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The question when and how dense granular materials start to flow under stress, despite many industrial and geophysical applications, remains largely unresolved. We develop and test a simple equation for the onset of quasi-static flows of granular materials which is based on the frictional aging of the granular packing. The result is a non-monotonic stress-strain relation which - akin to classical friction - is independent of the shear rate. This relation suffices to understand the below-threshold deformations of aging granular media, and its solid-to-liquid transition. Our results also elucidate the (flow) history dependence of the mechanical properties, and the sensitivity to initial preparation of granular media., 5 pages, 3 figures

We investigate the local viscosity of a polymer glass around its glass transition temperature using environment-sensitive fluorescent molecular rotors embedded in the polymer matrix. The rotors' fluorescence depends on the local viscosity, and measuring the fluorescence intensity and lifetime of the probe therefore allows to measure the local free volume in the polymer glass when going through the glass transition. This also allows us to study the local viscosity and free volume when the polymer film is put under an external stress. We find that the film does not flow homogeneously, but undergoes shear banding that is visible as a spatially varying free volume and viscosity., Comment: 8 pages, 7 figures

Spraying is a widely used method to produce a liquid sheet that breaks up into droplets of a certain size distribution. When spraying simple liquids, it is known which experimental parameters determine the droplet size distribution. For many applications, however, surfactants are added, producing a hitherto unknown effect on the droplet size distribution. Using two generic types of spraying nozzles, we sprayed solutions of different types of aqueous surfactants and measured the droplet size distribution of the sprays. We find that the breakup of surfactant solutions is similar to that of pure water but results in droplets that are smaller. The resulting droplet size distribution can be well described using the predictions for simple liquids provided that we replace the parameter of the equilibrium surface tension with the dynamic surface tension of the surfactant solution at a surface age of 15 ms, which is the characteristic time for destabilization and breakup of the liquid sheet. By rescaling with the mean droplet size, the droplet size distributions of water and sprays with different concentrations of surfactants all collapse onto a single curve that is given by the compound Gamma function found previously for pure liquids.

We observe a novel type of shear banding in the rheology of thixotropic yield-stress fluids that is due to the coupling of both non-locality and thixotropy. The latter is known to lead to shear banding even in homogeneous stress fields, but the bands observed in the presence of non-local effects appear different as the shear rate varies continuously over the shear band. Here, we introduce a simple non-local model for the shear banding (NL-SB), and we implement it for the analysis of micron-scale rheo-MRI velocimetry measurements of a milk microgel suspension in a cone-and-plate geometry. The proposed NL-SB model accurately quantifies the cooperativity length and yields values in the order of the aggregate size in the microgel.

We investigate the influence of surfactants on capillary rise and corner flow in angular pores. We therefore study capillary rise for simple fluids and surfactant solutions, comparing square to cylindrical capillaries. We show that fingers start to form in the corners of the square capillaries when the capillary rise slows down before reaching the equilibrium height. The corner flow scales as t1/3 and its quantitative understanding necessitates that the surface wettability is taken into account in terms of the liquid’s advancing contact angle on the capillary walls inside the corner. Adding surfactants to water greatly influences the corner flow in square capillaries: depending on the nature of the surfactant, the corner flow can be either suppressed completely due to autophobic effects or enhanced due to the presence of Marangoni stresses caused by a surface tension gradient inside the liquid fingers.

The formation and destabilisation of viscoelastic filaments are of importance in many industrial and biological processes. Filament instabilities have been observed for viscoelastic fluids but recently also for soft elastic solids. In this work, we address the central question how to connect the dynamical behavior of viscoelastic liquids to that of soft elastic solids. We take advantage of a biopolymer material whose viscoelastic properties can be tuned over a very large range by its pH, and study the destabilization and ensuing instabilities in uniaxial extensional deformation. In agreement with very recent theory, we find that the interface shapes dictated by the instabilities converge to an identical similarity solution for low-viscosity viscoelastic fluids and highly elastic gels. We thereby bridge the gap between very fluid and strongly elastic materials. In addition, we provide direct evidence that at late times an additional filament instability occurs due to a dynamical phase separation., 11 pages, 13 figures

Steady shear measurements on three yield-stress fluids, a foam and two types of emulsions, were carried out using a smooth torsional parallel-plate geometry, with different gap spacings to assess the effect of wall slip on the normal stress differences. The classical Mooney analysis gave slip-corrected flow curves that agreed with data from a roughened cone-and-plate for all three materials, despite the fact that the compatibility requirement between the flow curve and slip velocity functionalities was not satisfied, indicating that the method is robust for this geometry. All three materials exhibited finite normal stresses following yielding, with power-law exponents of approximately 0.4, as well as shear stresses that can be represented by the Herschel–Bulkley model. The systems showed complete slip for shear stresses below the yield stress, with the stress transmitted to the unyielded material through a thin liquid layer causing an elastic deformation that was measurable for the unyielded foam, which can be represented by the Mooney–Rivlin elastic constitutive equation. The unyielded foam exhibited large sample-to-sample variations in the apparent modulus for identical loading conditions.

From everyday experience, we all know that a solid edge can deflect a liquid flowing over it significantly, up to the point where the liquid completely sticks to the solid. Although important in pouring, printing, and extrusion processes, there is no predictive model of this so-called "teapot effect." By grazing vertical cylinders with inclined capillary liquid jets, here we use the teapot effect to attach the jet to the solid and form a new structure: the liquid helix. Using mass and momentum conservation along the liquid stream, we first quantitatively predict the shape of the helix and then provide a parameter-free inertial-capillary adhesion model for the jet deflection and critical velocity for helix formation.

The mechanism involved in stick-slip phenomena, such as earthquakes, is controlled by the interfacial shear stress., When two objects are in contact, the force necessary to overcome friction is larger than the force necessary to keep sliding motion going. This difference between static and dynamic friction is usually attributed to the growth of the area of real contact between rough surfaces in time when the system is at rest. We directly measure the area of real contact and show that it actually increases during macroscopic slip, despite the fact that dynamic friction is smaller than static friction. This signals a decrease in the interfacial shear strength, the friction per unit contact area, which is due to a mechanical weakening of the asperities. This provides a novel explanation for stick-slip phenomena in, e.g., earthquakes.

We investigate which property of non-Newtonian fluids determines the deceleration of a high-speed impacting object. Using high-speed camera footage, we measure the velocity decrease of a high-speed spherical object impacting a typical Newtonian fluid (water) as a reference and compare it with a shear thickening fluid (cornstarch) and a shear thinning viscoelastic fluid (a weakly cross-linked polymer gel). Three models describing the kinetic energy loss of the object are considered: fluid inertia, shear thickening and viscoelasticity. By fitting the three models to the experimental data, we conclude that the viscoelastic model works best for both the cornstarch and the polymer gel. Since the cornstarch is also viscoelastic, we conclude that the ability to stop objects of these complex fluids is given by their viscoelasticity rather than shear thickening or shear thinning.

Recent theories of drag reduction in wall turbulence assumed that the presence of the polymer leads to an effective viscosity, which increases linearly with the distance from the wall. Such a linear viscosity profile reduces the Reynolds stress (i.e., the momentum flux to the wall), which leads to drag reduction. For the usual flexible polymers employed in drag reduction, the effective viscosity is however a strongly non-linear effect that is difficult to quantify. We therefore investigate the turbulent drag reduction characteristics of a stiff rod-like polymer for which any effective viscosity changes are only due to the orientation of the polymers. The results show that close to the walls the polymers orient and the viscosity is low, whereas in the bulk the polymers are randomly oriented and the effective viscosity is high. This indeed leads to a reduction of the Reynolds stress and hence to a drag reduction.

Nanocomposites consisting of polymers reinforced with filler particles are important for a wide variety of industries and processes, but although they exhibit unique viscoelastic properties and as such are widely applied in e.g. tires, the precise mechanism of their reinforcement is at best incompletely understood at present. In order to understand it at a fundamental level, and ultimately control it in practice, it is essential to determine the impact of interactions between filler particles and polymer matrix on the nanocomposite microstructure and its macroscopic dynamic mechanical properties. To this end, we performed experiments on two model systems as well as molecular dynamics simulations, aiming to determine to what extent widely used shear-distortion models of the reinforcement are applicable as well as the role played by molecular interactions on the enhancement of the mechanical properties. In both experiments and simulations a linear dependence of the reinforcement on the inverse radius of the nanoparticles was obtained. Deformation simulations of a linearly increasing strain showed an overall increase of 50% in the linear modulus when fillers were added to the polymer matrix, regardless of the use of direct interactions among the nanoparticles. Furthermore, the use of attractive nanoparticle interactions resulted in a higher matrix densification at the interfaces and to a sharp increase in the reinforcement.

The non-Newtonian flow behavior of thermal and athermal disordered systems of dispersed uniform particles at high densities have strikingly similar features. By investigating the flow curves of yield-stress fluids and colloidal glasses having different volume fractions, particle sizes, and interactions, we show that both thermal and athermal systems exhibit power-law scaling with respect to the glass and jamming point, respectively, with the same exponents. All yield-stress flow curves can be scaled onto a single universal curve using the Laplace pressure as the stress scale for athermal systems and the osmotic pressure for the thermal systems. Strikingly, the details of interparticle interactions do not matter for the rescaling, showing that they are akin to usual phase transitions of the same universality class. The rescaling allows us to predict the flow properties of these systems from the volume fraction and known material properties.

The free energy of hard-sphere systems provides a direct link between the particle-scale structure and macroscopic thermodynamic properties. Here, we employ this framework to investigate the shear-induced structure of a colloidal glass, and link it to its macroscopic mechanical and thermodynamic state. We measure the nonequilibrium free energy under shear from the free volumes of the particles, and monitor its evolution with the applied strain. Unlike crystals, for which the elastic energy increases quadratically with strain due to affine particle displacements, for glasses the free energy decreases due to non-affine displacements and dissipation, reflecting the ability of the glass to reach deeper free-energy minima. We model this decrease using the nonaffine shear modulus and a standard viscous dissipative term. Our model and measurements allow us to disentangle the complex contributions of affine and nonaffine particle displacements in the transient shear deformation of glasses.

Biopolymer gels such as fibrin and collagen networks are known to develop tensile axial stress when subject to torsion. This negative normal stress is opposite to the classical Poynting effect observed for most elastic solids including synthetic polymer gels, where torsion provokes a positive normal stress. As recently shown, this anomalous behavior in fibrin gels depends on the open, porous network structure of biopolymer gels, which facilitates interstitial fluid flow during shear and can be described by a phenomenological two-fluid model with viscous coupling between network and solvent. Here we extend this model and develop a microscopic model for the individual diagonal components of the stress tensor that determine the axial response of semi-flexible polymer hydrogels. This microscopic model predicts that the magnitude of these stress components depends inversely on the characteristic strain for the onset of nonlinear shear stress, which we confirm experimentally by shear rheometry on fibrin gels. Moreover, our model predicts a transient behavior of the normal stress, which is in excellent agreement with the full time-dependent normal stress we measure., Comment: 12 pages, 8 figures

Homogeneous crystal nucleation from a metastable hard-sphere colloidal liquid has been extensively studied in simulations and experiments. A 12 order of magnitude difference between simulated and experimental nucleation rates is observed, the origin of which remains a puzzle. Here, we experimentally study crystal nucleation at the single particle level in suspensions of hard-sphere-like colloids under the influence of sedimentation. We find that sedimentation significantly enhances the nucleation rate, but contrary to what was previously thought, this is not due to simple density fluctuations, as the nucleation barriers become independent of the local density in a sedimentating fluid. Instead, we find an enhancement of the local dynamics, which suggests that local convective cells are responsible for shear-enhanced crystallization at low volume fractions.

The experimental flow curves of four different yield-stress fluids with different interparticle interactions are studied near the jamming concentration. By appropriate scaling with the distance to jamming all rheology data can be collapsed onto master curves below and above jamming that meet in the shear-thinning regime and satisfy the Herschel-Bulkley and Cross equations, respectively. In spite of differing interactions in the different systems, master curves characterized by universal scaling exponents are found for the four systems. A two-state microscopic theory of heterogeneous dynamics is presented to rationalize the observed transition from Herschel-Bulkley to Cross behavior and to connect the rheological exponents to microscopic exponents for the divergence of the length and time scales of the heterogeneous dynamics. The experimental data and the microscopic theory are compared with much of the available literature data for yield-stress systems.

Understanding the dynamics of direct electrospinning is the key to control fiber morphologies that are critical for the development of new electrospinning methods and novel materials. Here, we propose the theory for direct electrospinning based on theories for (liquid) "rope coiling" and experimentally test it. For the experiments, the buckling of microscale liquid ropes formed from polymer solutions is studied systematically using three different electrospinning setups and for different polymer concentrations. We show that different buckling regimes exist, whose dynamics are governed by an interplay of electrical, inertial, and viscous forces, and that three different buckling regimes emerge depending on the dominant forces. For low polymer concentrations, we observe an inertial regime similar to that observed for viscous liquid ropes at high velocities. By increasing the polymer concentration and consequently decreasing the rope velocity, we enter an inertial-electrical regime for which discontinuities occur in the buckling frequency as a function of applied voltage. These observations can be accounted for quantitatively by replacing the gravitational forces in viscous rope coiling theory with the electrical forces of our electrospinning experiment. Finally, for the highest polymer concentration, we observe a purely electrical regime for a solidified rope; this regime is well described by "elastic" rope coiling theory.

When subjected to shear, granular suspensions exhibit normal stresses perpendicular to the shear plane but the magnitude and sign of the different components of the normal stresses are still under debate. By performing both oscillatory and rotational rheology measurements on shear thickening granular suspensions and systematically varying the particle diameters and the gap sizes between two parallel-plates, we show that a transition from a positive to a negative normal stress can be observed. We find that frictional interactions which determine the shear thickening behavior of suspensions contribute to the positive normal stresses. Increasing the particle diameters or decreasing the gap sizes leads to a growing importance of hydrodynamic interactions, which results in negative normal stresses. We determine a relaxation time for the system, set by both the pore and the gap sizes, that governs the fluid flow through the inter-particle space. Finally, using a two-fluid model we determine the relative contributions from the particle phase and the liquid phase.

We report the observation of the oscillatory and irregular motion of solid spheres settling under the influence of gravity in a thixotropic yield-stress fluid, namely, a suspension of Laponite. The size of the ball and the aging time of the Laponite suspension are found to be two important parameters that determine whether oscillations occur. The irregular motion may be related to the existence of an unstable flow region and shear banding as is concluded from comparisons with rheological measurements, namely, the flow curve and creep tests, using the same Laponite suspensions.

While simple at first glance, the dense packing of sheets is a complex phenomenon that depends on material parameters and the packing protocol. We study the effect of plasticity on the crumpling of sheets of different materials by performing isotropic compaction experiments on sheets of different sizes and elasto-plastic properties. First, we quantify the material properties using a dimensionless foldability index. Then, the compaction force required to crumple a sheet into a ball as well as the average number of layers inside the ball are measured. For each material, both quantities exhibit a power-law dependence on the diameter of the crumpled ball. We experimentally establish the power-law exponents and find that both depend nonlinearly on the foldability index. However the exponents that characterize the mechanical response and morphology of the crumpled materials are related linearly. A simple scaling argument explains this in terms of the buckling of the sheets, and recovers the relation between the crumpling force and the morphology of the crumpled structure. Our results suggest a new approach to tailor the mechanical response of the crumpled objects by carefully selecting their material properties.

Shear thickening of particle suspensions is caused by a transition between lubricated and frictional contacts between the particles. Using three-dimensional (3D) numerical simulations, we study how the interparticle friction coefficient (μm) influences the effective macroscopic friction coefficient (μ) and hence the microstructure and rheology of dense shear thickening suspensions. We propose expressions for μ in terms of distance to jamming for varying shear stresses and μm values. We find μ to be rather insensitive to interparticle friction, which is perhaps surprising but agrees with recent theory and experiments. Unifying behaviors were observed between the average coordination numbers of particles across a wide range of viscous numbers and μm values.

International audience; We study the local and global rheology of non-Brownian suspensions in a solvent that is not density-matched, leading to either creaming or sedimentation of the particles. Both local and global measurements show that the incomplete density matching leads to the appearance of a critical shear rate above which the suspension is homogenized by the flow, and below which sedimentation or creaming happens. We show that the value of the critical shear rate and its dependence on the experimental parameters are governed by a competition between the viscous and the gravitational forces, and present a simple scaling model that agrees with the experimental results from different types of experiments (local and global) in different setups and systems.

International audience; In this study, two types of oscillatory shear rheology are applied on dark chocolate with varying volume fraction, particle size distribution, and soy lecithin concentration. The first, a conventional strain sweep, allows for the separation of the elastic and viscous properties during the yielding. The second, a constant strain rate sweep, where the strain rate amplitude is fixed as the frequency is varied, is analyzed to obtain Lissajous curves, dissipated energy, and higher order nonlinear contributions. It is shown that chocolate exhibits complex nonlinear behavior, namely shear thinning, shear thickening, and strain stiffening. The effects on this behavior related to volume fraction, particle size distribution, and lecithin concentration are investigated, and comparison with simple monodisperse hard-sphere suspensions is made.

We study the process of phase separation of colloid polymer mixtures in the (spinodal) two-phase region of the phase diagram in shear flow. We use a counter-rotating shear cell and image the system by means of confocal laser scanning microscopy. The system is quenched from an initially almost homogeneous state at very high ( 200 s(-1)) shear rate to a low shear rate (gamma)over dot. A spinodal decomposition pattern is observed. Initially, the characteristic length scale increases linearly with time. As the structure coarsens, the shear imposes a certain length scale on the structure and a clear asymmetry develops. The domains become highly stretched along the flow direction, and the domain width along the vorticity axis reaches a stationary size, which scales as approximate to(gamma)over dot(-0.35). Furthermore, on quenching from an intermediate (6.7 s(-1)) to a low shear rate the elongated structures become Rayleigh unstable and break up into smaller droplets. Still, the system eventually reaches the same steady state as was found from a direct high to low shear rate quench through coarsening.

The glass transition is perhaps the greatest unsolved problem in condensed matter physics: the main question is how to reconcile the liquid-like structure with solid-like mechanical properties. In solids, structure and mechanics are related directly through the vibrational density of states of the material. Here, we obtain for the first time the density of states of colloidal glasses and supercooled liquids from a normal-mode analysis of particle displacements measured using confocal microscopy. We find that the spectrum of the (non-linear) vibrations has many ‘soft’, low-frequency modes, more abundant and very different in nature from the usual acoustic vibrations of ordinary solids. This results in an anomalous low-frequency peak in the density of states which approaches zero frequency as one goes deeper into the glass. The observed soft modes are due to collective ‘swirling’ particle motions, that extend over surprisingly long length scales.

In the free-energy landscape picture of glassy systems, their slow dynamics is due to a complicated free-energy landscape with many local minima. We show that for a colloidal glassy material multiple paths can be taken through the free-energy landscape. The evolution of the nonergodicity parameter shows two distinct master curves that we identify as gels and glasses. We show that for a range of colloid concentrations, the transition to nonergodicity can occur in either direction (gel or glass), accompanied by "hesitations" between the two. Thus, colloidal gels and glasses are merely global free-energy minima in the same free-energy landscape, and the paths leading to these minima can be complicated. © 2007 The American Physical Society.

International audience; We study droplet formation in granular suspensions by systematically varying the volume fractions (ϕ) and particle diameters (d). For suspensions with water as the suspending liquid, we find three different regimes. For dilute suspensions (ϕ ≤ 45%), drop formation follows the predictions for inertial breakup and exhibits identical dynamics to that of pure water. The breakup is strongly asymmetrical in this case. Only for more concentrated suspensions (ϕ > 45%) does the presence of particles change the dynamics and two other regimes, a symmetrical inertial regime and a Bagnoldian regime, are uncovered. We construct and discuss a phase diagram that allows us to understand and predict the breakup behavior in granular suspensions.

International audience; Rigid blade coating of glass plates by oil in water emulsions stabilized by surfactants is studied. Complete surface coverage is obtained only for speeds exceeding a threshold velocity dependent on the height between the blade end and the surface. Below this threshold, the emulsion can be inverted in the vicinity of the blade. The inversion dynamics of the oil in water emulsion and the deposition patterns induced by this phase inversion are studied using a microscope mounted set up. We show that these dynamics are universal for different volume fractions and deposition velocities. This inversion as well as the destabilization of the emulsion film deposited at high speeds gives rise to different patterns on the glass surface. These patterns are discussed in terms of the emulsion characteristics as well as the deposition velocity.

International audience; The flow of dry and wet granular media is investigated in a Couette geometry using magnetic resonance imaging in order to test the applicability of the “fluidity model” for nonlocality in these materials. Local volume fraction measurements show that the systems become heterogeneous during flow. We find that the nonlocal rheology of suspensions can be correlated using the fluidity model, but the length scale that emerges is not a material property and the model cannot be used for predictive purposes. Rather, the suspension behavior is fully explained as a consequence of stress-driven particle migration and the resulting concentration gradient. The conclusion is less strong for the dry granular system, but it appears likely that the apparent nonlocal behavior is simply due to the formation of a shear band caused by granular dilatancy.

We study the rheological behavior of concentrated granular suspensions of simple spherical particles. Under controlled stress, the system exhibits an S-shaped flow curve (stress vs. shear rate) with a negative slope in between the low-viscosity Newtonian regime and the shear thickened regime. Under controlled shear rate, a discontinuous transition between the two states is observed. Stress visualization experiments with a novel fluorescent probe suggest that friction is at the origin of shear thickening. Stress visualization shows that the stress in the system remains homogeneous (no shear banding) if a stress is imposed that is intermediate between the high and low-stress branches. The S-shaped shear thickening is then due to the discontinuous formation of a frictional force network between particles upon increasing the stress., 5 pages + 6 figures

We present a comprehensive review of the physical behavior of yield stress materials in soft condensed matter, which encompass a broad range of materials from colloidal assemblies and gels to emulsions and non-Brownian suspensions. All these disordered materials display a nonlinear flow behavior in response to external mechanical forces, due to the existence of a finite force threshold for flow to occur: the yield stress. We discuss both the physical origin and rheological consequences associated with this nonlinear behavior, and give an overview of experimental techniques available to measure the yield stress. We discuss recent progress concerning a microscopic theoretical description of the flow dynamics of yield stress materials, emphasizing in particular the role played by relaxation time scales, the interplay between shear flow and aging behavior, the existence of inhomogeneous shear flows and shear bands, wall slip, and non-local effects in confined geometries., Comment: Review article: V1: 58 pages, 38 figs, 487 refs. V2: Final version 44 pages, 27 figs, 449 refs. Accepted for publication in Rev. Mod. Phys

We study the nonlinear rheological behaviour and the microscopic particle dynamics for a colloidal glass. The measurements allow us to relate the microscopic diffusion dynamics to the macroscopic viscosity of the system. We demonstrate that the competition between the spontaneous restructuration (ageing) and the destruction of the internal structure by the shear ('shear rejuvenation') leads to a bifurcation in rheological behaviour. For a stress smaller than a (time-dependent) critical value, the viscosity increases in time and the material eventually stops flowing. For slightly larger stresses the viscosity decreases continuously with time and the flow accelerates. Thus the viscosity jumps discontinuously to infinity at the critical stress.

We carried out systematic rheometrical tests under controlled stress with smooth and rough parallel disks, along with magnetic resonance imaging (MRI) tests in coaxial cylinder geometry, with foam and a model concentrated emulsion. At low shear stress wall slip appears to occur but the bulk fluid remains static, as proved by the fact that in this regime the apparent shear rate obtained for a given shear stress is inversely proportional to the gap between the disks. At high shear stress data with different surface types and gaps coincide, suggesting that wall slip is negligible in this regime. In parallel, MRI results show that, in contrast with the apparent, simple, yielding behavior observed in usual rheometry, there is an abrupt transition from a finite shear rate to a static one at critical stress. This critical shear rate precisely corresponds to the transition between the two regimes of slip. This suggests that different flow regimes occur with these materials: (1) at low stress, with smooth surfaces a layer of a different material is sheared along the solid surfaces whereas the rest of the fluid does not flow; with rough surfaces there is no flow; (2) beyond a critical stress, for both surface types, the bulk fluid starts to flow but the shear is localized in a thin layer; then the thickness of this layer increases when stress is applied; (3) for both surface types homogeneous flow is obtained only beyond slightly larger stress, which is associated to a critical, apparent shear rate., Des expériences de rhéometrie avec des surfaces lisses et rugueuses ont été réalisées en géométrie plan-plan ainsi que des expériences d'IRM en géométrie à cylindres coaxiaux, sur une mousse et une émulsion concentrée modèle. Aux faibles contraintes un glissement apparaît à proximité du mobile qui induit le cisaillement alors que le reste du matériau demeure immobile. Aux fortes contraintes les données coïncident quelle soit la nature de la surface, ceci nous indiquant que le glissement est négligeable dans ce régime. Un gradient de cisaillement critique correspond précisément à la transition entre ces deux régimes d'écoulement pour les différents types de surface.

We investigate the nonlinear rheological behavior of colloidal suspensions of Laponite, a synthetic clay, driven by a steady and homogeneous shear strain. We show that the external drive leads to a drastic slowing down of the aging dynamics or even, in some cases, in the rejuvenation of the system. Under shear, after a surprisingly long time, the spontaneous aging process observed at rest is suppressed. The system then reaches a non-equilibrium stationary state, characterised by a complex viscosity depending on the applied shear rate. In addition, the glass exhibits a non-Newtonian shear-thinning behavior. These rheological behaviors confirm recent numerical and theoretical predictions., Comment: 17 pages, Latex, 6 figures, figures included in the body of the text, to appear in Journal of Rheology

The Stokes–Einstein (SE) relation is a form of the fluctuation-dissipation theorem (FDT), and relates the diffusion coefficient of colloidal particles to the viscosity via the thermal energy kBT. We study the diffusion coefficient and viscosity of concentrated hard-sphere colloidal model systems in the frequency domain. We show that for these metastable fluid systems strong deviations from the SE relation occur, contrary to predictions of mode coupling theory. Using the FDT, these deviations can be quantified by an effective temperature, Teff. The deviation Teff/T−1 exhibits power-law behavior over several decades in frequency.

A simple mean-field theory is presented which describes the basic observations of recent experiments revealing rich wetting behaviour of n-alkane/methanol mixtures at the liquid-vapour interface. The theory, qualitative and in part heuristic, is based on a microscopic lattice-gas model from which a Cahn–Landau approach is distilled. Besides the physics associated with the short-range components of the intermolecular interactions, effects of the long-range tails of the net van der Waals forces between interfaces are also taken into account. Further, gravitational thinning of the wetting phase is incorporated. The calculation of the spreading coefficient S is extended to the experimentally relevant situation in which the bulk adsorbate is slightly away from two-phase coexistence due to gravity. Analysis of this novel approximation to S for systems with short-range forces leads to the conclusion that the surface specific heat exponents α s =1,1/2, and 0, for first-order wetting, tricritical wetting and critical wetting, respectively, are robust with respect to (weak) gravitational thinning, consistently with experiment. For three different systems the adsorption is calculated as a function of temperature and compared with the experimentally measured ellipticity. Including weak long-range forces which favour wetting in the theory does not visibly alter the critical wetting transition for the nonane/methanol mixture, in contrast with the generic expectation of first-order wetting for such systems, but in good agreement with experiment. For decane/methanol weak long-range forces bring the transition very close to the prewetting critical point, leading to an adsorption behaviour closely reminiscent of short-range tricritical wetting, observed experimentally for alkane chain length between 9.6 and 10. Finally, for undecane/methanol the transition is clearly of first order. First-order wetting is also seen in the experiment.

We study the viscous fingering or Saffman–Taylor instability in two different dilute or semi-dilute polymer solutions. The different solutions exhibit only one non-Newtonian property, in the sense that other non-Newtonian effects can be neglected. The viscosity of solutions of stiff polymers has a strong shear rate dependence. Relative to Newtonian fluids, narrower fingers are found for rigid polymers. For solutions of flexible polymers, elastic effects such as normal stresses are dominant, whereas the shear viscosity is almost constant. Wider fingers are found in this case. We characterize the non-Newtonian flow properties of these polymer solutions completely, allowing for separate and quantitative investigation of the influence of the two most common non-Newtonian properties on the Saffman–Taylor instability. The effects of the non-Newtonian flow properties on the instability can in all cases be understood quantitatively by redefining the control parameter of the instability.

The surfactant sodium bis(2-ethylhexyl) sulphosuccinate (AOT) in water forms lamellar phases at low salinities and sponge phases at higher salinities. For the lowest salinities, the lamellar phase contains many onion defects and is very viscous and elastic. At higher salinities but still in the lamellar phase, the sample has a low viscosity. The sponge phase is a Newtonian fluid with a very low viscosity. When either the low-viscosity lamellar or the sponge phase are sheared, they exhibit a transition, after a long time, to a phase which has the same rheological properties and the same texture as the very viscous lamellar `onion' phase. The random nature of the transition suggests that the formation of the shear-induced phase is due to activated processes, which we discuss here. In addition, the relaxation of the shear-induced phases is very slow; some of its relaxation mechanisms are described.

A mean-field theory is presented which describes the basic observations of recent experiments revealing rich wetting behaviour of n-alkane/methanol mixtures at the liquid-vapour interface. The theory is based on a microscopic lattice-gas model from which a Cahn-Landau phenomenological approach is derived. Besides the physics associated with the short-range components of the intermolecular interactions, the effects of the long-range tails of the net van der Waals forces between interfaces are also taken into account. The tricritical wetting transition, which is featured in the theory when long-range forces are ignored, is replaced by a critical prewetting transition when these forces are included. The experimental observations agree to a large extent with the predictions of the theory for short-range tricritical wetting.

Nanosized filler particles enhance the mechanical properties of polymer composites in a size-dependent fashion. This is puzzling, because classical elasticity is inherently scale-free, and models for the elasticity of composite systems never predict a filler-size dependence. Here, we study the industrially important system of silica-filled rubbers, together with a well-characterized model-filled crosslinked gel and show that at high filler content both the linear and nonlinear elastic properties of these systems exhibit a unique scaling proportional to the cube of the volume fraction divided by the particle size. This remarkable behavior makes it possible to predict the full mechanical response of particle-filled rubbers for small but finite deformations based solely on the rheology of the matrix and the size and modulus of the filler particles.

We report a shear-induced sponge (L3) to lamellar (L(alpha)) transition in a surfactant system. Under a constant shear rate, after a delay time t(n) we observe random nucleation and subsequent growth of the L(alpha) phase, demonstrating that the shear-induced transition is first order. A simple argument for the energy of a two-dimensional nucleus accounts for the observed delay and its shear-rate dependence.

We study the Saffman-Taylor or viscous fingering instability in yield stress fluids. The theory for yield stress fluids shows that the dispersion equation of the instability is similar to that for Newtonian fluids; however, the capillary number governing the instability now contains the yield stress. Experiments using gels and foams reveal very branched fingers in the gel. The results are in excellent agreement with theory for the gel, with, in addition, a crossover from yield stress dominated to viscous behavior. The results for foams are very different due to the existence of wall slip.

Viscous fingers form when a less viscous fluid pushes a more viscous fluid in a linear channel. The instability of the interface results from a competition between viscous and capillary forces. We show here that by using complex fluids such as polymer or surfactant solutions one can act on the viscosity or the surface tension and modify the instability drastically. Two different polymer solutions, that exhibit either shear thinning or normal stress effects, are used. For the first fluid the viscous forces are altered leading to finger narrowing, whereas for the second fluid the viscous forces are supplemented by normal stresses, which leads to finger widening. For the surfactant solutions the modification of the capillary forces leads to finger widening.

We study the Saffman–Taylor instability in a rectangular Hele-Shaw cell. The driven fluid is a dilute (or semidilute) polymer solution, with a viscosity that exhibits shear thinning. Other non-Newtonian properties such as elastic effects are negligible under the present experimental conditions; the system thus allows for separate investigation of the influence of shear thinning on the instability. The experiments show that, for weak shear-thinning, the results for the width of the fingers as a function of the capillary number collapse onto the universal curve for Newtonian fluids, provided the shear-thinning viscosity is used to calculate the capillary number. For stronger shear thinning, narrower fingers are found. The experiment allows also for a study of the applicability of Darcy’s law to shear thinning fluids. For Newtonian fluids, this law gives the finger velocity as a function of the pressure gradient. For weakly shear-thinning fluids, we find that an effective Darcy’s law, in which the constant v...

The flow deformation and rheology of vesicles of a soluble surfactant are studied. Direct observation under shear flow reveals that the vesicles become strongly elongated to form an entangled structure of connected bilayer tubes. The large deformation is due to the permeability of the membrane and the large solubility of the surfactant. The formation of the entangled structure is observed in the rheology as a strong increase of the viscosity with time.

We study the rheological properties of self-assembled surfactant structures: lyotropic liquid crystals exhibiting plane lamellar and ‘‘onion’’ ~concentric bilayer! textures. Both systems behave similarly: they are gel-like and exhibit extreme shear-thinning behavior. We demonstrate that this results in a hysteresis in the stress-strain curve when the stress is imposed. Controlled shear-rate experiments reveal the origin of the hysteresis by demonstrating the existence of two extrema in the stress-strain curve. The bistability leads to the formation of shear bands in the system and is illustrated by demonstrating the existence of sudden jumps in the viscosity of the fluid, following the viscosity of the fluid in time. @S1063-651X~98!01208-2#

We study stable and metastable surface states in adsorbed liquid mixtures from the point of view of classical nucleation theory. We propose an interpretation of recent measurements of the lifetime of metastable thin wetting films, invoking the existence of a surface spinodal. A preliminary account of this work is to be found in D. Bonn and J.O. Indekeu, Phys. Rev. Lett. 74 , 3844 (1995).

International audience; We show experimentally that the sliding friction on sand is greatly reduced by the addition of some—but not too much—water. The formation of capillary water bridges increases the shear modulus of the sand, which facilitates the sliding. Too much water, on the other hand, makes the capillary bridges coalesce, resulting in a decrease of the modulus; in this case, we observe that the friction coefficient increases again. Our results, therefore, show that the friction coefficient is directly related to the shear modulus; this has important repercussions for the transport of granular materials. In addition, the polydispersity of the sand is shown to also have a large effect on the friction coefficient. DOI

International audience; We study the pinch-off dynamics of droplets of yield stress and shear thinning fluids. To separate the two non-Newtonian effects, we use a yield stress material for which the yield stress can be tuned without changing the shear thinning behavior, and a shear thinning system (without a yield stress) for which the shear thinning can be controlled over a large range, without introducing too much elasticity into the system. We find that the pinch-off remains very similar to that of constant viscosity Newtonian liquids, and consequently thinning in shear flow does not imply a thinning in elongational flow.