arXiv subjects

Elie Raphaël

Publications and source records attributed to Elie Raphaël.

At least 19 recordsLinked to original sources

arXiv2025

Stationary and transient correlations in driven electrolytes

Particle-particle correlation functions in ionic systems control many of their macroscopic properties. In this work, we use stochastic density functional theory to compute these correlations, and then we analyze their long-range behavior. In particular, we study the system's response to a rapid change (quench) in the external electric field. We show that the correlation functions relax diffusively toward the non-equilibrium stationary state and that in a stationary state, they present a universal conical shape. This shape distinguishes this system from systems with short-range interactions, where the correlations have a parabolic shape. We relate this temporal evolution of the correlations to the algebraic relaxation of the total charge current reported previously.

cond-mat.stat-mech↗

arXiv2023

Nanoparticle Taylor dispersion near charged surfaces with an open boundary

The dispersive spreading of microscopic particles in shear flows is influenced both by advection and thermal motion. At the nanoscale, interactions between such particles and their confining boundaries become unavoidable. We address the roles of electrostatic repulsion and absorption on the spatial distribution and dispersion of charged nanoparticles in near-surface shear flows, observed under evanescent illumination. The electrostatic repulsion between particles and the lower charged surface is tuned by varying electrolyte concentrations. Particles leaving the field of vision can be neglected from further analysis, such that the experimental ensemble is equivalent to that of Taylor dispersion with absorption. These two ingredients modify the particle distribution, deviating strongly from the Gibbs-Boltzmann one at the nanoscale studied here. The overall effect is to restrain the accessible space available to particles, leading to a striking, ten-fold reduction in the spreading dynamics as compared to the non-interacting case.

cond-mat.soft↗

arXiv2022

Enhanced Dip Coating on a Soft Substrate

A solid, withdrawn from a liquid bath, entrains a thin liquid film. This simple process, first described by Landau, Levich and Derjaguin (LLD), is commonly observed in everyday life. It also plays a central role in liquid capture by animals, and is widely used for surface-coating purposes in industry. Motivated by the emerging interest in the mechanics of very soft materials, and in particular the resulting elastocapillary coupling, we develop a dip-coating model that accounts for the additional presence of a soft solid layer atop the rigid plate. The elastic response of this soft layer is described by a Winkler's foundation. Using a combination of numerical, scaling and asymptotic-matching methods, we find a new softness-dependent power-law regime for the thickness of entrained liquid at small capillary number, which corresponds to a modified physics at play in the dynamic meniscus. The crossover between this regime and the classical dip-coating one occurs when the substrate's deformation is comparable to the thickness of the entrained liquid film.

cond-mat.soft↗

arXiv2022

Contactless Rheology of Soft Gels over a Broad Frequency Range

We report contactless measurements of the viscoelastic rheological properties of soft gels. The experiments are performed using a colloidal-probe Atomic Force Microscope (AFM) in a liquid environment and in dynamic mode. The mechanical response is measured as a function of the liquid gap thickness for different oscillation frequencies. Our measurements reveal an elastohydrodynamic (EHD) coupling between the flow induced by the probe oscillation and the viscoelastic deformation of the gels. The data are quantitatively described by a viscoelastic lubrication model. The frequency-dependent storage and loss moduli of the polydimethylsiloxane (PDMS) gels are extracted from fits of the data to the model and are in good agreement with the Chasset--Thirion law. Our results demonstrate that contactless colloidal-probe methods are powerful tools that can be used for probing soft interfaces finely over a wide range of frequencies.

cond-mat.mtrl-sci↗

arXiv2021

Time dependence of advection-diffusion coupling for nanoparticle ensembles

Advection-diffusion coupling can enhance particle and solute dispersion by orders of magnitude as compared to pure diffusion, with a steady state being reached for confined flow regions such as a nanopore or blood vessel. Here, by using evanescent wave microscopy, we measure for the first time the full dynamics of Taylor dispersion, highlighting the crucial role of the initial concentration profile. We make time-dependent, nanometrically-resolved particle dispersion measurements varying nanoparticle size, velocity gradient, and viscosity in sub-micrometric near-surface flows. Such resolution permits a measure of the full dynamical approach and crossover into the steady state, revealing a family of master curves. Remarkably, our results show that the dynamics depend sensitively on the initial spatial distribution of the nanoparticles. These observations are in quantitative agreement with existing analytical models and numerical simulations performed herein. We anticipate that our study will be a first step toward observing and modelling more complex situations at the nanoscale, such as target finding and chemical reactions in nanoconfined flows, dynamical adsorption and capture problems, as well as nanoscale drug delivery systems.

cond-mat.soft↗

arXiv2020

Unsteady Wave Drag on a Disturbance Moving Along an Arbitrary Trajectory

We derive analytical formulas for the wake and wave drag of a disturbance moving arbitrarily at the air-water interface. We show that, provided a constant velocity is reached in finite time, the unsteady surface displacement converges to its well-known steady counterpart as given by Havelock's famous formula. Finally we assess, in a specific situation, to which extent one can rightfully use Havelock's steady wave drag formula for non-uniform motion (quasi-static). Such an approach can be used to legitimize or discredit a number of studies which used steady wave drag formulas in unsteady situations.

physics.flu-dyn↗

arXiv2019

Cooperative strings and glassy dynamics in various confined geometries

Previously, we developed a minimal model based on random cooperative strings for the relaxation of supercooled liquids in the bulk and near free interfaces, and we recovered some key experimental observations. In this article, after recalling the main ingredients of the cooperative string model, we study the effective glass transition and surface mobility of various experimentally-relevant confined geometries: freestanding films, supported films, spherical particles, and cylindrical particles, with free interfaces and/or passive substrates. Finally, we introduce a novel way to account for a purely attractive substrate, and explore the impact of the latter in the previous geometries.

cond-mat.dis-nn↗

arXiv2018

Hydroelastic wake on a thin elastic sheet floating on water

We investigate the hydroelastic wake created by a perturbation moving at constant speed along a thin elastic sheet floating at the surface of deep water. Using a high-resolution cross-correlation imaging technique, we characterize the waves as a function of the perturbation speed, for different sheet thicknesses. The general theoretical expression for the dispersion relation of hydroelastic waves includes three components: gravity, bending and stretching. The bending modulus and the tension in the sheet are independently measured. Excellent agreement is found between the experimental data and the theoretical expression.

physics.flu-dyn↗

arXiv2018

Unsteady wave pattern generation by water striders

We perform an experimental and theoretical study of the wave pattern generated by the leg strokes of water striders during a propulsion cycle. Using the synthetic Schlieren method, we are able to measure the dynamic response of the free surface accurately. In order to match experimental conditions, we extend Bühler's theory of impulsive forcing (\cite{buhler}) to finite depth. We demonstrate the improved ability of this approach to reproduce the experimental findings, once the observed continuous forcing and hence non-zero temporal and spatial extent of the leg strokes is also taken into account.

physics.flu-dyn↗

arXiv2018

Elastowetting of Soft Hydrogel Spheres

When a soft hydrogel sphere is placed on a rigid hydrophilic substrate, it undergoes arrested spreading by forming an axisymmetric foot near the contact line, while conserving its global spherical shape. In contrast, liquid water (that constitutes greater than 90% of the hydrogel's volume) spreads into a thin film on the same surface. We study systematically this elastowetting of gel spheres on substrates of different surface energies, and find that their contact angle increases as the work of adhesion between the gel and the substrate decreases, as one would observe for drops of pure water - albeit being larger than in the latter case. This difference in the contact angles of gel and water appears to be due to the elastic shear stresses that develop in the gel and oppose its spreading. Indeed, by increasing the elastic modulus of the gel spheres, we find that their contact angle also increases. In addition, the length of the contact foot increases with the work of adhesion and sphere size, while it decreases when the elastic modulus of the gel is increased. We discuss those experimental results in light of a minimal analysis based on energy minimization, volume conservation, and scaling arguments.

cond-mat.soft↗

arXiv2017

Adsorption-Induced Slip Inhibition for Polymer Melts on Ideal Substrates

Hydrodynamic slip of a liquid at a solid surface represents a fundamental phenomenon in fluid dynamics that governs liquid transport at small scales. For polymeric liquids, de Gennes predicted that the Navier boundary condition together with the theory of polymer dynamics imply extraordinarily large interfacial slip for entangled polymer melts on ideal surfaces; this Navier-de Gennes model was confirmed using dewetting experiments on ultra-smooth, low-energy substrates. Here, we use capillary leveling - surface tension driven flow of films with initially non-uniform thickness - of polymeric films on these same substrates. Measurement of the slip length from a robust one-parameter fit to a lubrication model is achieved. We show that at the lower shear rates involved in leveling experiments as compared to dewetting ones, the employed substrates can no longer be considered ideal. The data is instead consistent with physical adsorption of polymer chains at the solid/liquid interface. We extend the Navier-de Gennes description using one additional parameter, namely the density of physically adsorbed chains per unit surface. The resulting formulation is found to be in excellent agreement with the experimental observations.

cond-mat.soft↗

arXiv2017

Elastocapillary Levelling of Thin Viscous Films on Soft Substrates

A thin liquid film with non-zero curvature at its free surface spontaneously flows to reach a flat configuration, a process driven by Laplace pressure gradients and resisted by the liquid's viscosity. Inspired by recent progresses on the dynamics of liquid droplets on soft substrates, we here study the relaxation of a viscous film supported by an elastic foundation. Experiments involve thin polymer films on elastomeric substrates, where the dynamics of the liquid-air interface is monitored using atomic force microscopy. A theoretical model that describes the coupled evolution of the solid-liquid and the liquid-air interfaces is also provided. In this soft-levelling configuration, Laplace pressure gradients not only drive the flow, but they also induce elastic deformations on the substrate that affect the flow and the shape of the liquid-air interface itself. This process represents an original example of elastocapillarity that is not mediated by the presence of a contact line. We discuss the impact of the elastic contribution on the levelling dynamics and show the departure from the classical self-similarities and power laws observed for capillary levelling on rigid substrates.

cond-mat.soft↗

arXiv2017

Cooperative strings in glassy nanoparticles

Motivated by recent experimental results on glassy polymer nanoparticles, we develop a minimal theoretical framework for the glass transition in spherical confinement. This is accomplished using our cooperative-string model for supercooled dynamics, that was successful at recovering the bulk phenomenology and describing the thin-film anomalies. In particular, we obtain predictions for the mobile-layer thickness as a function of temperature, and for the effective glass-transition temperature as a function of the radius of the spherical nanoparticle - including the existence of a critical particle radius below which vitrification never occurs. Finally, we compare the theoretical results to experimental data on polystyrene from the recent literature, and we discuss the latter.

cond-mat.stat-mech↗

arXiv2017

Liquid droplets act as "compass needles" for the stresses in a deformable membrane

We examine the shape of droplets atop deformable thin elastomeric films prepared with an anisotropic tension. As the droplets generate a deformation in the taut film through capillary forces, they assume a shape that is elongated along the high tension direction. By measuring the contact line profile, the tension in the membrane can be completely determined. Minimal theoretical arguments lead to predictions for the droplet shape and membrane deformation that are in excellent agreement with the data. On the whole, the results demonstrate that droplets can be used as probes to map out the stress field in a membrane.

cond-mat.soft↗

arXiv2017

Molecular dynamics simulation of the capillary leveling of viscoelastic polymer films

Surface tension-driven flow techniques have recently emerged as an efficient means of shedding light into the rheology of thin polymer films. Motivated by experimental and theoretical approaches in films bearing a varying surface topography, we present results on the capillary relaxation of a square pattern at the free surface of a viscoelastic polymer film, using molecular dynamics simulations of a coarse-grained polymer model. Height profiles are monitored as a function of time after heating the system above its glass-transition temperature and their time dependence is fitted to the theory of capillary leveling. Results show that the viscosity is not constant, but time dependent. In addition to providing a complementary insight about the local inner mechanisms, our simulations of the capillary-leveling process therefore probe the viscoelasticity of the polymer and not only its viscosity, in contrast to previous experimental approaches.

cond-mat.soft↗

arXiv2016

Van der Waals interaction between a moving nano-cylinder and a liquid thin film

We study the static and dynamic interaction between a horizontal cylindrical nano-probe and a thin liquid film. The effects of the physical and geometrical parameters, with a special focus on the film thickness, the probe speed, and the distance between the probe and the free surface are analyzed. Deformation profiles have been computed numerically from a Reynolds lubrication equation, coupled to a modified Young-Laplace equation, which takes into account the probe/liquid and the liquid/substrate non-retarded van der Waals interactions. We have found that the film thickness and the probe speed have a significant effect on the threshold separation distance below which the jump-to-contact instability is triggered. These results encourage the use of horizontal cylindrical nano-probes to scan thin liquid films, in order to determine either the physical or geometrical properties of the latter, through the measurement of interaction forces.

cond-mat.mes-hall↗

arXiv2016

Capillary levelling of free-standing liquid nanofilms

We report on the capillary-driven levelling of a topographical perturbation at the surface of a free-standing liquid nanofilm. The width of a stepped surface profile is found to evolve as the square root of time. The hydrodynamic model is in excellent agreement with the experimental data. In addition to exhibiting an analogy with diffusive processes, this novel system serves as a precise nanoprobe for the rheology of liquids at interfaces in a configuration that avoids substrate effects.

cond-mat.soft↗

arXiv2016

Elastohydrodynamic wake and wave resistance

The dynamics of a thin elastic sheet lubricated by a narrow layer of liquid is relevant to various situations and length scales. In the continuity of our previous work on viscous wakes, we study theoretically the effects of an external pressure disturbance moving at constant speed along the surface of a thin lubricated elastic sheet. In the comoving frame, the imposed pressure field creates a stationary deformation of the free interface that spatially vanishes in the far-field region. The shape of the wake and the way it decays depend on the speed and size of the external disturbance, as well as the rheological properties of both the elastic and liquid layers. The wave resistance, namely the force that has to be externally furnished in order to maintain the wake, is analyzed in detail.

physics.flu-dyn↗