Searcharxiv⌕ Search

arXiv subjects

Thomas Salez

Publications and source records attributed to Thomas Salez.

At least 55 records · Page 3Linked to original sources

Numerical simulations of confined Brownian-yet-non-Gaussian motion

Brownian motion is a central scientific paradigm. Recently, due to increasing efforts and interests towards miniaturization and small-scale physics or biology, the effects of confinement on such a motion have become a key topic of investigation. Essentially, when confined near a wall, a particle moves much slower than in the bulk due to friction at the boundaries. The mobility is therefore locally hindered and space-dependent, which in turn leads to the apparition of so-called multiplicative noises, and associated non-Gaussianities which remain difficult to resolve at all times. Here, we exploit simple, optimized and efficient numerical simulations to address Brownian motion in confinement in a broadrange and quantitative way. To do so, we integrate the overdamped Langevin equation governing the thermal dynamics of a negatively-buoyant single spherical colloid within a viscous fluid confined by two rigid walls, including surface charges. From the produced large set of long random trajectories, we perform a complete statistical analysis and extract all the key quantities, such as the probability distributions in displacements and their main moments. In particular, we propose a novel method to compute high-order cumulants by reducing convergence problems, and employ it to efficiently characterize the inherent non-Gaussianity of the confined process.

cond-mat.stat-mech↗

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↗

Non-Gaussian diffusion near surfaces

We study the diffusion of particles confined close to a single wall and in double-wall planar channel geometries where the local diffusivities depend on the distance to the boundaries. Displacement parallel to the walls is Brownian as characterized by its variance, but it is non-Gaussian having a non-zero fourth cumulant. Establishing a link with Taylor dispersion, we calculate the fourth cumulant and the tails of the displacement distribution for general diffusivity tensors along with potentials generated by either the walls or externally, for instance gravity. Experimental and numerical studies of the motion of a colloid in the direction parallel to the wall give measured fourth cumulants which are correctly predicted by our theory. Interestingly, contrary to models of Brownian-yet-non-Gaussian diffusion, the tails of the displacement distribution are shown to be Gaussian rather than exponential. All together, our results provide additional tests and constraints for the inference of force maps and local transport properties near surfaces.

cond-mat.soft↗

Mechanical response of a thick poroelastic gel in contactless colloidal-probe rheology

When a rigid object approaches a soft material in a viscous fluid, hydrodynamic stresses arise in the lubricated contact region and deform the soft material. The elastic deformation modifies in turn the flow, hence generating a soft-lubrication coupling. Moreover, soft elastomers and gels are often porous. These materials may be filled with solvent or uncrosslinked polymer chains, and might be permeable to the surrounding fluid, which complexifies further the description. Here, we derive the point-force response of a semi-infinite and permeable poroelastic substrate. Then, we use this fundamental solution in order to address the specific poroelastic lubrication coupling associated with contactless colloidal-probe methods. In particular, we derive the conservative and dissipative components of the force associated with the oscillating vertical motion of a sphere close to the poroelastic substrate. Our results may be relevant for dynamic surface force apparatus and contactless colloidal-probe atomic force microscopy experiments on soft, living and/or fragile materials, such as swollen hydrogels and biological membranes.

cond-mat.mtrl-sci↗

On the bridge hypothesis in the glass transition of freestanding polymer films

Freestanding thin polymer films with high molecular weights exhibit an anomalous decrease in the glass-transition temperature with film thickness. Specifically, in such materials, the measured glass-transition temperature evolves in an affine way with the film thickness, with a slope that weakly depends on the molecular weight. De Gennes proposed a sliding mechanism as the hypothetical dominant relaxation process in these systems, where stress kinks could propagate in a reptation-like fashion through so called bridges, i.e. from one free interface to the other along the backbones of polymer macromolecules. Here, by considering the exact statistics of finite-sized random walks within a confined box, we investigate in details the bridge hypothesis. We show that the sliding mechanism cannot reproduce the basic features appearing in the experiments, and we exhibit the fundamental reasons behind such a fact.

cond-mat.mtrl-sci↗

Surface and Bulk Relaxation of Vapour-Deposited Polystyrene Glasses

We have studied the liquid-like response of the surface of vapour-deposited glassy films of polystyrene to the introduction of gold nanoparticles on the surface. The build-up of polymer material was measured as a function of time and temperature for both as-deposited films, as well as films that have been rejuvenated to become normal glasses cooled from the equilibrium liquid. The temporal evolution of the surface profile is well described by the characteristic power law of capillary-driven surface flows. In all cases, the surface evolution of the as-deposited films and the rejuvenated films are enhanced compared to bulk and are not easily distinguishable from each other. The temperature dependence of the measured relaxation times determined from the surface evolution is found to be quantitatively comparable to similar studies for high molecular weight spincast polystyrene. Comparisons to numerical solutions of the glassy thin film equation provide quantitative estimates of the surface mobility. For temperatures sufficiently close to the glass-transition temperature, particle embedding is also measured and used as a probe of bulk dynamics, and in particular bulk viscosity.

cond-mat.mtrl-sci↗

Near-critical spreading of droplets

We study the spreading of droplets in a near-critical phase-separated liquid mixture, using a combination of experiments, lubrication theory and finite-element numerical simulations. The classical Tanner's law describing the spreading of viscous droplets is robustly verified when the critical temperature is neared. Furthermore, the microscopic cut-off length scale emerging in this law is obtained as a single free parameter for each given temperature. In total-wetting conditions, this length is interpreted as the thickness of the thin precursor film present ahead of the apparent contact line. The collapse of the different evolutions onto a single Tanner-like master curve demonstrates the universality of viscous spreading before entering in the fluctuation-dominated regime. Finally, our results reveal a counter-intuitive and sharp thinning of the precursor film when approaching the critical temperature, which is attributed to the vanishing spreading parameter at the critical point.

cond-mat.soft↗

Microscopic foundation of the $μ$(I) rheology for dense granular flows on inclined planes

Macroscopic and microscopic properties of dense granular layers flowing down inclined planes are obtained from Discrete-Element-Method simulations for both frictionless and frictional grains. Three fundamental observations for dense granular flows are recovered, namely the occurrence of a critical stress, the Bagnold velocity profile, as well as well-defined friction and dilatancy laws. The microscopic aspects of the grain motion highlight the formation of transient clusters. From this microscopic picture, we derive a theoretical scaling model without any empirical input that explains quantitatively the fundamental laws of dense granular flows in incline plane and shear geometries. The adequacy between the model and the observed results suggests that granular flows can be viewed as flows from thermal fluids of hard spheres.

cond-mat.dis-nn↗

Large and non-linear permeability amplification with polymeric additives in hydrogel membranes

Hydrogels which are hydrophilic and porous materials have recently emerged as promising systems for filtration applications. In our study, we prepare hydrogel membranes by the photopolymerization of a mixture of poly (ethylene glycol) diacrylate (PEGDA) and large poly(ethylene glycol) (PEG) chains of 300 000 g.mol-1 in the presence of a photoinitiator. We find that this addition of free PEG chains induces a large and non-linear increase of the water permeability. Indeed, by changing the content of PEG chains added, we obtain variations of the hydrogel water permeability over two orders of magnitude. The highest water permeability values are obtained for the membranes when the PEG concentration is equal to its critical overlap concentration C*. Moreover, we find that the flow rate of water through the membranes varies non-linearly with the pressure. We relate this result to the deformability of the membranes as the applied pressure leads to a compression of the pores. This study provides new perspectives for the design of flexible hydrogel membranes with controlled permeability and their application in water treatment and bioseparation.

cond-mat.mtrl-sci↗

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↗

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↗

Universal Self-Similar Attractor in the Bending-Driven Leveling of Thin Viscous Films

We study theoretically and numerically the bending-driven leveling of thin viscous films within the lubrication approximation. We derive the Green's function of the linearized thin-film equation and further show that it represents a universal self-similar attractor at long times. As such, the rescaled perturbation of the film profile converges in time towards the rescaled Green's function, for any summable initial perturbation profile. In addition, for stepped axisymmetric initial conditions, we demonstrate the existence of another, short-term and one-dimensional-like self-similar regime. Besides, we characterize the convergence time towards the long-term universal attractor in terms of the relevant physical and geometrical parameters, and provide the local hydrodynamic fields and global elastic energy in the universal regime as functions of time. Finally, we extend our analysis to the non-linear thin-film equation through numerical simulations.

cond-mat.mtrl-sci↗

Dewetting of a thin polymer film under shear

The objective of this work is to study the role of shear on the rupture of ultrathin polymer films. To do so, a finite-difference numerical scheme for the resolution of the thin film equation was set up taking into account capillary and van der Waals (vdW) forces. This method was validated by comparing the dynamics obtained from an initial harmonic perturbation to established theoretical predictions. With the addition of shear, three regimes have then been evidenced as a function of the shear rate. In the case of low shear rates the rupture is delayed when compared to the no-shear problem, while at higher shear rates it is even suppressed: the perturbed interface goes back to its unperturbed state over time. In between these two limiting regimes, a transient one in which shear and vdW forces balance each other, leading to a non-monotonic temporal evolution of the perturbed interface, has been identified. While a linear analysis is sufficient to describe the rupture time in the absence of shear, the nonlinearities appear to be essential otherwise.

cond-mat.mtrl-sci↗

Soft-lubrication interactions between a rigid sphere and an elastic wall

The motion of an object within a viscous fluid and in the vicinity of a soft surface induces a hydrodynamic stress field that deforms the latter, thus modifying the boundary conditions of the flow. This results in elastohydrodynamic (EHD) interactions experienced by the particle. Here, we derive a soft-lubrication model, in order to compute all the forces and torque applied on a rigid sphere that is free to translate and rotate near an elastic wall. We focus on the limit of small deformations of the surface with respect to the fluid-gap thickness, and perform a perturbation analysis in dimensionless compliance. The response is computed in the framework of linear elasticity, for planar elastic substrates in the limiting cases of thick and thin layers. The EHD forces are also obtained analytically using the Lorentz reciprocal theorem.

cond-mat.soft↗

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↗

Stochastic Inference of Surface-Induced Effects using Brownian Motion

Brownian motion in confinement and at interfaces is a canonical situation, encountered from fundamental biophysics to nanoscale engineering. Using the Lorenz-Mie framework, we optically record the thermally-induced tridimensional trajectories of individual microparticles, within salty aqueous solutions, in the vicinity of a rigid wall, and in the presence of surface charges. We construct the time-dependent position and displacement probability density functions, and study the non-Gaussian character of the latter which is a direct signature of the hindered mobility near the wall. Based on these distributions, we implement a novel, robust and self-calibrated multifitting method, allowing for the thermal-noise-limited inference of diffusion coefficients spatially-resolved at the nanoscale, equilibrium potentials, and forces at the femtoNewton resolution.

cond-mat.soft↗

Nanobubble-induced flow of immersed glassy polymer films

We study the free-surface deformation dynamics of an immersed glassy thin polymer film supported on a substrate, induced by an air nanobubble at the free surface.We combine analytical and numerical treatments of the glassy thin film equation, resulting from the lubrication approximation applied to the surface mobile layer of the glassy film, under the driving of an axisymmetric step function in the pressure term accounting for the nanobubble's Laplace pressure. Using the method of Green's functions, we derive a general solution for the film profile. We show that the lateral extent of the surface perturbation follows an asymptotic viscocapillary power-law behaviour in time, and that the film's central height decays logarithmically in time in this regime. This process eventually leads to film rupture and dewetting at finite time, for which we provide an analytical prediction exhibiting explicitly the dependencies in surface mobility, film thickness and bubble size, among others. Finally, using finite-element numerical integration, we discuss how non-linear effects induced by the curvature and film profile can affect the evolution.

cond-mat.mtrl-sci↗

Contactless rheology of finite-size air-water interfaces

We present contactless atomic-force microscopy measurements of the hydrodynamic interactions between a rigid sphere and an air bubble in water at the micro-scale. The size of the bubble is found to have a significant effect on the response due to the long-range capillary deformation of the air-water interface. To rationalize the experimental data, we develop a viscocapillary lubrication model accounting for the finite-size effect. The comparison between experiments and theory allows us to measure the air-water surface tension, without contact, paving the way towards robust contactless tensiometry of polluted air-water interfaces.

cond-mat.soft↗