The relationship between viscoelasticity and elasticity.

Soft materials that are subjected to large deformations exhibit an extremely rich phenomenology, with properties lying in between those of simple fluids and those of elastic solids. In the continuum description of these systems, one typically follows either the route of solid mechanics (Lagrangian description) or the route of fluid mechanics (Eulerian description). The purpose of this review is to highlight the relationship between the theories of viscoelasticity and of elasticity, and to leverage this connection in contemporary soft matter problems. We review the principles governing models for viscoelastic liquids, for example solutions of flexible polymers. Such materials are characterized by a relaxation time λ, over which stresses relax. We recall the kinematics and elastic response of large deformations, and show which polymer models do (and which do not) correspond to a nonlinear elastic solid in the limit λ → ∞. With this insight, we split the work done by elastic stresses into reversible and dissipative parts, and establish the general form of the conservation law for the total energy. The elastic correspondence can offer an insightful tool for a broad class of problems; as an illustration, we show how the presence or absence of an elastic limit determines the fate of an elastic thread during capillary instability.

Influence of the surface viscous stress on the pinch-off of free surfaces loaded with nearly-inviscid surfactants.

We analyze the breakup of a pendant water droplet loaded with SDS. The free surface minimum radius measured in the experiments is compared with that obtained from a numerical solution of the Navier-Stokes equations for different values of the shear and dilatational surface viscosities. This comparison shows the small but measurable effect of the surface viscous stresses for sufficiently small spatiotemporal distances from the breakup point, and allows to establish upper bounds for the values of the shear and dilatational viscosities. We study numerically the distribution of Marangoni and viscous stresses over the free surface as a function of the time to the pinching, and describe how surface viscous stresses grow in the pinching region as the free surface approaches its breakup. When Marangoni and surface viscous stresses are taken into account, the surfactant is not swept away from the thread neck in the time interval analyzed. Surface viscous stresses eventually balance the driving capillary pressure in the pinching region for small enough values of the time to pinching. Based on this result, we propose a scaling law to account for the effect of the surface viscosities on the last stage of temporal evolution of the neck radius.

A method for measuring the interfacial tension for density-matched liquids.

We propose a method to measure the interfacial tension characterizing the interface between two immiscible liquids of practically the same density. In this method, a cylindrical liquid bridge made of one the liquids is vibrated laterally inside a tank filled with the other. The first resonance frequency is determined and equated to the first eigenfrequency of the m=1 linear mode to infer the interfacial tension value. The method does not involve the density jump across the interface. Therefore, its accuracy is affected neither by the smallness of the Bond number nor by errors of the density difference. The experimental setup is relatively simple, and the procedure does not use image processing techniques. The results satisfactorily agree with those measured by TIFA-AI (Theoretical Fitting Image Analysis-Axisymmetric Interfaces) for the same liquid bridges when the density difference is sufficiently large for TIFA-AI to be valid. We conduct numerical simulations of the Navier-Stokes equations to determine the best parameter conditions for the proposed method. The transfer function characterizing the frequency response of the fluid configuration is measured in some experiments to quantify non-linear effects and to study the role played by the outer bath vibration.

Stability of a jet moving in a rectangular microchannel.

We study numerically the basic flow and linear stability of a capillary jet confined in a rectangular microchannel. We consider both the case where the interface does not touch the solid surfaces and that in which the jet adheres to them with a contact angle slightly smaller than 180^{∘}. Given an arbitrary set of values of the governing parameters, the fully developed (parallel) two-dimensional basic flow is calculated and then the growth rate of the dominant perturbation mode is determined as a function of the wave number. The flow is linearly stable if that growth rate is negative for all the wave numbers considered. We show that when the coflowing stream viscosity is sufficiently small in terms of that of the jet, there is an interval of the flow rate ratio Q for which the jet adheres to the walls or not depending on whether the flow is established by decreasing or increasing the value of Q. When the distance between the interface and the channel wall is of the order of the jet radius, the jet is unconditionally unstable. However, for sufficiently small interface-to-wall distances, the viscous stress can dominate the capillary pressure and fully stabilize the flow. Our results suggest that the capillary modes are suppressed and the flow becomes stable when the jet adheres to the channel walls. The combination of the above results indicates that, under certain parametric conditions, stable or unstable jets can be formed depending on whether the experimenter sets the flow rate ratio by decreasing or increasing progressively the jet flow rate while keeping constant that of the outer stream. Our theoretical predictions for the stablity of a coflow in a rectangular channel are consistent with previous experimental results [Humphry et al., Phys. Rev. E 79, 056310 (2009)PLEEE81539-375510.1103/PhysRevE.79.056310].

Electrospray cone-jet mode for weakly viscoelastic liquids.

We study theoretically the influence of viscoelasticity on the steady cone-jet mode of electrospray for small stress relaxation times. For this purpose, we numerically integrate the leaky-dielectric model together with the Oldroyd-B constitutive relationship and calculate both the base flow and linear eigenmodes characterizing its stability as a function of the governing parameters. We describe the effect of the polymeric stresses on both the cone-jet mode and the minimum flow rate stability limit. There are considerable differences between the Newtonian and viscoelastic electrospray realizations even for relatively small stress relaxation times due to the intense extensional deformation suffered by the fluid particles in the cone-jet transition region The axial polymeric stress shrinks the liquid meniscus and stabilizes it by pushing the fluid particle in the cone-to-jet transition region.

Aerodynamically stabilized Taylor cone jets.

We introduce a way to stabilize steady micro/nanoliquid jets issuing from Taylor cones together with coflowing gas streams. We study the dripping-jetting transition of this configuration theoretically through a global stability analysis as a function of the governing parameters involved. A balance between the local radial acceleration to the surface tension gradient, the mass conservation, and the energy balance equations enable us to derive two coupled scaling laws that predict both the minimum jet diameter and its maximum velocity. The theoretical prediction provides a single curve that describes not only the numerical computations but also experimental data from the literature for cone jets assisted with gas coflow. Additionally, we performed a set of experiments to verify what parameters influence the jet length. We adopt a very recent model for capillary jet length to our configuration by combining electrohydrodynamic effects with the gas flow through an equivalent liquid pressure. Due to diameters below 1 µm and high speeds attainable in excess of 100 m/s, this concept has the potential to be utilized for structural biology analyses with x-ray free-electron lasers at megahertz repetition rates as well as other applications.

Erratum: Influence of the Surface Viscosity on the Breakup of a Surfactant-Laden Drop [Phys. Rev. Lett. 118, 024501 (2017)].

This corrects the article DOI: 10.1103/PhysRevLett.118.024501.

Viscous Effects on Inertial Drop Formation.

The breakup of low-viscosity droplets like water is a ubiquitous and rich phenomenon. Theory predicts that in the inviscid limit one observes a finite-time singularity, giving rise to a universal power law, with a prefactor that is universal for a given density and surface tension. This universality has been proposed as a powerful tool to determine the dynamic surface tension at short time scales. We combine high-resolution experiments and simulations to show that this universality is unobservable in practice: in contrast to previous studies, we show that fluid and system parameters do play a role; notably a small amount of viscosity is sufficient to alter the breakup dynamics significantly.

Stabilization of axisymmetric liquid bridges through vibration-induced pressure fields.

Previous theoretical studies have indicated that liquid bridges close to the Plateau-Rayleigh instability limit can be stabilized when the upper supporting disk vibrates at a very high frequency and with a very small amplitude. The major effect of the vibration-induced pressure field is to straighten the liquid bridge free surface to compensate for the deformation caused by gravity. As a consequence, the apparent Bond number decreases and the maximum liquid bridge length increases. In this paper, we show experimentally that this procedure can be used to stabilize millimeter liquid bridges in air under normal gravity conditions. The breakup of vibrated liquid bridges is examined experimentally and compared with that produced in absence of vibration. In addition, we analyze numerically the dynamics of axisymmetric liquid bridges far from the Plateau-Rayleigh instability limit by solving the Navier-Stokes equations. We calculate the eigenfrequencies characterizing the linear oscillation modes of vibrated liquid bridges, and determine their stability limits. The breakup process of a vibrated liquid bridge at that stability limit is simulated too. We find qualitative agreement between the numerical predictions for both the stability limits and the breakup process and their experimental counterparts. Finally, we show the applicability of our technique to control the amount of liquid transferred between two solid surfaces.

Influence of the Surface Viscosity on the Breakup of a Surfactant-Laden Drop.

We examine both theoretically and experimentally the breakup of a pendant drop loaded with an insoluble surfactant. The experiments show that a significant amount of surfactant is trapped in the resulting satellite droplet. This result contradicts previous theoretical predictions, where the effects of surface tension variation were limited to solutocapillarity and Marangoni stresses. We solve numerically the hydrodynamic equations, including not only those effects but also those of surface shear and dilatational viscosities. We show that surface viscosities play a critical role to explain the accumulation of surfactant in the satellite droplet.

Convective-to-absolute instability transition in a viscoelastic capillary jet subject to unrelaxed axial elastic tension.

The convective-to-absolute instability transition in an Oldroyd-B capillary jet subject to unrelaxed axial stress is examined theoretically. There is a critical Weber number below which the jet is absolutely unstable under axisymmetric perturbations. We analyze the dependence of this critical parameter with respect to the Reynolds and Deborah numbers, as well as the unrelaxed axial stress. For small Deborah numbers, the unrelaxed stress destabilizes the viscoelastic jet, increasing the critical Weber number for which the convective-to-absolute instability transition takes place. If the Deborah number takes higher values, then the transitional Weber number decreases as the unrelaxed stress increases until two solution branches cross each other. The dominant branch for large axial stress leads to a threshold of this quantity above which the viscoelastic jet becomes absolutely unstable independently of the Weber number. The threshold depends on neither the Reynolds nor the Deborah number for sufficiently large values of these parameters.

Dynamics of an axisymmetric liquid bridge close to the minimum-volume stability limit.

We analyze both theoretically and experimentally the dynamical behavior of an isothermal axisymmetric liquid bridge close to the minimum-volume stability limit. First, the nature of this stability limit is investigated experimentally by determining the liquid bridge response to a mass force pulse for volumes just above that limit. In our experiments, the liquid bridge breakup takes place only when the critical volume is surpassed and is never triggered by the mass force pulse. Second, the growth of the small-amplitude perturbation mode initiating the liquid bridge breakage is measured experimentally and calculated from the linearized Navier-Stokes equations. The results of the linear stability analysis allow one to explain why liquid bridges with volumes just above the stability limit are so robust. Finally, the nonlinear process leading to the liquid bridge breakup is described from both experimental data and the solution of the full Navier-Stokes equations. Special attention is paid to the free-surface pinchoff. The results show that the flow becomes universal (independent of both the initial and boundary conditions) sufficiently close to that singularity and suggest that the transition from the inviscid to the viscous regime is about to take place in the final stage of both the experiments and numerical simulations.

Production of microbubbles from axisymmetric flow focusing in the jetting regime for moderate Reynolds numbers.

We analyze both experimentally and numerically the formation of microbubbles in the jetting regime reached when a moderately viscous liquid stream focuses a gaseous meniscus inside a converging micronozzle. If the total (stagnation) pressure of the injected gas current is fixed upstream, then there are certain conditions on which a quasisteady gas meniscus forms. The meniscus tip is sharpened by the liquid stream down to the gas molecular scale. On the other side, monodisperse collections of microbubbles can be steadily produced in the jetting regime if the feeding capillary is appropriately located inside the nozzle. In this case, the microbubble size depends on the feeding capillary position. The numerical simulations for an imposed gas flow rate show that a recirculation cell appears in the gaseous meniscus for low enough values of that parameter. The experiments allow one to conclude that the bubble pinch-off comprises two phases: (i) a stretching motion of the precursor jet where the neck radius versus the time before the pinch essentially follows a potential law, and (ii) a final stage where a very thin and slender gaseous thread forms and eventually breaks apart into a number of micron-sized bubbles. Because of the difference between the free surface and core velocities, the gaseous jet breakage differs substantially from that of liquid capillary jets and gives rise to bubbles with diameters much larger than those expected from the Rayleigh-type capillary instability. The dependency of the bubble diameter upon the flow-rate ratio agrees with the scaling law derived by A. M. Gañán-Calvo [Phys. Rev. E 69, 027301 (2004)], although a slight influence of the Reynolds number can be observed in our experiments.

Theoretical investigation of a technique to produce microbubbles by a microfluidic T junction.

A microfluidic technique is proposed to produce microbubbles. A gaseous stream is injected through a T junction into a channel transporting a liquid current. The gas adheres to a hydrophobic strip printed on the channel surface. When the gas and liquid flow rates are set appropriately, a gaseous rivulet flows over that strip. The rivulet breaks up downstream due to a capillary pearling instability, which leads to a monodisperse collection of microbubbles that can be much smaller than the channel size. The physics of the process is theoretically investigated, using both full numerical simulation of the Navier-Stokes equations and a linear stability analysis of an infinite gaseous rivulet driven by a coflowing liquid stream. This stability analysis allows one to determine a necessary condition to get this effect in a T junction device. It also provides reasonably good predictions for the size of the produced microbubbles as obtained from numerical experiments.

Numerical simulation of electrospray in the cone-jet mode.

We present a robust and computationally efficient numerical scheme for simulating steady electrohydrodynamic atomization processes (electrospray). The main simplification assumed in this scheme is that all the free electrical charges are distributed over the interface. A comparison of the results with those calculated with a volume-of-fluid method showed that the numerical scheme presented here accurately describes the flow pattern within the entire liquid domain. Experiments were performed to partially validate the numerical predictions. The simulations reproduced accurately the experimental shape of the liquid cone jet, providing correct values of the emitted electric current even for configurations very close to the cone-jet stability limit.

Global stability of the focusing effect of fluid jet flows.

The global stability of the steady jetting mode of liquid jets focused by coaxial gas streams is analyzed both theoretically and experimentally. Numerical simulations allow one to identify the physical mechanisms responsible for instability in the low viscosity and very viscous regimes of the focused liquid. The characteristic flow rates for which global instability takes place are estimated by a simple scaling analysis. These flow rates do not depend on the pressure drop (energy) applied to the system to produce the microjet. Their dependencies on the liquid viscosity are opposite for the two extremes studied: the characteristic flow rate increases (decreases) with viscosity for very low (high) viscosity liquids. Experiments confirmed the validity of these conclusions. The minimum flow rates below which the liquid meniscus becomes unstable are practically independent of the applied pressure drop for sufficiently large values of this quantity. For all the liquids analyzed, there exists an optimum value of the capillary-to-orifice distance for which the minimum flow rate attains a limiting value. That limiting value represents the lowest flow rate attainable with a given experimental configuration in the steady jetting regime. A two-dimensional stability map with a high degree of validity is plotted on the plane defined by the Reynolds and capillary numbers based on the limiting flow rate.

Spatiotemporal instability of a confined capillary jet.

Recent experimental studies on the instability of capillary jets have revealed the suitability of a linear spatiotemporal instability analysis to ascertain the parametrical conditions for specific flow regimes such as steady jetting or dripping. In this work, an extensive analytical, numerical, and experimental description of confined capillary jets is provided, leading to an integrated picture both in terms of data and interpretation. We propose an extended, accurate analytic model in the low Reynolds number limit, and introduce a numerical scheme to predict the system response when the liquid inertia is not negligible. Theoretical predictions show remarkable accuracy when compared with the extensive experimental mapping.

Self-rotation in electrocapillary flows.

The mechanism of appearance of swirl in a certain class of converging flows is investigated numerically. The analysis is motivated by the spontaneous generation of swirl, which has been observed in electrified menisci (Taylor cones). The electrical stress acting on the cone surface drives these electrified millimetric fluid flows. Numerical results show that the primarily swirl-free meridian flow is unstable within an interval of values of the Reynolds number based on the surface stress. For values of the Reynolds number outside this interval, which depends on the forcing conditions and the geometry of the flow, the nonswirling meridian flow is stable. The instability mechanism of circulation amplification, which has nothing to do with the well-known increase of swirl velocity due to the vortex stretching mechanism, is due to a convection-diffusion effect. The circulation accumulated at the axis zone by the converging meridian motion is pumped by diffusion toward the conical surface. This feedback loop mechanism shoots the circulation amplification for values of the Reynolds number larger than a critical one. The same instability mechanism of swirl amplification could also appear in other converging flows generated by body forces (natural convection, electrical forces, etc.).