arXiv subjects

Laurence Ramos

Publications and source records attributed to Laurence Ramos.

At least 37 records · Page 2Linked to original sources

arXiv2016

Rearrangement zone around a crack tip in a double self-assembled transient network

We investigate the nucleation and propagation of cracks in self-assembled viscoelastic fluids, which are made of surfactant micelles reversibly linked by telechelic polymers. The morphology of the micelles can be continuously tuned, from spherical to rod-like to wormlike, thus producing transient double networks when the micelles are sufficiently long and entangled, and transient single networks otherwise. For a single network, we show that cracks nucleate when the sample deformation rate involved is comparable to the relaxation time scale of the network. For a double network, by contrast, significant rearrangements of the micelles occur as a crack nucleates and propagates. We show that birefringence develops at the crack tip over a finite length, $ξ$, which corresponds to the length scale over which micelles alignment occur. We find that $ξ$ is larger for slower cracks, suggesting an increase of ductility.

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arXiv2015

Bursting of Dilute Emulsion-Based Liquid Sheets Driven by a Marangoni Effect

We study the destabilization mechanism of thin liquid sheets expanding in air and show that dilute oil-in-water emulsion-based sheets disintegrate through the nucleation and growth of holes that perforate the sheet. The velocity and thickness fields of the sheet outside the holes are not perturbed by holes and hole opening follows a Taylor-Culick law. We find that a pre-hole, which widens and thins out the sheet with time, systematically precedes the hole nucleation. The growth dynamics of the pre-hole follows the law theoretically predicted for a liquid spreading on another liquid of higher surface tension due to Marangoni stresses. Classical Marangoni spreading experiments quantitatively corroborate our findings.

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arXiv2015

Viscoelasticity of colloidal polycrystals doped with impurities

We investigate how the microstructure of a colloidal polycrystal influences its linear viscoelasticity. We use thermosensitive copolymer micelles that arrange in water in a cubic crystalline lattice, yielding a colloidal polycrystal. The polycrystal is doped with a small amount of nanoparticles, of size comparable to that of the micelles, which behave as impurities and thus partially segregate in the grain boundaries. We show that the shear elastic modulus only depends on the packing of the micelles and does not vary neither with the presence of nanoparticles nor with the crystal microstructure. By contrast, we find that the loss modulus is strongly affected by the presence of nanoparticles. A comparison between rheology data and small-angle neutron scattering data suggests that the loss modulus is dictated by the total amount of nanoparticles in the grain boundaries, which in turn depends on the sample microstructure.

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arXiv2015

Spontaneous gelation of wheat gluten proteins in a food grade solvent

Structuring wheat gluten proteins into gels with tunable mechanical properties would provide more versatility for the production of plant protein-rich food products. Gluten, a strongly elastic protein material insoluble in water, is hardly processable. We use a novel fractionation procedure allowing the isolation from gluten of a water/ethanol soluble protein blend, enriched in glutenin polymers at an unprecedented high ratio (50%). We investigate here the viscoelasticity of suspensions of the protein blend in a water/ethanol (50/50 v/v) solvent, and show that, over a wide range of concentrations, they undergo a spontaneous gelation driven by hydrogen bonding. We successfully rationalize our data using percolation models and relate the viscoelasticity of the gels to their fractal dimension measured by scattering techniques. The gluten gels display self-healing properties and their elastic plateaus cover several decades, from 0.01 to 10000 Pa. In particular very soft gels as compared to standard hydrated gluten can be produced.

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arXiv2014

Free radially expanding liquid sheet in air: time- and space-resolved measurement of the thickness field

The collision of a liquid drop against a small target results in the formation of a thin liquid sheet that extends radially until it reaches a maximum diameter. The subsequent retraction is due to the air-liquid surface tension. We have used a time- and space-resolved technique to measure the thickness field of this class of liquid sheet, based on the grey level measurement of the image of a dyed liquid sheet recorded using a fast camera. This method enables a precise measurement of the thickness in the range $(10-450) \, \mathrm{μm}$, with a temporal resolution equal to that of the camera. We have measured the evolution with time since impact, $t$, and radial position, $r$, of the thickness, $h(r,t)$, for various drop volumes and impact velocities. Two asymptotic regimes for the expansion of the sheet are evidenced. The scalings of the thickness with $t$ and $r$ measured in the two regimes are those that were predicted in \citet{Rozhkov2004} fort the short-time regime and \citet{Villermaux2011} for the long time regime, but never experimentally measured before. Interestingly, our experimental data also evidence the existence of a maximum of the film thickness $h_{\rm{max}}(r)$ at a radial position $r_{\rm{h_{max}}}(t)$ corresponding to the crossover of these two asymptotic regimes. The maximum moves with a constant velocity of the order of the drop impact velocity, as expected theoretically. Thanks to our visualization technique, we also evidence an azimuthal thickness modulation of the liquid sheets.

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arXiv2014

Polymeric Assembly of Gluten Proteins in an Aqueous Ethanol Solvent

The supramolecular organization of wheat gluten proteins is largely unknown due to the intrinsic complexity of this family of proteins and their insolubility in water. We fractionate gluten in a water/ethanol (50/50 v/v) and obtain a protein extract which is depleted in gliadin, the monomeric part of wheat gluten proteins, and enriched in glutenin, the polymeric part of wheat gluten proteins. We investigate the structure of the proteins in the solvent used for extraction over a wide range of concentration, by combining X-ray scattering and multi-angle static and dynamic light scattering. Our data show that, in the ethanol/water mixture, the proteins display features characteristic of flexible polymer chains in a good solvent. In the dilute regime, the protein form very loose structures of characteristic size 150 nm, with an internal dynamics which is quantitatively similar to that of branched polymer coils. In more concentrated regimes, data highlight a hierarchical structure with one characteristic length scale of the order of a few nm, which displays the scaling with concentration expected for a semi-dilute polymer in good solvent, and a fractal arrangement at much larger length scale. This structure is strikingly similar to that of polymeric gels, thus providing some factual knowledge to rationalize the viscoelastic properties of wheat gluten proteins and their assemblies.

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arXiv2014

Plasticity of a colloidal polycrystal under cyclic shear

We use confocal microscopy and time-resolved light scattering to investigate plasticity in a col- loidal polycrystal, following the evolution of the network of grain boundaries as the sample is submitted to thousands of shear deformation cycles. The grain boundary motion is found to be ballistic, with a velocity distribution function exhibiting non-trivial power law tails. The shear- induced dynamics initially slow down, similarly to the aging of the spontaneous dynamics in glassy materials, but eventually reach a steady state. Surprisingly, the cross-over time between the ini- tial aging regime and the steady state decreases with increasing probed length scale, hinting at a hierarchical organization of the grain boundary dynamics.

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arXiv2013

Fingering to fracturing transition in a transient gel

Fracture processes are ubiquitous in soft materials, even in complex fluids, subjected to stresses. To investigate these processes in a simple geometry, we use a model self-assembled transient gel and study the instability patterns obtained in a radial Hele-Shaw cell when a low viscosity oil pushes the more viscous transient gel. Thanks to an analysis of the morphology of the patterns, we find a discontinuous transition between the standard Saffman-Taylor fingering instability and a fracturing instability as the oil injection rate increases. Our data suggest that the flow properties of the gel ahead of the finger tip controls the transition towards fracturing. By analyzing the displacement field of the gel in the vicinity of the fingers and cracks, we show that in the fingering regime, the oil gently pushes the gel, whereas in the fracturing regime, the crack tears apart the gel, resulting in a strong drop of the gel velocity ahead of the crack tip as compared to the tip velocity. We find a unique behavior for the whole displacement field of a gel around a crack, which is drastically different from that around a finger, and reveals the solid-like behavior of the gel at short time. Our experiments and analysis provide quantitative yet simple tools to unambiguously discriminate a finger from a crack in a visco-elastic material.

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arXiv2012

Tuning the porosity of bimetallic nanostructures by a soft templating approach

We use hexagonal mesophases made of oil-swollen surfactant-stabilized tubes arranged on a triangular lattice in water and doped with metallic salts as templates for the radiolytic synthesis of nanostructures. The nanostructures formed in this type of soft matrix are bimetallic palladium-platinum porous nanoballs composed of 3D-connected nanowires, of typical thickness 2.5 nm, forming hexagonal cells. We demonstrate using electron microscopy and small-angle X-ray scattering that the pore size of the nanoballs is directly determined by the diameter of the oil tube of the doped mesophases, which we have varied in a controlled fashion from 10 to 55 nm. Bimetallic nanostructures comprising various proportions of palladium and platinum can be synthesized. Their alloy structure was evidenced by X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy, and high-angular dark field scanning transmission electron microscopy experiments. Our templating approach allows therefore the synthesis of bimetallic nanoballs of tunable porosity and composition.

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arXiv2012

Structure of nanoparticles embedded in micellar polycrystals

We investigate by scattering techniques the structure of water-based soft composite materials comprising a crystal made of Pluronic block-copolymer micelles arranged in a face-centered cubic lattice and a small amount (at most 2% by volume) of silica nanoparticles, of size comparable to that of the micelles. The copolymer is thermosensitive: it is hydrophilic and fully dissolved in water at low temperature (T ~ 0°C), and self-assembles into micelles at room temperature, where the block-copolymer is amphiphilic. We use contrast matching small-angle neuron scattering experiments to probe independently the structure of the nanoparticles and that of the polymer. We find that the nanoparticles do not perturb the crystalline order. In addition, a structure peak is measured for the silica nanoparticles dispersed in the polycrystalline samples. This implies that the samples are spatially heterogeneous and comprise, without macroscopic phase separation, silica-poor and silica-rich regions. We show that the nanoparticle concentration in the silica-rich regions is about tenfold the average concentration. These regions are grain boundaries between crystallites, where nanoparticles concentrate, as shown by static light scattering and by light microscopy imaging of the samples. We show that the temperature rate at which the sample is prepared strongly influence the segregation of the nanoparticles in the grain-boundaries.

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arXiv2012

Grain refinement and partitioning of impurities in the grain boundaries of a colloidal polycrystal

We study the crystallization of a colloidal model system in presence of secondary nanoparticles acting as impurities. Using confocal microscopy, we show that the nanoparticles segregate in the grain boundaries of the colloidal polycrystal. We demonstrate that the texture of the polycrystal can be tuned by varying independently the nanoparticle volume fraction and the crystallization rate, and quantify our findings using standard models for the nucleation and growth of crystalline materials. Remarkably, we find that the efficiency of the segregation of the nanoparticles in the grain-boundaries is determined solely by the typical size of the crystalline grains.

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arXiv2012

Structural Signature of a Brittle-to-Ductile Transition in Self-Assembled Networks

We study the nonlinear rheology of a novel class of transient networks, made of surfactant micelles of tunable morphology reversibly linked by block copolymers. We couple rheology and time-resolved structural measurements, using synchrotron radiation, to characterize the highly nonlinear viscoelastic regime. We propose the fluctuations of the degree of alignment of the micelles under shear as a probe to identify a fracture process. We show a clear signature of a brittle-to-ductile transition in transient gels, as the morphology of the micelles varies, and provide a parallel between the fracture of solids and the fracture under shear of viscoelastic fluids.

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arXiv2008

Copolymer-induced stabilizing effect of highly swollen hexagonal mesophases

We show quantitatively that tiny amounts of copolymer that decorate a oil/water interfaces can greatly enhance the stability of swollen surfactant hexagonal phases, comprising oil tubes regularly arranged in a water matrix. Such soft composite materials, whose both radius of the tubes and water channel between the tubes can be controlled independently over large ranges, offer a potential interest for the synthesis of mesoporous materials.

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arXiv2008

Direct-space investigation of the ultraslow ballistic dynamics of a soft glass

We use light microscopy to investigate the aging dynamics of a glass made of closely packed soft spheres, following a rapid transition from a fluid to a solid-like state. By measuring time-resolved, coarse-grained displacements fields, we identify two classes of dynamical events, corresponding to reversible and irreversible rearrangements, respectively. The reversible events are due to the small, experimentally unavoidable fluctuations of the temperature imposed to the sample, leading to transient thermal expansions and contractions that cause shear deformations. The irreversible events are plastic rearrangements, induced by the repeated shear cycles. We show that the displacement due to the irreversible rearrangements grows linearly with time, both on average and at a local level. The velocity associated with this ballistic motion decreases exponentially with sample age, accounting for the observed slowing down of the dynamics. The displacement field due to the irreversible rearrangements has a vortex-like structure and is spatially correlated over surprisingly long distances.

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arXiv2007

Investigation of $q$-dependent dynamical heterogeneity in a colloidal gel by x-ray photon correlation spectroscopy

We use time-resolved X-Photon Correlation Spectroscopy to investigate the slow dynamics of colloidal gels made of moderately attractive carbon black particles. We show that the slow dynamics is temporally heterogeneous and quantify its fluctuations by measuring the variance $χ$ of the instantaneous intensity correlation function. The amplitude of dynamical fluctuations has a non-monotonic dependence on scattering vector $q$, in stark contrast with recent experiments on strongly attractive colloidal gels [Duri and Cipelletti, \textit{Europhys. Lett.} \textbf{76}, 972 (2006)]. We propose a simple scaling argument for the $q$-dependence of fluctuations in glassy systems that rationalizes these findings.

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arXiv2007

Real-time observation of polyelectrolyte-induced binding of charged bilayers

We present real-time observations by confocal microscopy of the dynamic behavior of multilamellar vesicles (MLVs), composed of charged synthetic lipids, when put in contact with oppositely charged polyelectrolyte (PE) molecules. We find that the MLVs exhibit astonishing morphological transitions, which result from the discrete and progressive binding of the charged bilayers induced by a high PE concentration gradient. Our physical picture is confirmed by quantitative measurements of the fluorescence intensity as the bilayers bind to each other. The shape transitions lead eventually to the spontaneous formation of hollow capsules, whose thick walls are composed of lipid multilayers condensed with PE molecules. This class of objects may have some (bio)technological applications.

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arXiv2007

Linear viscoelasticity of entangled wormlike micelles bridged by telechelic polymers : an experimental model for a double transient network

We survey the linear viscoelasticity of a new type of transient network: bridged wormlike micelles, whose structure has been characterized recently [Ramos and Ligoure, (2007)]. This composite material is obtained by adding telechelic copolymers (water-soluble chains with hydrophobic stickers at each extremity) to a solution of entangled wormlike micelles (WM). For comparison, naked WM and WM decorated by amphiphilic copolymers are also investigated. While these latter systems exhibit almost a same single ideal Maxwell behavior, solutions of bridged WM can be described as two Maxwell fluids components blends, characterized by two markedly different characteristic times, t_fast and t_slow, and two elastic moduli, G_fast and G_slow, with G_fast >> G_slow. We show that the slow mode is related to the viscoelasticity of the transient network of entangled WM, and the fast mode to the network of telechelic active chains (i.e. chains that do not form loops but bridge two micelles). The dependence of the viscoelasticity with the surfactant concentration, phi, and the sticker-to-surfactant molar ratio, beta, is discussed. In particular, we show that G_fast is proportional to the number of active chains in the material, phi beta. Simple theoretical expectations allow then to evaluate the bridges/loops ratio for the telechelic polymers.

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arXiv2006

Origin of the slow dynamics and the aging of a soft glass

We study by light microscopy a soft glass consisting of a compact arrangement of polydisperse elastic spheres. We show that its slow and non-stationary dynamics results from the unavoidable small fluctuations of temperature, which induce intermittent local mechanical shear in the sample, because of thermal expansion and contraction. Temperature-induced shear provokes both reversible and irreversible rearrangements whose amplitude decreases with time, leading to an exponential slowing down of the dynamics with sample age.

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