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The antagonistic effect of processing and thermal annealing on both the filler structure and the polymer matrix is explored in polymer nanocomposites based on natural rubber with precipitated silica incorporated by coagulation from aqueous suspension followed by roll-milling. Their structure and linear and non-linear rheology have been studied, with a particular emphasis on the effect of high-temperature thermal treatment and the number of milling passes. Small-angle X-ray scattering intensities show that the silica is organized in small, unbreakable aggregates containing ca. 50 primary nanoparticles, which are reorganized on a larger scale in filler networks percolating at the highest silica contents. As expected, the filler network structure is found to be sensitive to milling, more milling inducing rupture, as evidenced by the decreasing Payne effect. After thermal treatment, the nanocomposite structure is found to be rejuvenated, erasing the effect of the previous milling on the low-strain modulus. In parallel, the dynamics of the samples described by the rheology or the calorimetric glass-transition temperature remain unchanged, whereas the natural latex polymer network structure is modified by milling towards a more fluid-like rheology, and cannot be recovered.

International audience; A novel and simple method for the measurement of cloud point temperatures of solutions is presented. Cloud point determination , which is currently used to establish the phase diagrams of protein solutions, is indicative of proteins interactions and constitutes a useful tool for food products engineering. We describe a novel experimental setup that allows screening of a large number of physical-chemical conditions in one measurement and the determination of cloud point temperatures both above and below ambient temperature. We use a simple method to avoid solvent evaporation and condensation, so that the setup can be used for solutions prepared with a volatile solvent. We present the operating parameter range and the precision of the measurement. The optical properties of the system are calibrated with solutions of known transmittance, and the determination of cloud point temperatures is validated on a standard non-ionic surfactant solution. Finally, we demonstrate the efficiency of the method by determining the phase diagram of a wheat protein extract, soluble in a water/ethanol mixture. Complemented with differential scanning calorimetry measurements, the liquid-liquid phase transition can be determined up to a protein concentration of 250 g/L, a range inaccessible with conventional methods for this protein extract.

International audience; Deformations of heavy elastic cylinders with their axis in the direction of earth's gravity field are investigated. The specimens, made of polyacrylamide hydrogels, are attached from their top circular cross section to a rigid plate. An equilibrium configuration results from the interplay between gravity that tends to deform the cylinders downwards under their own weight, and elasticity that resists these distortions. The corresponding steady state exhibits fascinating shapes which are measured with lab-based micro-tomography. For any given initial radius to height ratio, the deformed cylinders are no longer axially symmetric beyond a critical value of a control parameter that depends on the volume force, the height and the elastic modulus: self-similar wrinkling hierarchies develop, and dimples appear at the bottom surface of the shallowest samples. We show that these patterns are the consequences of elastic instabilities.

International audience; We investigate the non-linear buckling patterns produced by the elastic Rayleigh-Taylor instability in a hyper-elastic slab hanging below a rigid horizontal plane, using a combination of experiments, weakly non-linear expansions and numerical simulations. Our experiments reveal the formation of hexagonal patterns through a discontinuous transition. As the unbuckled state is transversely isotropic, a continuum of linear modes become critical at the first bifurcation load: the critical wavevectors form a circle contained in a horizontal plane. Using a weakly non-linear post-bifurcation expansion, we investigate how these linear modes cooperate to produce buckling patterns: by a mechanism documented in other transversely isotropic structures, three-modes coupling make the unbuckled configuration unstable with respect to hexagonal patterns by a transcritical bifurcation. Stripe and square patterns are solutions of the post-bifurcation expansion as well but they are unstable near the threshold. These analytical results are confirmed and complemented by numerical simulations.

We investigate freely expanding sheets formed by ultrasoft gel beads, and liquid and viscoelastic drops, produced by the impact of the bead or drop on a silicon wafer covered with a thin layer of liquid nitrogen that suppresses viscous dissipation thanks to an inverse Leidenfrost effect. Our experiments show a unified behaviour for the impact dynamics that holds for solids, liquids, and viscoelastic fluids and that we rationalize by properly taking into account elastocapillary effects. In this framework, the classical impact dynamics of solids and liquids as far as viscous dissipation is negligible, appears as the asymptotic limits of a universal theoretical description. A novel material-dependent characteristic velocity that includes both capillary and bulk elasticity emerges from this unified description of the physics of impact., Comment: to appear in PRL

Subcritical crack growth and crack closure are analysed using the double cleavage drilled compression method, in two calcium phosphate-based glasses. The measurements of the crack velocity as a function of temperature, from ambient to 250 °C, are reported for two different relative humidity levels. Studied glasses present unusual trends characterized by a non-gradual shift of V–K I curves versus temperature. Moreover, when the load is released and crack closes, expulsion of a “liquid-like” phase is observed forming droplets along the crack path. These droplets are only formed at certain temperatures, but both under high and low water humidity. They evolve towards residues when temperature is decreased.

We develop and thoroughly test a stress-controlled, parallel plates shear cell that can be coupled to an optical microscope or a small angle light scattering setup, for simultaneous investigation of the rheological properties and the microscopic structure of soft materials under an imposed shear stress. In order to minimize friction, the cell is based on an air bearing linear stage, the stress is applied through a contactless magnetic actuator, and the strain is measured through optical sensors. We discuss the contributions of inertia and of the small residual friction to the measured signal and demonstrate the performance of our device in both oscillating and step stress experiments on a variety of viscoelastic materials., 14 pages, 10 figures

Blood viscosity decreases with shear stress, a property essential for an efficient perfusion of the vascular tree. Shear thinning is intimately related to the dynamics and mutual interactions of RBCs, the major component of blood. Because of the lack of knowledge about the behavior of RBCs under physiological conditions, the link between RBC dynamics and blood rheology remains unsettled. We performed experiments and simulations in microcirculatory flow conditions of viscosity, shear rates, and volume fractions, and our study reveals rich RBC dynamics that govern shear thinning. In contrast to the current paradigm, which assumes that RBCs align steadily around the flow direction while their membranes and cytoplasm circulate, we show that RBCs successively tumble, roll, deform into rolling stomatocytes, and, finally, adopt highly deformed polylobed shapes for increasing shear stresses, even for semidilute volume fractions of the microcirculation. Our results suggest that any pathological change in plasma composition, RBC cytosol viscosity, or membrane mechanical properties will affect the onset of these morphological transitions and should play a central role in pathological blood rheology and flow behavior.

The Continuous Droplet Interface Crossing Encapsulation (cDICE) is an easy and robust method for producing, at high yield, monodisperse lipid vesicles with a controlled content as well as capsules with a designed shell. It consists in forcing a droplet through an interface between two imiscible fluids, using an external force such as centrifugation. At high inertia, the droplet entrain fluid that will constitute the shell of the capsule. At low inertia, the presence of amphiphile and the deformable interface interactions lead to monolayers zipping and formation of an amphiphile bilayer around the droplet. We will discuss the physical mechanisms involved in the production of both cDICE vesicles (low droplets inertia) and capsules (at high inertia), and the potential applications of this method. This method founds indeed many applications in biomimetics as it allows to encapsulate various biological solutions (biopolymers, hemoglobin, colloids, polymeric gels, cells. . . ) in membranes that can be composite and/or assymetric, or polymeric, and in the field of microencapsulation.

We use Photon Correlation Imaging, a recently introduced space-resolved dynamic light scattering method, to investigate the spatial correlation of the dynamics of a variety of jammed and glassy soft materials. Strikingly, we find that in deeply jammed soft materials spatial correlations of the dynamics are quite generally ultra-long ranged, extending up to the system size, orders of magnitude larger than any relevant structural length scale, such as the particle size, or the mesh size for colloidal gel systems. This has to be contrasted with the case of molecular, colloidal and granular ``supercooled'' fluids, where spatial correlations of the dynamics extend over a few particles at most. Our findings suggest that ultra long range spatial correlations in the dynamics of a system are directly related to the origin of elasticity. While solid-like systems with entropic elasticity exhibit very moderate correlations, systems with enthalpic elasticity exhibit ultra-long range correlations due to the effective transmission of strains throughout the contact network., Comment: To appear in Soft Matter

International audience; We demonstrate the instability of the free surface of a soft elastic solid facing downwards. Experiments are carried out using a gel of constant density rho, shear modulus mu, put in a rigid cylindrical dish of depth h. When turned upside down, the free surface of the gel undergoes a normal outgoing acceleration g. It remains perfectly flat for rhogh/mu

Under the effect of surface tension, a blob of liquid adopts a spherical shape when immersed in another fluid. We demonstrate experimentally that soft, centimeter-size elastic solids can exhibit a similar behavior: when immersed into a liquid, a gel having a low elastic modulus undergoes large, reversible deformations. We analyze three fundamental types of deformations of a slender elastic solid driven by surface stress, depending on the shape of its cross section: a circular elastic cylinder shortens in the longitudinal direction and stretches transversally; the sharp edges of a square based prism get rounded off as its cross sections tend to become circular; and a slender, triangular based prism bends. These experimental results are compared to analysis and nonlinear simulations of neo-Hookean solids deformed by surface tension and are found to be in good agreement with each other.

We report the observation of a Plateau instability in a thin filament of solid gel with a very small elastic modulus. A longitudinal undulation of the surface of the cylinder reduces its area thereby triggering capillary instability, but is counterbalanced by elastic forces following the deformation. This competition leads to a nontrivial instability threshold for a solid cylinder. The ratio of surface tension to elastic modulus defines a characteristic length scale. The onset of linear instability is when the radius of the cylinder is one-sixth of this length scale, in agreement with theory presented here.