that, unlike the dynamic wetting of an impermeable solid substrate, where the dynamic contact angle has to be specified as a boundary condition in terms of the wetting velocity and other flow characteristics, the `effective' dynamic contact angle on an unsaturated porous substrate is completely determined by the requirement of existence of a solution, i.e. the absence of a nonintegrable singularity in the spreading fluid's pressure at the `effective' contact line. The obtained velocity dependence of the `effective' contact angle determines the critical point at which a transition to a different flow regime takes place, where the fluid above the substrate stops spreading whereas the wetting front inside it continues to propagate., Comment: Accepted for publication in the Journal of Fluid Mechanics

A mathematically challenging model of dynamic wetting as a process of interface formation has been, for the first time, fully incorporated into a numerical code based on the finite element method and applied, as a test case, to the problem of capillary rise. The motivation for this work comes from the fact that, as discovered experimentally more than a decade ago, the key variable in dynamic wetting flows -the dynamic contact angle - depends not just on the velocity of the three-phase contact line but on the entire flow field/geometry. Hence, to describe this effect, it becomes necessary to use the mathematical model that has this dependence as its integral part. A new physical effect, termed the `hydrodynamic resist to dynamic wetting', is discovered where the influence of the capillary's radius on the dynamic contact angle, and hence on the global flow, is computed. The capabilities of the numerical framework are then demonstrated by comparing the results to experiments on the unsteady capillary rise, where excellent agreement is obtained. Practical recommendations on the spatial resolution required by the numerical scheme for a given set of non-dimensional similarity parameters are provided, and a comparison to asymptotic results available in limiting cases confirms that the code is converging to the correct solution. The appendix gives a user-friendl step-by-step guide specifying the entire implementation and allowing the reader to easily reproduce all presented results, including the benchmark calculations., Comment: Minor errors in Eq 53, 63 and resulting expressions corrected which were never present in the code - i.e. all previous results remain valid and unchanged

The process of coalescence of two identical liquid drops is simulated numerically in the framework of two essentially different mathematical models, and the results are compared with experimental data on the very early stages of the coalescence process reported recently. The first model tested is the “conventional” one, where it is assumed that coalescence as the formation of a single body of fluid occurs by an instant appearance of a liquid bridge smoothly connecting the two drops, and the subsequent process is the evolution of this single body of fluid driven by capillary forces. The second model under investigation considers coalescence as a process where a section of the free surface becomes trapped between the bulk phases as the drops are pressed against each other, and it is the gradual disappearance of this “internal interface” that leads to the formation of a single body of fluid and the conventional model taking over. Using the full numerical solution of the problem in the framework of each of the two models, we show that the recently reported electrical measurements probing the very early stages of the process are better described by the interface formation/disappearance model. New theory-guided experiments are suggested that would help to further elucidate the details of the coalescence phenomenon. As a by-product of our research, the range of validity of different “scaling laws” advanced as approximate solutions to the problem formulated using the conventional model is established.\ud

We show that an attempt to compute numerically a viscous flow in a domain with a piece-wise smooth boundary by straightforwardly applying well-tested numerical algorithms (and numerical codes based on their use, such as COMSOL Multiphysics) can lead to spurious multivaluedness and nonintegrable singularities in the distribution of the fluid's pressure. The origin of this difficulty is that, near a corner formed by smooth parts of the piece-wise smooth boundary, in addition to the solution of the inhomogeneous problem, there is also an eigensolution. For obtuse corner angles this eigensolution (a) becomes dominant and (b) has a singular radial derivative of velocity at the corner. A method is developed that uses the knowledge about the eigensolution to remove multivaluedness and nonintegrability of the pressure. The method is first explained in the simple case of a Stokes flow in a corner region and then generalised for the full-scale unsteady Navier-Stokes flow in a domain with a free surface., Comment: Under consideration for publication in the Journal of Fluid Mechanics. Figure bouding box problems resolved