We investigate by time-resolved synchrotron ultra-small X-ray scattering the dynamics of liquid–liquid phase-separation (LLPS) of gluten protein suspensions following a temperature quench. Samples at a fixed concentration (237 mg ml−1) but with different protein compositions are investigated. In our experimental conditions, we show that fluid viscoelastic samples depleted in polymeric glutenin phase-separate following a spinodal decomposition process. We quantitatively probe the late stage coarsening that results from a competition between thermodynamics that speeds up the coarsening rate as the quench depth increases and transport that slows down the rate. For even deeper quenches, the even higher viscoelasticity of the continuous phase leads to a “quasi” arrested phase separation. Anomalous phase-separation dynamics is by contrast measured for a gel sample rich in glutenin, due to elastic constraints. This work illustrates the role of viscoelasticity in the dynamics of LLPS in protein dispersions.

We show that compressive sensing (CS) calculations are very ecient to reconstruct in 3D sparse objects whose 2D hologram has been recorded by digital holographic microscopy. The method is well adapted to image small scattering objects moving within a larger motionless object. This situation corresponds to red blood cells (RBCs) circulating in the vascular system of a zebrash (Danio rerio) larva. RBCs positions are imaged in 3D from a single hologram, while the RBCs trajectories, i.e. the perfused blood vessels, are imaged from a sequence of holograms. With respect to previous work (Donnarumma et al., Opt. express, 24, 26887, 2016), we get a gain of ∼ 500 in calculation speed.

Natural protein sources often display a huge complexity, being composed of a blend of polypeptides of various molecular weight, pHi and charge density. Gluten, the proteins extracted from wheat flour is one of such. Gluten is widely used for its viscoelastic properties as an improver of cereal products (bread, pastry, etc.). It is composed of two classes of proteins, named gliadin and glutenin, similar in their amounts in glutamine (30%) and proline (10%). The more than 25 different polypeptides belonging to the gliadin class are hard to fractionate into individual components because of high redundancy in the primary sequences. Glutenin are in the form of polymers made from several distinct polypeptides concatenated through inter-chain disulfide bonds. Their molecular weights are evenly distributed from 100 kg/mol to 7,000 kg/mol.While it is well established that gliadin confers viscosity to gluten whereas glutenin polymers are at the origin of its elastic resistance, the interactions existing between both classes of gluten protein remain unknown. We previously showed by SLS and multi-angle DLS that gluten proteins suspended in ethanol/water (50/50, v/v), a theta solvent, includes large proteins assemblies (26,000 kg/mol, Rh 100nm) displaying an internal dynamic1. To get a better insight of the composition of those assemblies, we combined biochemical and physicochemical approaches. On the one hand, gluten proteins suspended in ethanol/water were fractionated by Asymmetrical- Flow-Field-Flow Fractionation (A4F) coupled to UV, SLS and QELS detectors. On the other hand, gluten proteins were partitioned by liquid-phase decomposition in respect with temperature. Protein composition of partitioned phases and eluting fractions recovered from A4F were characterized by size-exclusion chromatography. A specific interaction between omega-gliadin and glutenin polymers was evidenced.This result strengthens a very recent study that demonstrates a significant positive correlation between glutenin polymeric proteins, the ω‐gliadin fraction, and dough properties.

A combined small-angle scattering of neutrons (SANS) and X-rays (SAXS) study of thestructure of polymer layers pre-adsorbed on silica nanoparticles (NP) which are subsequentlyincorporated into polymer nanocomposites (PNCs) is presented. Pre-adsorbed chains are foundto promote ideal dispersion, before desorption in the late stages of nanocomposite formation.The microstructure of the interfacial polymer layer is characterized by detailed modeling of X-rayand neutron scattering. Only in ideally well-dispersed systems a static interfacial layer ofreduced polymer density over a thickness of ca. 2 nm is evidenced based on the analysis with aform-free density profile optimized using reverse Monte Carlo simulations. This interfacialgradient layer is found to be independent of the thickness and mass of the initially adsorbedpolymer, but appears to be generated by out-of-equilibrium packing and folding of the preadsorbedlayer. The impact of annealing is investigated to study the approach of equilibrium,showing that initially ideally well-dispersed systems adopt a repulsive hard-sphere structure,while the static interfacial layer disappears.In parallel, SANS and the use of zero average contrast conditions allow the measurement ofchain conformation in the PNCs with and without pre-adsorption. Surprisingly, we evidenced thespontaneous formation of thermally-stable adsorbed layers in PNCs containing matrix chains ofdifferent mass, whereas a symmetric matrix of identical chain masses does not show this effect.This study contributes thus to the fundamental understanding of the interplay betweeneffects which are decisive for macroscopic material properties: polymer-mediated interparticleinteractions, and particle interfacial effects on surrounding polymer.

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.

Despite the relevance to environmental, biological and industrial processes, the motion of a colloidal particle close to a fluid interface and the way it interacts with the water surface are still largely elusive and intriguing physical phenomena.We explored the system of individual colloidal particles close to an air-water interface by recording highly resolved 3D trajectories through a dual wave reflection interference setup (DW-RIM). Contrary to other established experimental techniques, DW-RIM allows accurate measurements of the absolute particle-interface distance and thus does not require any calibration or assumption to know the location of the interface. The particle-interface system shows two different potential energy landscapes resulting to two different equilibrium particle-interface distances. The larger one can be fairly explained by Van der Waals and electrostatic interactions combined with gravity. The shorter one highlights the existence of an unexpected additional attractive interaction. Surface heterogeneities as possible origin of such an interaction are considered and discussed.Concerning the friction the particle undergoes, the air-water interface peculiarly acts as a slip boundary for the particle motion parallel to the interface and as a no-slip boundary for the perpendicular motion. This experimental result is rationalized considering recent models based on surface incompressibility.

To date, aqueous stable graphene flakes solutionscan be obtained by simple REDOX reactions.1–5 Most of the current applications regardinggraphene require ordered nanostructuredcomposites materials. Liquid crystal phases orderingrepresent an opportunity to arrange theminto macroscopic assemblies with long-rangeordering. 1,2 Preparing organized materials andthin films from these dispersions then requires agood control of the liquid crystal ordering duringthe deposition and the drying of the films. As amatter of fact, it turns out that graphene flakeseasily align at high shear.3,4 On the other hand,Graphene Flakes Liquid Crystals (GFLC) exhibita very interesting behaviour at low shear or undersmall displacements, thin films often showspeculiar patterns (such as the periodic texturesshown in Fig.72-72). We have shown how tocreate and stabilize large-sized periodic texturesin GFLC. The patterns have been characterizedunder optical and electronic microscopies. Theirstability can be explained by the competition betweenthe anchoring field of the substrate andthe presence of a yield stress resulting fromthe peculiar elastic and rheological properties ofthe GFLC. Our findings also clarify why longstandinghypotheses on the presence of exoticphases1 at large concentrations are present inthe literature.
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[2] Zamora-Ledezma, C.; Puech, N.; Zakri, C.; Grelet, E.; Moulton, S. E.; Wallace, G. G.; Gambhir, S.; Blanc, C.; Anglaret, E.;Poulin, P. The journal of physical chemistry letters 2012, 3, 2425–2430..
[3] Poulin, P.; Jalili, R.; Neri, W.; Nallet, F.; Divoux, T.; Colin, A.; Aboutalebi, S. H.; Wallace, G.; Zakri, C. Proceedings of theNational Academy of Sciences 2016, 113, 11088–11093..
[4] Zamora-Ledezma, C.; Jeridi, H.; Anglaret, E.; Blanc, C. Orientations and periodic textures in graphene liquid crystals. 27thInternational Liquid Crystal Conference (ILCC2018). 2018..
[5] Xu, Z.; Gao, C. Nature communications 2011, 2, 571.