arXiv subjects

Thomas Salez

Publications and source records attributed to Thomas Salez.

At least 91 records · Page 5Linked to original sources

arXiv2018

Microfluidic probing of the complex interfacial rheology of multilayer capsules

Encapsulation of chemicals using polymer membranes enables to control their transport and delivery for applications such as agrochemistry or detergency. To rationalize the design of polymer capsules, it is necessary to understand how the membranes' mechanical properties control the transport and release of the cargo. In this article, we use microfluidics to produce model polymer capsules and study in situ their behavior in controlled elongational flows. Our model capsules are obtained by assembling polymer mono and hydrogen-bonded bilayers at the surface of an oil droplet in water. We also use microfluidics to probe in situ the mechanical properties of the membranes in a controlled elongational flow generated by introducing the capsules through a constriction and then in a larger chamber. The deformation and relaxation of the capsules depend on their composition and especially on the molecular interactions between the polymer chains that form the membranes and the anchoring energy of the first layer. We develop a model and perform numerical simulations to extract the main interfacial properties of the capsules from the measurement of their deformations in the microchannels.

cond-mat.soft↗

arXiv2018

Adsorption dynamics of hydrophobically modified polymers at an air-water interface

Using surface-tension measurements, we study the brush-limited adsorption dynamics of a range of amphiphilic polymers, PAAH-$α$-$\textrm{C}_n$ composed of a poly(acrylic acid) backbone, PAAH, grafted with a fraction $α$ of alkyl moieties, containing either $n=8$ or $n=12$ carbon atoms, at pH conditions where the PAAH backbone is not charged. At short times, the surface tension decreases more sharply as the degree of grafting increases while at long times, the adsorption dynamics becomes logarithmic in time and is slower as the degree of grafting increases. This logarithmic behavior at long times indicates the building of a free-energy barrier which grows over time. To account for the observed surface tension evolution with the degree of grafting we propose a scenario, where the free-energy barrier results from both the deformation of the incoming polymer coils and the deformation of the adsorbed brush. Our model involves only two fitting parameters, the monomer size and the area needed for one molecule during adsorption and is in agreement with the experimental data. We obtain a reasonable value for the monomer size and find an area per adsorbed polymer chain of the order of 1nm$^2$, showing that the polymer chains are strongly stretched as they adsorb.

cond-mat.soft↗

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

Influence of outer-layer finite-size effects on the rupture kinetics of a thin polymer film embedded in an immiscible matrix

In capillary-driven fluid dynamics, simple departures from equilibrium offer the chance to quantitatively model the resulting relaxations. These dynamics in turn provide insight on both practical and fundamental aspects of thin-film hydrodynamics. In this work, we describe a model trilayer dewetting experiment elucidating the effect of solid, no-slip confining boundaries on the bursting of a liquid film in a viscous environment. This experiment was inspired by an industrial polymer processing technique, multilayer coextrusion, in which thousands of alternating layers are stacked atop one another. When pushed to the nanoscale limit, the individual layers are found to break up on time scales shorter than the processing time. To gain insight on this dynamic problem, we here directly observe the growth rate of holes in the middle layer of the trilayer films described above, wherein the distance between the inner film and solid boundary can be orders of magnitude larger than its thickness. In otherwise identical experimental conditions, thinner films break up faster than thicker ones. This observation is found to agree with a scaling model that balances capillary driving power and viscous dissipation with, crucially, a no-slip boundary condition at the solid substrate/viscous environment boundary. In particular, even for the thinnest middle-layers, no finite-size effect is needed to explain the data. The dynamics of hole growth is captured by a single master curve over four orders of magnitude in the dimensionless hole radius and time, and is found to agree well with predictions including analytic expressions for the dissipation.

cond-mat.soft↗

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↗

arXiv2018

Transient deformation of a droplet near a microfluidic constriction : a quantitative analysis

We report on experiments that consist in deforming a collection of monodisperse droplets produced by a microfluidic chip through a flow-focusing device. We show that a proper numerical modelling of the flow is necessary to access the stress applied by the latter on the droplet along its trajectory through the chip. This crucial step enables the full integration of the differential equation governing the dynamical deformation, and consequently the robust measurement of the interfacial tension by fitting the experiments with the calculated deformation. Our study thus demonstrates the feasibility of quantitative in-situ rheology in microfluidic flows involving e.g. droplets, capsules or cells.

cond-mat.soft↗

arXiv2018

Surface energy of strained amorphous solids

Surface stress and surface energy are fundamental quantities which characterize the interface between two materials. Although these quantities are identical for interfaces involving only fluids, the Shuttleworth effect demonstrates that this is not the case for most interfaces involving solids, since their surface energies change with strain. Crystalline materials are known to have strain dependent surface energies, but in amorphous materials, such as polymeric glasses and elastomers, the strain dependence is debated due to a dearth of direct measurements. Here, we utilize contact angle measurements on strained glassy and elastomeric solids to address this matter. We show conclusively that interfaces involving polymeric glasses exhibit strain dependent surface energies, and give strong evidence for the absence of such a dependence for incompressible elastomers. The results provide fundamental insight into our understanding of the interfaces of amorphous solids and their interaction with contacting liquids.

cond-mat.soft↗

arXiv2017

Adhesion-induced fingering instabilities in thin elastic films under strain

In this study, thin elastic films supported on a rigid substrate are brought into contact with a spherical glass indenter. Upon contact, adhesive fingers emerge at the periphery of the contact patch with a characteristic wavelength. Elastic films are also pre-strained along one axis before initiation of contact, causing the fingering pattern to become anisotropic and align with the axis along which the strain was applied. This transition from isotropic to anisotropic patterning is characterized quantitatively and a simple model is developed to understand the origin of the anisotropy.

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

Emergent Strain-Stiffening in Interlocked Granular Chains

Granular chain packings exhibit a striking emergent strain-stiffening behavior despite the individual looseness of the constitutive chains. Using indentation experiments on such assemblies, we measure an exponential increase in the collective resistance force $F$ with the indentation depth $z$, and with the square root of the number $\mathcal{N}$ of beads per chain. These two observations are respectively reminiscent of the self-amplification of friction in a capstan or in interleaved books, as well as the physics of polymers. The experimental data are well captured by a novel model based on these two ingredients. Specifically, the resistance force is found to vary according to the universal relation: $\log F \sim μ\sqrt{\mathcal{N}} Φ^{11/8}z/ b $, where $μ$ is the friction coefficient between two elementary beads, $b$ is their size, and $Φ$ is the volume fraction of chain beads when semi-diluted in a surrounding medium of unconnected beads. Our study suggests that theories normally confined to the realm of polymer physics at a molecular level can be used to explain phenomena at a macroscopic level. This class of systems enables the study of friction in complex assemblies, with practical implications for the design of new materials, the textile industry, and biology.

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

Rotation of an immersed cylinder sliding near a thin elastic coating

It is known that an object translating parallel to a soft wall in a viscous fluid produces hydro- dynamic stresses that deform the wall, which, in turn, results in a lift force on the object. Recent experiments with cylinders sliding under gravity near a soft incline, which confirmed theoretical arguments for the lift force, also reported an unexplained steady-state rotation of the cylinders [Saintyves et al. PNAS 113(21), 2016]. Motivated by these observations, we show, in the lubrication limit, that an infinite cylinder that translates in a viscous fluid parallel to a soft wall at constant speed and separation distance must also rotate in order to remain free of torque. Using the Lorentz reciprocal theorem, we show analytically that for small deformations of the elastic layer, the angular velocity of the cylinder scales with the cube of the sliding speed. These predictions are confirmed numerically. We then apply the theory to the gravity-driven motion of a cylinder near a soft incline and find qualitative agreement with the experimental observations, namely that a softer elastic layer results in a greater angular speed of the cylinder.

physics.flu-dyn↗

arXiv2017

One-Step Fabrication of pH-Responsive Membranes and Microcapsules through Interfacial H-Bond Polymer Complexation

Biocompatible microencapsulation is of widespread interest for the targeted delivery of active species in fields such as pharmaceuticals, cosmetics and agro-chemistry. Capsules obtained by the self-assembly of polymers at interfaces enable the combination of responsiveness to stimuli, biocompatibility and scaled up production. Here, we present a one-step method to produce in situ membranes at oil-water interfaces, based on the hydrogen bond complexation of polymers between H-bond acceptor and donor in the oil and aqueous phases, respectively. This robust process is realized through different methods, to obtain capsules of various sizes, from the micrometer scale using microfluidics or rotor-stator emulsification up to the centimeter scale using drop dripping. The polymer layer exhibits unique self-healing and pH-responsive properties. The membrane is viscoelastic at pH = 3, softens as pH is progressively raised, and eventually dissolves above pH = 6 to release the oil phase. This one-step method of preparation paves the way to the production of large quantities of functional capsules.

cond-mat.soft↗

arXiv2017

Existence of a critical layer thickness in PS/PMMA nanolayered films

An experimental study was carried out to investigate the existence of a critical layer thickness in nanolayer coextrusion, under which no continuous layer is observed. Polymer films containing thousands of layers of alternating polymers with individual layer thicknesses below 100 nm have been prepared by coextrusion through a series of layer multiplying elements. Different films composed of alternating layers of poly(methyl methacrylate) (PMMA) and polystyrene (PS) were fabricated with the aim to reach individual layer thicknesses as small as possible, varying the number of layers, the mass composition of both components and the final total thickness of the film. Films were characterized by atomic force microscopy (AFM) and a statistical analysis was used to determine the distribution in layer thicknesses and the continuity of layers. For the PS/PMMA nanolayered systems, results point out the existence of a critical layer thickness around 10 nm, below which the layers break up. This critical layer thickness is reached regardless of the processing route, suggesting it might be dependent only on material characteristics but not on process parameters. We propose this breakup phenomenon is due to small interfacial perturbations that are amplified by (van der Waals) disjoining forces.

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↗