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Thomas Gibaud

Publications and source records attributed to Thomas Gibaud.

At least 37 records · Page 2Linked to original sources

Light-controlled aggregation and gelation of viologen-based coordination polymers

Ditopic bis-(triazole-pyridine)viologens are bidentate ligands that self-assemble into coordination polymers. In such photo-responsive materials, light irradiation initiates photo-induced electron transfer to generate pi-radicals that can self-associate to form pi-dimers. This leads to a cascade of events: processes at the supramolecular scale associated with mechanical and structural transition at the macroscopic scale. By tuning the irradiation power and duration, we evidence the formation of aggregates and gels. Using microscopy, we show that the aggregates are dense polydisperse micron size spindle shaped particles which grow in time. Using microscopy and time resolved micro-rheology, we follow the gelation kinetics which leads to a gel characterized by a correlation length of a few microns and a weak elastic modulus. The analysis of the aggregates and the gel states vouch for an arrested phase separation process.

cond-mat.soft↗

Mechanics and structure of carbon black gels under high-power ultrasound

Colloidal gels made of carbon black particles dispersed in light mineral oil are "rheo-acoustic" materials, i.e., their mechanical and structural properties can be tuned using high-power ultrasound, sound waves with submicron amplitude and frequency larger than 20~kHz . The effects of high-power ultrasound on the carbon black gel are demonstrated using two experiments: rheology coupled to ultrasound to test for the gel mechanical response and a timeresolved ultra small-angle X-ray scattering experiment (TRUSAXS) coupled to ultrasound to test for structural changes within the gel. We show that high-power ultrasound above a critical amplitude leads to a complex viscoelastic transient response of the gels within a few seconds: a softening of its storage modulus accompanied by a strong overshoot in its loss modulus. Under high-power ultrasound, the gel displays a viscoelastic spectrum with glass-like features and a significant decrease in its yield strain. Those effects are attributed to the formation of intermittent micro-cracks in the bulk of the gel as evidenced by TRUSAXS. Provided that the shear rate is not large enough to fully fluidize the sample, high-power ultrasound also facilitates the flow of the gel, reducing its yield stress as well as increasing the shear-thinning index, thanks again to the formation of micro-cracks.

cond-mat.soft↗

Nonlinear mechanics of colloidal gels: creep, fatigue and shear-induced yielding

Colloidal gels are formed through the aggregation of attractive particles, whose size ranges from 10~nm to a few micrometers, suspended in a liquid. Such gels are ubiquitous in everyday life applications, from food products to paints or construction materials, in particular thanks to their ability to easily "yield", i.e., to turn from a solid to a liquid under the application of a weak external load. Understanding and controlling the mechanical response of colloidal gels is therefore of prime importance. Depending on the details of the system, however, the resulting gel networks present different microstructural organisations that may lead to widely different mechanical responses. This raises important challenges in fully characterizing yielding and in uncovering the mechanisms of nonlinear response in colloidal gels. In this paper, we distinguish between two classes of colloidal gels showing respectively reversible yielding, where the gel network reforms upon load release, and irreversible yielding, where the network is fully destroyed through fractures and phase separation. This broad, empirical distinction is achieved through rheology and local experiments at a mesoscopic scale, intermediate between the network characteristic size and the sample size. We further discuss how the observables derived from creep and fatigue experiments may be modelled to predict yielding and highlight open questions and future research directions in the domain.

cond-mat.soft↗

Colloidal transport in bacteria suspensions: from bacteria scattering to anomalous and enhanced diffusion

Colloids coupled to a bath of swimming cells generically display enhanced diffusion. This transport dynamics stems from a subtle interplay between the active and passive particles that still resists our understanding despite decades of intense research. Here, we tackle the root of the problem by providing a quantitative characterisation of the single scattering events between a colloid and a bacterium. Based on our experiments, we build a minimal model that quantitatively predicts the geometry of the scattering trajectories, and enhanced colloidal diffusion at long times. This quantitative confrontation between theory and experiments elucidates the microscopic origin of enhanced transport. Collisions are solely ruled by stochastic contact interactions responsible both for genuine anomalous diffusion at short times and enhanced diffusion at long times with no ballistic regime at any scale.

cond-mat.soft↗

Rheo-acoustic gels: Tuning mechanical and flow properties of colloidal gels with ultrasonic vibrations

Colloidal gels, where nanoscale particles aggregate into an elastic yet fragile network, are at the heart of materials that combine specific optical, electrical and mechanical properties. Tailoring the viscoelastic features of colloidal gels in real-time thanks to an external stimulus currently appears as a major challenge in the design of "smart" soft materials. Here we introduce "rheo-acoustic" gels, a class of materials that are sensitive to ultrasonic vibrations. By using a combination of rheological and structural characterization, we evidence and quantify a strong softening in three widely different colloidal gels submitted to ultrasonic vibrations (with submicron amplitude and frequency 20-500 kHz). This softening is attributed to micron-sized cracks within the gel network that may or may not fully heal once vibrations are turned off depending on the acoustic intensity. Ultrasonic vibrations are further shown to dramatically decrease the gel yield stress and accelerate shear-induced fluidization. Ultrasound-assisted fluidization dynamics appear to be governed by an effective temperature that depends on the acoustic intensity. Our work opens the way to a full control of elastic and flow properties by ultrasonic vibrations as well as to future theoretical and numerical modeling of such rheo-acoustic gels.

cond-mat.soft↗

Etude des effets non linéaires observés sur les oscillations d'un pendule simple

In this paper we present a study of the non-linear effects of anharmonicity of the potential of the simple pendulum. In a theoretical reminder we highlight that anharmonicity of the potential generates additional harmonics and the non-isochronism of oscillations. These phenomena are all the more important as we move away from the oscillations at small angles, which represent the domain of validity of the harmonic approximation. The measurement is apprehended by means of the acquisition box SYSAM-SP5 coupled with the Latis pro software and the Eurosmart pendulum. We show that only a detailed analysis by fitting the recorded curve can provide sufficient accuracy to describe the quadratic evolution of the period as a function of the amplitude of the oscillations. We we can detect the additional harmonics in the oscillations when the amplitude becomes very high.

physics.ed-ph↗

Vidange d'un réservoir

We show in this article that depending on the flow conditions the same fluid can be considered as a perfect fluid or on the contrary as viscous fluid. These properties are addressed by emptying a tank. we show that we pass from one regime to another by just changing the length of the outlet tube of the tank is drained. This change of regime takes place in accordance with a criterion defined in the theoretical part.

physics.flu-dyn↗

Equation of State of Colloidal Membranes

In the presence of a non-adsorbing polymer, monodisperse rod-like colloids assemble into one-rod-length thick liquid-like monolayers, called colloidal membranes. The density of the rods within a colloidal membrane is determined by a balance between the osmotic pressure exerted by the enveloping polymer suspension and the repulsion between the colloidal rods. We developed a microfluidic device for continuously observing an isolated membrane while dynamically controlling the osmotic pressure of the polymer suspension. Using this technology we measured the membrane rod density over a range of osmotic pressures than is wider that what is accessible in equilibrium samples. With increasing density we observed a first-order phase transition, in which the in-plane membrane order transforms from a 2D fluid into a 2D solid. In the limit of low osmotic pressures, we measured the rate at which individual rods evaporate from the membrane. The developed microfluidic technique could have wide applicability for in situ investigation of various soft materials and how their properties depend on the solvent composition.

cond-mat.soft↗

Irreversible hardening of a colloidal gel under shear: the smart response of natural rubber latex gels

Natural rubber is obtained by processing natural rubber latex, a liquid colloidal suspension that rapidly gels after exudation from the tree. We prepared such gels by acidification, in a large range of particle volume fractions, and investigated their rheological properties. We show that natural rubber latex gels exhibit a unique behavior of irreversible strain hardening: when subjected to a large enough strain, the elastic modulus increases irreversibly. Hardening proceeds over a large range of deformations in such a way that the material maintains an elastic modulus close to, or slightly higher than the imposed shear stress. Local displacements inside the gel are investigated by ultrasound imaging coupled to oscillatory rheometry, together with a Fourier decomposition of the oscillatory response of the material during hardening. Our observations suggest that hardening is associated with irreversible local rearrangements of the fractal structure, which occur homogeneously throughout the sample.

cond-mat.soft↗

Uncovering instabilities in the spatiotemporal dynamics of a shear-thickening cornstarch suspension

Recent theories predict that discontinuous shear-thickening (DST) involves an instability, the nature of which remains elusive. Here, we explore unsteady dynamics in a dense cornstarch suspension by coupling long rheological measurements under constant shear stresses to ultrasound imaging. We demonstrate that unsteadiness in DST results from localized bands that travel along the vorticity direction with a specific signature on the global shear rate response. These propagating events coexist with quiescent phases for stresses slightly above DST onset, resulting in intermittent, turbulent-like dynamics. Deeper into DST, events proliferate, leading to simpler, Gaussian dynamics. We interpret our results in terms of unstable vorticity bands as inferred from recent model and numerical simulations.

cond-mat.soft↗

Filamentous phages as building blocks for reconfigurable and hierarchical self-assembly

Filamentous bacteriophages such as fd-like viruses are monodisperse rod-like colloids that have well defined properties: diameter, length, rigidity, charge and chirality. Engineering those viruses leads to a library of colloidal rods which can be used as building blocks for reconfigurable and hierarchical self-assembly. Their condensation in aqueous solution þ{with additive polymers which act as depletants to induce} attraction between the rods leads to a myriad of fluid-like micronic structures ranging from isotropic/nematic droplets, colloid membranes, achiral membrane seeds, twisted ribbons, $π$-wall, pores, colloidal skyrmions, Möbius anchors, scallop membranes to membrane rafts. Those structures and the way they shape shift not only shed light on the role of entropy, chiral frustration and topology in soft matter but it also mimics many structures encountered in different fields of science. On one hand, filamentous phages being an experimental realization of colloidal hard rods, their condensation mediated by depletion interactions constitutes a blueprint for self-assembly of rod-like particles and provides fundamental foundation for bio- or material oriented applications. On the other hand, the chiral properties of the viruses restrict the generalities of some results but vastly broaden the self-assembly possibilities.

cond-mat.soft↗

Synthetic Schlieren -- application to the visualization and characterization of air convection

Synthetic schlieren is an digital image processing optical method relying on the variation of optical index to visualize the flow of a transparent fluid. In this article, we present a step-by step, easy-to-implement and affordable experimental realization of this technique. The method is applied to air convection caused by a warm surface. We show that the velocity of rising convection plumes can be linked to the temperature of the warm surface and propose a simple physical argument to explain this dependence. Moreover, using this method, one can reveal the tenuous convection plumes rising from ounce's hand, a phenomenon invisible to the naked eye. This spectacular result may help student realize the power of careful data acquisition combined with astute image processing techniques.

physics.flu-dyn↗

Predicting and assessing rupture in protein gels under oscillatory shear

Soft materials may break irreversibly upon applying sufficiently large shear oscillations, a process which physical mechanism remains largely elusive. In this work, the rupture of protein gels made of sodium caseinate under an oscillatory stress is shown to occur in an abrupt, brittle-like manner. Upon increasing the stress amplitude, the build-up of harmonic modes in the strain response can be rescaled for all gel concentrations. This rescaling yields an empirical criterion to predict the rupture point way before the samples are significantly damaged. "Fatigue" experiments under stress oscillations of constant amplitude can be mapped onto the former results, which indicates that rupture is independent of the temporal pathway in which strain and damage accumulate. Finally, using ultrasonic imaging, we measure the local mechanical properties of the gels before, during and after breakdown, showing that the strain field remains perfectly homogeneous up to rupture but suddenly gives way to a solid-fluid phase separation upon breakdown.

cond-mat.soft↗

Achiral symmetry breaking and positive Gaussian modulus lead to scalloped colloidal membranes

In the presence of a non-adsorbing polymer, monodisperse rod-like particles assemble into colloidal membranes, which are one rod-length thick liquid-like monolayers of aligned rods. Unlike 3D edgeless bilayer vesicles, colloidal monolayer membranes form open structures with an exposed edge, thus presenting an opportunity to study physics of thin elastic sheets. Membranes assembled from single-component chiral rods form flat disks with uniform edge twist. In comparison, membranes comprised of mixture of rods with opposite chiralities can have the edge twist of either handedness. In this limit disk-shaped membranes become unstable, instead forming structures with scalloped edges, where two adjacent lobes with opposite handedness are separated by a cusp-shaped point defect. Such membranes adopt a 3D configuration, with cusp defects alternatively located above and below the membrane plane. In the achiral regime the cusp defects have repulsive interactions, but away from this limit we measure effective long-ranged attractive binding. A phenomenological model shows that the increase in the edge energy of scalloped membranes is compensated by concomitant decrease in the deformation energy due to Gaussian curvature associated with scalloped edges, demonstrating that colloidal membranes have positive Gaussian modulus. A simple excluded volume argument predicts the sign and magnitude of the Gaussian curvature modulus that is in agreement with experimental measurements. Our results provide insight into how the interplay between membrane elasticity, geometrical frustration and achiral symmetry breaking can be used to fold colloidal membranes into 3D shapes.

cond-mat.soft↗

Local Oscillatory Rheology from Echography

Local Oscillatory Rheology from Echography (LORE) consists in a traditional rheology experiment synchronized with high-frequency ultrasonic imaging which gives access to the local material response to oscillatory shear. Besides classical global rheological quantities, this method provides quantitative time-resolved information on the local displacement across the entire gap of the rheometer. From the local displacement response, we compute and decompose the local strain in its Fourier components and measure the spatially-resolved viscoelastic moduli. After benchmarking our method on homogeneous Newtonian fluids and soft solids, we demonstrate that this technique is well suited to characterize spatially heterogeneous samples, wall slip, and the emergence of nonlinearity under large amplitude oscillatory stress in soft materials.

cond-mat.soft↗

Differential Dynamic Microscopy to characterize Brownian motion and bacteria motility

We have developed a lab work module where we teach undergraduate students how to quantify the dynamics of a suspension of microscopic particles, measuring and analyzing the motion of those particles at the individual level or as a group. Differential Dynamic Microscopy (DDM) is a relatively recent technique that precisely does that and constitutes an alternative method to more classical techniques such as dynamics light scattering (DLS) or video particle tracking (VPT). DDM consists in imaging a particle dispersion with a standard light microscope and a camera. The image analysis requires the students to code and relies on digital Fourier transform to obtain the intermediate scattering function, an autocorrelation function that characterizes the dynamics of the dispersion. We first illustrate DDM on the textbook case of colloids where we measure the diffusion coefficient. Then we show that DDM is a pertinent tool to characterize biologic systems such as motile bacteria i.e.bacteria that can self propel, where we not only determine the diffusion coefficient but also the velocity and the fraction of motile bacteria. Finally, so that our paper can be used as a tutorial to the DDM technique, we have joined to this article movies of the colloidal and bacterial suspensions and the DDM algorithm in both Matlab and Python to analyze the movies.

cond-mat.soft↗

Multiple yielding processes in a colloidal gel under large amplitude oscillatory stress

Fatigue refers to the changes in material properties caused by repeatedly applied loads. It has been widely studied for, e.g., construction materials, but much less has been done on soft materials. Here, we characterize the fatigue dynamics of a colloidal gel. Fatigue is induced by large amplitude oscillatory stress (LAOStress), and the local displacements of the gel are measured through high-frequency ultrasonic imaging. We show that fatigue eventually leads to rupture and fluidization. We evidence four successive steps associated with these dynamics: (i) the gel first remains solid, (ii) it then slides against the walls, (iii) the bulk of the sample becomes heterogeneous and displays solid-fluid coexistence, and (iv) it is finally fully fluidized. It is possible to homogeneously scale the duration of each step with respect to the stress oscillation amplitude $σ_0$. The data are compatible with both exponential and power-law scalings with $σ_0$, which hints at two possible interpretations in terms of delayed yielding in terms activated processes or of the Basquin law. Surprisingly, we find that the model parameters behave nonmonotonically as we change the oscillation frequency and/or the gel concentration.

cond-mat.soft↗

Entropic forces stabilize diverse emergent structures in colloidal membranes

The depletion interaction mediated by non-adsorbing polymers promotes condensation and assembly of repulsive colloidal particles into diverse higher-order structures and materials. One example, with particularly rich emergent behaviors, is the formation of two-dimensional colloidal membranes from a suspension of filamentous $\it{fd}$ viruses, which act as rods with effective repulsive interactions, and dextran, which acts as a condensing, depletion-inducing agent. Colloidal membranes exhibit chiral twist even when the constituent virus mixture lacks macroscopic chirality, change from a circular shape to a striking starfish shape upon changing the chirality of constituent rods, and partially coalesce via domain walls through which the viruses twist by $180^\circ$. We formulate an entropically-motivated theory that can quantitatively explain these experimental structures and measurements, both previously published and newly performed, over a wide range of experimental conditions. Our results elucidate how entropy alone, manifested through the viruses as Frank elastic energy and through the depletants as an effective surface tension, drives the formation and behavior of these diverse structures. Our generalizable principles propose the existence of analogous effects in molecular membranes and can be exploited in the design of reconfigurable colloidal structures.

cond-mat.soft↗