Ref HAL: hal-03672529_v1
Ref Arxiv: 2111.06144
DOI: 10.1039/d1sm01075a
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We use the impact of drops on a small solid target as a tool to investigate the behavior of viscoelastic fluids under extreme deformation rates. We study two classes of transient networks: semidilute solutions of supramolecular polymers and suspensions of spherical oil droplets reversibly linked by polymers. The two types of samples display very similar linear viscoelastic properties, which can be described with a Maxwell fluid model, but contrasting nonlinear properties due to different network structure. Upon impact, weakly viscoelastic samples exhibit a behavior qualitatively similar to that of Newtonian fluids: A smooth and regular sheet forms, expands, and then retracts. By contrast, for highly viscoelastic fluids, the thickness of the sheet is found to be very irregular, leading to instabilities and eventually formation of holes. We find that material rheological properties rule the onset of instabilities. We first provide a simple image analysis of the expanding sheets to determine the onset of instabilities. We then demonstrate that a Deborah number related to the shortest relaxation time associated to the sample structure following a high shear is the relevant parameter that controls the heterogeneities in the thickness of the sheet, eventually leading to the formation of holes. When the sheet tears-up, data suggest by contrast that the opening dynamics depends also on the expansion rate of the sheet.

Ref HAL: hal-03648934_v1
Ref Arxiv: 2110.01097
DOI: 10.1073/pnas.2103995118
WoS: WOS:000720926900021
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Mucus is a biological gel protecting several tissues. Its key properties result from a crucial balance between solid-like and fluid-like behavior, ensured by the nonpermanent nature of the bonds between its macromolecular constituents. Our understanding of the micrometer-scale response of mucus to an applied stress is still rudimentary, although in living organisms, stresses acting on mucus are ubiquitous, from bacterial penetration to coughing and peristalsis. We show that under a modest applied stress, in the mechanical linear regime, the microscopic dynamics of pig gastric mucus transiently accelerate by up to 2 orders of magnitude. A simple model rationalizes this previously unrecognized fluidization mechanism stemming from elastic recoil following bond breaking and generalizes our findings to networks with reversible bonds.Mucus is a biological gel covering the surface of several tissues and ensuring key biological functions, including as a protective barrier against dehydration, pathogen penetration, or gastric acids. Mucus biological functioning requires a finely tuned balance between solid-like and fluid-like mechanical response, ensured by reversible bonds between mucins, the glycoproteins that form the gel. In living organisms, mucus is subject to various kinds of mechanical stresses, e.g., due to osmosis, bacterial penetration, coughing, and gastric peristalsis. However, our knowledge of the effects of stress on mucus is still rudimentary and mostly limited to macroscopic rheological measurements, with no insight into the relevant microscopic mechanisms. Here, we run mechanical tests simultaneously to measurements of the microscopic dynamics of pig gastric mucus. Strikingly, we find that a modest shear stress, within the macroscopic rheological linear regime, dramatically enhances mucus reorganization at the microscopic level, as signaled by a transient acceleration of the microscopic dynamics, by up to 2 orders of magnitude. We rationalize these findings by proposing a simple, yet general, model for the dynamics of physical gels under strain and validate its assumptions through numerical simulations of spring networks. These results shed light on the rearrangement dynamics of mucus at the microscopic scale, with potential implications in phenomena ranging from mucus clearance to bacterial and drug penetration.ASCII and Excel files for all the datasets shown in the figures of the main text and SI Appendix have been deposited in Zenodo (DOI: 10.5281/zenodo.5533877) (74).

Ref HAL: hal-03359470_v1
DOI: 10.1021/acs.analchem.1c00527
WoS: 000645428400029
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12 Citations
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Aggregation mechanisms of amyloid β peptides depend on multiple intrinsic and extrinsic physicochemical factors (e.g., peptide chain length, truncation, peptide concentration, pH, ionic strength, temperature, metal concentration, etc.). Due to this high number of parameters, the formation of oligomers and their propensity to aggregate make the elucidation of this physiopathological mechanism a challenging task. From the analytical point of view, up to our knowledge, few techniques are able to quantify, in real time, the proportion and the size of the different soluble species during the aggregation process. This work aims at demonstrating the efficacy of the modern Taylor dispersion analysis (TDA) performed in capillaries (50 μm i.d.) to unravel the speciation of β-amyloid peptides in low-volume peptide samples (∼100 μL) with an analysis time of ∼3 min per run. TDA was applied to study the aggregation process of Aβ(1-40) and Aβ(1-42) peptides at physiological pH and temperature, where more than 140 data points were generated with a total volume of ∼1 μL over the whole aggregation study (about 0.5 μg of peptides). TDA was able to give a complete and quantitative picture of the Aβ speciation during the aggregation process, including the sizing of the oligomers and protofibrils, the consumption of the monomer, and the quantification of different early- and late-formed aggregated species.

Ref HAL: hal-03189744_v1
DOI: 10.1021/acs.langmuir.0c03441
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The adsorption of a sunflower protein extract at two air− water and oil−water interfaces is investigated using tensiometry, dilational viscoelasticity, and ellipsometry. For both interfaces, a three step mechanism was evidenced thanks to master curve representations of the data taken at different aging times and protein concentrations. At short times, a diffusion limited adsorption of proteins at interfaces is demonstrated. First, a two-dimensional protein film is formed with a partition of the polypeptide chains in the two phases that depends strongly on the nature of the hydrophobic phase: most of the film is in the aqueous phase at the air−water interface, while it is mostly in the organic phase at the oil−water interface. Then a three-dimensional saturated monolayer of proteins is formed. At short times, adsorption mechanisms are analogous to those found with typical globular proteins, while strong divergences are observed at longer adsorption times. Following the saturation step, a thick layer expands in the aqueous phase and appears associated with the release of large objects in the bulk. The kinetic evolution of this second layer is compatible with a diffusion limited adsorption of the minor population of polymeric complexes with hydrodynamic radius R H ∼ 80 nm, evidenced in equilibrium with hexameric globulins (R H ∼ 6 nm) in solution. These complexes could result from the presence of residual polyphenols in the extract and raise the question of the role of these compounds in the interfacial properties of plant protein extracts.

Ref HAL: hal-03351539_v1
DOI: 10.1122/8.0000303
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We report on the response of semi-dilute shear-banding wormlike micelles to time-dependent flow protocols such as step stress and shear startup. We use global rheology coupled to direct optical visualisations in Taylor-Couette flow to provide a detailed 2D description of the spatio-temporal dynamics of the shear banding flow under imposed stress. We compare these dynamics to their extensively studied counterpart under imposed shear rate. We show that, for a given asymptotic state, the onset of banding is delayed and the transients are longer when the stress is used as control parameter. The way the banding structure is built up strongly depends on the control parameter. In the two cases, secondary flows develop on top of the shear-banding instability: after shear startup, the interface between bands is formed in the bulk of the system and migrates inwards to its stationary position in the gap of the Taylor-Couette device, before being destabilized due to elastic instability; under creep flow, the interface between bands forms at the inner wall and becomes wavy while it is still migrating outwards to its steady position, leading to permanent rearrangements of the flow structure until steady state is reached, potentially explaining longer transients. We also outline the possible mechanical signature of the onset of shear banding in terms of shape of the bulk mechanical signals, which is the subject of the second part of this work [Briole et al., submitted].

Ref HAL: hal-03345301_v1
DOI: 10.1122/8.0000304
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Complex systems often exhibit shear banding-the coexistence of two different states characterized by their internal structuring and local shear rates. For some of them, the heterogeneous flow corresponds to the final steady state response while for others, shear banding can only be transient, the banding structure healing back to homogeneous flow in the ultimate steady state after long-lived periods. In order to explain the diversity of observations, Moorcroft and Fielding have established general criteria for the onset of banding in time-dependent flows of complex systems, ranging from polymeric fluids to soft glassy materials [Moorcroft et al., Phys. Rev. Lett., 2013, 110, 086001]. The proposed criteria are based on the time evolution of the bulk rheological response function of the system to a given time-dependent flow protocol and are associated with a specific signature in the mechanical response. In this contribution, we test the validity of these criteria in the case of two common time-dependent flow protocols: a step stress and a shear startup. Two types of fluids are examined. On the one hand, a wormlike micelles system exhibiting steady shear banding is studied experimentally, using rheometry coupled with direct visualisations and particle image velocimetry. On the other hand, we analyse previous literature on yield stress fluids exhibiting transient shear banding. Under creep flow, for both types of fluids the onset of banding arises in a time window compatible with the Moorcroft-Fielding criterion. However, the mechanical signature, i.e. the shape of the bulk mechanical signal as a function of time is not the one expected within some of the specific models with which the general Moorcroft-Fielding criteria were tested numerically. Under shear startup, both types of fluids behave differently. The criterion holds for yield stress fluids, the onset of banding arising just after the stress overshoot, as expected. On the contrary, for wormlike micelles the window of instability is delayed, even if the overshoot clearly plays a crucial role in the nucleation of the shear-induced structures. Regardless of the flow protocol or the system, wall slip seems to go hand in hand with banding indicating that it is a key ingredient to take into account.

Ref HAL: hal-03324137_v1
Ref Arxiv: 2107.13348
DOI: 10.1063/5.0057316
WoS: 000691864900008
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2 Citations
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When a drop of fluid hits a small solid target of comparable size, it expands radially until reaching a maximum diameter and subsequently recedes. In this work, we show that the expansion process of liquid sheets is controlled by a combination of shear (on the target) and biaxial extensional (in the air) deformations. We propose an approach toward a rational description of the phenomenon for Newtonian and viscoelastic fluids by evaluating the viscous dissipation due to shear and extensional deformations, yielding a prediction of the maximum expansion factor of the sheet as a function of the relevant viscosity. For Newtonian systems, biaxial extensional and shear viscous dissipation are of the same order of magnitude. On the contrary, for thinning solutions of supramolecular polymers, shear dissipation is negligible compared to biaxial extensional dissipation and the biaxial thinning extensional viscosity is the appropriate quantity to describe the maximum expansion of the sheets. Moreover, we show that the rate-dependent biaxial extensional viscosities deduced from drop impact experiments are in good quantitative agreement with previous experimental data and theoretical predictions for various viscoelastic liquids.