We study the effect of insoluble surfactants on the wave dynamics of vertically-falling liquid films. We use three-dimensional numerical simulations and employ a hybrid interface-tracking/level-set method, taking into account Marangoni stresses induced by gradients of interfacial surfactant concentration. Our numerical predictions for the evolution of the surfactant-free, three-dimensional wave topology are validated against the experimental work of Park & Nosoko (2003). The addition of surfactants is found to influence significantly the development of horseshoe-shaped waves. At low Marangoni numbers, we show that the wave fronts exhibit spanwise oscillations before eventually acquiring a quasi two-dimensional shape. In addition, the presence of Marangoni stresses are found to suppress the peaks of the travelling waves and preceding capillary wave structures. At high Marangoni numbers, a near complete rigidification of the interface is observed.
In this paper we propose several models that describe the dynamics of liquid films which are covered by a high concentration layer of insoluble surfactant. First, we briefly review the 'classical' hydrodynamic form of the coupled evolution equations for the film height and surfactant concentration that are well established for small concentrations. Then we re-formulate the basic model as a gradient dynamics based on an underlying free energy functional that accounts for wettability and capillarity. Based on this re-formulation in the framework of nonequilibrium thermodynamics, we propose exten…
Electric modification of mode competition in viscous films with insoluble surfactants on vertical fibers
School of Astronautics, Beihang University（航空航天大学，北京航空航天大学）；Aircraft and Propulsion Laboratory, Ningbo Institute of Technology, Beihang University（飞机与推进实验室，宁波理工学院，北京航空航天大学）
We have developed a multi-phase SPH method to simulate arbitrary interfaces containing surface active agents (surfactants) that locally change the properties of the interface, such the surface tension coefficient. Our method incorporates the effects of surface diffusion, transport of surfactant from/to the bulk phase to/from the interface and diffusion in the bulk phase. Neglecting transport mechanisms, we use this method to study the impact of insoluble surfactants on drop deformation and breakup in simple shear flow and present the results in a fluid dynamics video.
The spreading dynamics of surfactant molecules on a thin fluid layer is of both fundamental and practical interest. A mathematical model formulated by Gaver and Grotberg 1990 describing the spreading of a single layer of insoluble surfactant has become widely accepted, and several experiments on axisymmetric spreading have confirmed its predictions for both the height profile of the free surface and the spreading exponent (the radius of the circular area covered by surfactant grows as t^{1/4}). However, these prior experiments have primarily utilized surfactant quantities exceeding (sometimes …
In this work, we study the effect of insoluble surfactants on the three-dimensional rim-driven retraction dynamics of thin water sheets in air. We employ an interface-tracking/level-set method to ensure the full coupling between the surfactant-induced Marangoni-stresses, interfacial diffusion, and inertia. Our findings are contrasted with the (Newtonian) dynamics of a liquid sheet edge finding that the surfactant concentration can prevent, or delay, the breakup of the rim. Our simulations use the fastest growing Rayleigh-Plateau instability to drive droplet detachment from the fluid sheet (rim…
New diffuse interface and sharp interface models for soluble and insoluble surfactants fulfilling energy inequalities are introduced. We discuss their relation with the help of asymptotic analysis and present an existence result for a particular diffuse interface model.
We model the advective Marangoni spreading of insoluble surfactant at the free surface of a viscous fluid that is confined within a two-dimensional rectangular cavity. Interfacial deflections are assumed small, with contact lines pinned to the walls of the cavity, and inertia is neglected. Linearizing the surfactant transport equation about the equilibrium state allows a modal decomposition of the dynamics, with eigenvalues corresponding to decay rates of perturbations. Computation of the family of mutually orthogonal two-dimensional eigenfunctions reveals singular flow structures near each co…
We study the effect of insoluble surfactants on the spatio-temporal evolution of turbulent jets. We use three-dimensional numerical simulations and employ an interface-tracking/level-set method that accounts for surfactant-induced Marangoni stresses. The present study builds on our previous work (Constante et al., 2021, J. Fluid Mech., 922, A6) in which we examined in detail the vortex-surface interaction in the absence of surfactants. Numerical solutions are obtained for a wide range of Weber and elasticity numbers in which vorticity production is generated by surface deformation and surfacta…
A conservation-consistent boundary condition for nonlinear models of soluble-surfactant-laden falling films
Centre for Applied Sciences (CAS), International Institute of Information Technology（国际信息技术学院应用科学中心）；Universite Claude Bernard Lyon 1, LMFA, UMR5509, CNRS, Ecole Centrale de Lyon, INSA Lyon（里昂第一大学，LMFA，UMR5509，CNRS，里昂中央理工学院，里昂国立应用科学学院）；Department of Mathematics, Vivekananda Mahavidyalaya（维韦卡南达学院数学系）
We study spreading of a droplet, with insoluble surfactant covering its capillary surface, on a textured substrate. In this process, the surfactant-dependent surface tension dominates the behaviors of the whole dynamics, particularly the moving contact lines. This allows us to derive the full dynamics of the droplets laid by the insoluble surfactant: (i) the moving contact lines, (ii) the evolution of the capillary surface, (iii) the surfactant dynamics on this moving surface with a boundary condition at the contact lines and (iv) the incompressible viscous fluids inside the droplet. Our deriv…
We derive a general integrodifferential equation for the transient behaviour of small-amplitude capillary waves on the planar surface of a viscous fluid in the presence of the Marangoni effect. The equation is solved for an insoluble surfactant solution in concentration below the critical micelle concentration (cmc) undergoing convective-diffusive surface transport. The special case of a diffusion-driven surfactant is considered near the the critical damping wavelength. The Marangoni effect is shown to contribute to the overall damping mechanism and a first-order term correction to the critica…
The exact solution for a small falling drop is a classical result by Hadamard and Rybczynski. But experiments show that small drops fall slower than predicted, giving closer agreement with Stokes' result for a falling hard sphere. Increasing the drop size, a transition between these two extremes is found. This is due to surfactants present in the system, and previous work has led to the stagnant-cap model. We present here an alternative approach which we call the continuous-interface model. In contrast to the stagnant-cap model, we do not consider a surfactant advection-diffusion equation at t…
The linear instability of a surfactant-laden two-layer falling film over an inclined slippery wall is analyzed under an influence of external shear which is imposed on the top surface of the flow. The free surface of the flow as well as the interface among the fluids are contaminated by insoluble surfactants. Dynamics of both the layers are governed by the Navier--Stokes equations, and the surfactant transport equation regulates the motion of the insoluble surfactants at the interface and free surface. Instability mechanisms are compared by imposing the external shear along and opposite to the…
A thin liquid film covered with an insoluble surfactant in the vicinity of a first-order phase transition is discussed. Within the lubrication approximation we derive two coupled equations to describe the height profile of the film and the surfactant density. Thermodynamics of the surfactant is incorporated via a Cahn-Hilliard type free-energy functional which can be chosen to describe a transition between two stable phases of different surfactant density. Within this model, a linear stability analysis of stationary homogeneous solutions is performed, and drop formation in a film covered with …
The behaviour of a single sub-millimetre-size water drop falling through a viscous oil while subjected to an electric field is of fundamental importance to industrial applications such as crude oil electrocoalescers. Detailed studies, both experimental and computational, have been performed previously, but an often challenging issue has been the characterization of the fluids. As numerous authors have noted, it is very difficult to have a perfectly clean water-oil system even for very pure model oils, and the presence of trace chemicals may significantly alter the interface behaviour. In this …
We consider the spreading dynamics of some insoluble surface-active species along an aqueous interface. The model includes both diffusion, Marangoni convection and first-order reaction kinetics. An exact solution of the nonlinear transport equations is derived in the regime of large Schmidt number, where viscous effects are dominant. We demonstrate that the variance of the surfactant distribution increases linearly with time, providing an unambiguous definition for the enhanced diffusion coefficient observed in the experiments. The model thus presents new insight regarding the actuation of cam…
The surface shear viscosity of an insoluble surfactant monolayer often depends strongly on its surface pressure. Here, we show that a particle moving within a bounded monolayer breaks the kinematic reversibility of low-Reynolds-number flows. The Lorentz reciprocal theorem allows such irreversibilities to be computed without solving the full nonlinear equations, giving the leading-order contribution of surface-pressure-dependent surface viscosity. In particular, we show that a disk translating or rotating near an interfacial boundary experiences a force in the direction perpendicular to that bo…
The motion of a viscous droplet in unbounded Poiseuille flow under the combined influence of bulk-insoluble surfactant and linearly varying temperature field aligned in the direction of imposed flow is studied analytically. Neglecting fluid inertia, thermal convection and shape deformation, asymptotic analysis is performed to obtain the velocity of a force-free surfactant-laden droplet. The present study is focused on two limiting situations of surfactant transport: (i) small surface Peclet number, and (ii) high surface Peclet number. Thermocapillary-induced Marangoni stress, strength of which…
The present study theoretically predicts the effect of interfacial viscosity on the deformation of a compound drop as well as on the bulk rheology. The system at hand comprises of a dilute emulsion of concentric compound drops, laden with surfactants and suspended in a linear flow. Two types of linear flows are considered in this study, namely, a uniaxial extensional flow and a simple shear flow. Presence of surfactants along the drop surface leads to the generation of an interfacial viscosity, which is different from the bulk. This interfacial viscosity generates a viscous drag that along wit…
Thin liquid films are central to everyday life. They are ubiquitous in modern technology (pharmaceuticals, coatings), consumer products (foams, emulsions) and also serve vital biological functions (tear film of the eye, pulmonary surfactants in the lung). A common feature in all these examples is the presence of surface-active molecules at the air-liquid interface. Though they form only molecularly-thin layers, these surfactants produce complex surface stresses on the free surface, which have important consequences for the dynamics and stability of the underlying thin liquid film. Here we cond…
We study the thermocapillary creeping flow induced by a thermal gradient at the liquid-air interface in the presence of insoluble surfactants (impurities). Convective sweeping of the surfactants causes density inhomogeneities that confers in-plane elastic features to the interface. This mechanism is discussed for radially symmetric temperature fields, in both the deep and shallow water regimes. When mass transport is controlled by convection, it is found that surfactants are depleted from a region whose size is inversely proportional to the interfacial elasticity. Both the concentration and th…
We investigate the dynamics of an insoluble surfactant on the surface of a thin viscous fluid spreading inward to fill a surfactant-free region. During the initial stages of surfactant self-healing, Marangoni forces drive an axisymmetric ridge inward to coalesce into a growing central distension; this is unlike outward-spreading, in which the ridge decays. In later dynamics, the distension slowly decays and the surfactant concentration equilibrates. We present results from experiments in which we simultaneously measure the surfactant concentration (using fluorescently-tagged lipids) and the fl…
Marangoni propulsion is a form of locomotion wherein an asymmetric release of surfactant by a body located at the surface of a liquid leads to its directed motion. We present in this paper a mathematical model for Marangoni propulsion in the viscous regime. We consider the case of a thin rigid circular disk placed at the surface of a viscous fluid and whose perimeter has a prescribed concentration of an insoluble surfactant, to which the rest of its surface is impenetrable. Assuming a linearized equation of state between surface tension and surfactant concentration, we derive analytically the …
Solutocapillary instability in slipping falling films
Centre for Applied Sciences (CAS), International Institute of Information Technology（国际信息技术学院应用科学中心）；Université Claude Bernard Lyon 1, LMFA, UMR 5509, CNRS, Ecole Centrale de Lyon, INSA Lyon（里昂第一大学）；Department of Mathematics, Vivekananda Mahavidyalaya（维韦卡南达学院数学系）
A hybrid Volume of Fluid Phase-Field method for Direct Numerical Simulations of soluble surfactant-laden interfacial flows
Univ. Lille, CNRS, Centrale Lille, Univ. Polytechnique Hauts-de-France, UMR 8520, IEMN（里尔大学、法国国家科学研究中心、中央里尔学院、上法兰西高等工学院）；Institut Universitaire de France（法国国立高等教育学院）；Department of Chemical Engineering, Indian Institute of Technology Roorkee（印度鲁尔基理工学院化学工程系）
When surface-active molecules are released at a liquid interface, their spreading dynamics is controlled by Marangoni flows. Though such Marangoni spreading was investigated in different limits, exact solutions remain very few. Here we consider the spreading of an insoluble surfactant along the interface of a deep fluid layer. For two-dimensional Stokes flows, it was recently shown that the non-linear transport problem can be exactly mapped to a complex Burgers equation [Crowdy, SIAM J. Appl. Math. 81, 2526 (2021)]. We first present a very simple derivation of this equation. We then provide fu…
A horizontal flow of two immiscible fluid layers with different densities, viscosities and thicknesses, subject to vertical gravitational forces and with an insoluble surfactant present at the interface, is investigated. The base Couette flow is driven by the horizontal motion of the channel walls. Linear and nonlinear stages of the (inertialess) surfactant and gravity dependent long-wave instability are studied using the lubrication approximation, which leads to a system of coupled nonlinear evolution equations for the interface and surfactant disturbances. The linear stability is determined …
A linear stability analysis of a two-layer plane Couette flow of two immiscible fluid layers with different densities, viscosities and thicknesses, bounded by two infinite parallel plates moving at a constant relative velocity to each other, with an insoluble surfactant along the interface and in the presence of gravity is carried out. The normal modes approach is applied to the equations governing flow disturbances. These equations, together with boundary conditions at the plates and the interface, yield a linear eigenvalue problem. When inertia is neglected velocity amplitudes are linear com…
Two-component liquid-vapor systems are modeled as two bulk phases divided by a two-dimensional surface phase and the mass and momentum balances are theoretically studied. Comparing the derived equations with some typical models of surface rheology, useful information about the interface location is obtained. It is demonstrated that the surface phase, set on the surface of tension, coincides with the equimolecular interface for insoluble surfactants, whereas it is placed on the surface of zero total mass density excess for soluble ones. The applicability of the model to surface electrostatics i…
