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result(s) for
"Gibaud, Thomas"
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Uncovering Instabilities in the Spatiotemporal Dynamics of a Shear-Thickening Cornstarch Suspension
by
Saint-Michel, Brice
,
Gibaud, Thomas
,
Manneville, Sébastien
in
Antiballistic materials
,
Computational fluid dynamics
,
Contact force
2018
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, turbulentlike 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.
Journal Article
Reconfigurable self-assembly through chiral control of interfacial tension
by
Yang, Yasheng
,
Henglin, Mir
,
Zakhary, Mark J.
in
639/301/923
,
639/638/403/935
,
639/638/541/966
2012
Molecular chirality can be used to control interfacial tension in multi-component mixtures of chiral molecules, and tuning the chirality makes it possible to produce and manipulate self-assembling complex chiral structures.
Self assembly with an edge
The most familiar approach to modifying interfacial tension, an important property of complex multicomponent materials, is to add surfactants. Examples include simple cleaning agents and the protein/lipid surfactant found in the mammalian lung. Here Zvonimir Dogic and colleagues describe a new way of manipulating interfacial tension, this time in a two-dimensional colloidal membrane, through molecular chirality. They show that the slight twist of chiral viruses, incorporated in a two-dimensional liquid crystal membrane, cannot be supported. Instead, the twist is expelled to the edge of the membrane. The chirality of the viruses can be tuned using temperature, and this allows the line tension of the membrane edge to be manipulated, ultimately leading to polymorphic transitions. The system can be manipulated to produce reconfigurable structures using optical tweezers, offering the potential for the nanosculpture of versatile new materials with complex topologies.
From determining the optical properties of simple molecular crystals to establishing the preferred handedness in highly complex vertebrates, molecular chirality profoundly influences the structural, mechanical and optical properties of both synthetic and biological matter on macroscopic length scales
1
,
2
. In soft materials such as amphiphilic lipids and liquid crystals, the competition between local chiral interactions and global constraints imposed by the geometry of the self-assembled structures leads to frustration and the assembly of unique materials
3
,
4
,
5
,
6
. An example of particular interest is smectic liquid crystals, where the two-dimensional layered geometry cannot support twist and chirality is consequently expelled to the edges in a manner analogous to the expulsion of a magnetic field from superconductors
7
,
8
,
9
,
10
. Here we demonstrate a consequence of this geometric frustration that leads to a new design principle for the assembly of chiral molecules. Using a model system of colloidal membranes
11
, we show that molecular chirality can control the interfacial tension, an important property of multi-component mixtures. This suggests an analogy between chiral twist, which is expelled to the edges of two-dimensional membranes, and amphiphilic surfactants, which are expelled to oil–water interfaces
12
. As with surfactants, chiral control of interfacial tension drives the formation of many polymorphic assemblages such as twisted ribbons with linear and circular topologies, starfish membranes, and double and triple helices. Tuning molecular chirality
in situ
allows dynamical control of line tension, which powers polymorphic transitions between various chiral structures. These findings outline a general strategy for the assembly of reconfigurable chiral materials that can easily be moved, stretched, attached to one another and transformed between multiple conformational states, thus allowing precise assembly and nanosculpting of highly dynamical and designable materials with complex topologies.
Journal Article
Rheoacoustic Gels: Tuning Mechanical and Flow Properties of Colloidal Gels with Ultrasonic Vibrations
2020
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 “rheoacoustic” 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 rheoacoustic gels.
Journal Article
Achiral symmetry breaking and positive Gaussian modulus lead to scalloped colloidal membranes
by
Sharma, Prerna
,
Zakhary, Mark J.
,
Powers, Thomas R.
in
Applied Physical Sciences
,
Bilayers
,
Broken symmetry
2017
In the presence of a nonadsorbing 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 elasticity of fluid sheets. Membranes assembled from single-component chiral rods form flat disks with uniform edge twist. In comparison, membranes composed of a 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.
Journal Article
Bonded straight and helical flagellar filaments form ultra-low-density glasses
by
Schwenger, Walter
,
Yardimci, Sevim
,
Sartucci, Matthew R.
in
Applied Physical Sciences
,
Biological Physics
,
Block copolymers
2023
We study how the three-dimensional shape of rigid filaments determines the microscopic dynamics and macroscopic rheology of entangled semidilute Brownian suspensions. To control the filament shape we use bacterial flagella, which are microns-long helical or straight filaments assembled from flagellin monomers. We compare the dynamics of straight rods, helical filaments, and shape-diblock copolymers composed of seamlessly joined straight and helical segments. Caged by their neighbors, straight rods preferentially diffuse along their long axis, but exhibit significantly suppressed rotational diffusion. Entangled helical filaments escape their confining tube by corkscrewing through the dense obstacles created by other filaments. By comparison, the adjoining segments of the rod-helix shape-diblocks suppress both the translation and the corkscrewing dynamics. Consequently, the shape-diblock filaments become permanently jammed at exceedingly low densities. We also measure the rheological properties of semidilute suspensions and relate their mechanical properties to the microscopic dynamics of constituent filaments. In particular, rheology shows that an entangled suspension of shape rod-helix copolymers forms a low-density glass whose elastic modulus can be estimated by accounting for how shear deformations reduce the entropic degrees of freedom of constrained filaments. Our results demonstrate that the three-dimensional shape of rigid filaments can be used to design rheological properties of semidilute fibrous suspensions.
Journal Article
Condensation and dissolution of nematic droplets in dispersions of colloidal rods with thermo–sensitive depletants
2015
Nematic droplets are droplets composed of elongated molecules that tend to point in the same direction but do not have any positional order. Such droplets are well known to adopt a spindle shape called tactoid. How such droplets condensate or melt and how the orientational symmetry is broken remains however unclear. Here we use a colloidal system composed of filamentous viruses as model rod–like colloids and pnipam microgel particles to induce thermo–sensitive depletion attraction between the rods. Microscopy experiments coupled to particle tracking reveal that the condensation of a nematic droplet is preceded by the formation of a new phase, an isotropic droplet. As the viruses constitute an excellent experimental realization of hard rods, it follows that the phenomenology we describe should be relevant to diverse micro- and nano-sized rods that interact through excluded volume interactions. This transition between isotropic and nematic droplets provides a new and reversible pathway to break the symmetry and order colloidal rods within a droplet with an external stimulus and could constitute a benchmark experiment for a variety of technologies relying on reconfigurable control of rods.
Journal Article
In vivo measurements of fascia lata effective mechanics combined to a memory fiber recruitment viscoelastic modeling approach
2026
The fascia lata plays a central role in force transmission and body mechanics, yet its in vivo mechanical behavior remains poorly characterized. Existing approaches -- shear wave elastography and direct force measurements alike -- share a fundamental limitation: none simultaneously captures both the elastic and viscous components of fascial mechanics within a single experiment. The primary aim of this study is therefore to develop an experimental and modeling framework that enables the reproducible measurement of the effective viscoelastic properties of the fascia lata in vivo. To this end, we combine controlled ramp-relaxation experiments on the human fascia lata with a constitutive model that integrates fiber recruitment and dual-timescale viscoelastic relaxation. We emphasize that this is an effective model: rather than describing intrinsic local material properties, it characterizes the mechanical response of the fascia lata complex including its coupling to the hip-thigh musculoskeletal system under controlled loading conditions. The model captures both the nonlinear stiffening during elongation and the dual decay of force during relaxation, using a minimal set of physically interpretable parameters. Repeated trials demonstrate good reproducibility, with parameter variability within 10%. Our results support the view that fascia lata behaves as a hierarchical, hydrated composite whose macroscopic mechanical response emerges from the coupled effects of collagen alignment, matrix viscoelasticity, and fluid flow. This work provides a quantitative foundation for future in vivo investigations into how training, rehabilitation, or aging influence the evolution of fascial mechanical properties.
Shear-driven memory effects in carbon black gels
2025
In recent years, significant effort has been devoted to developing smart materials whose mechanical properties can adapt under physical stimuli. Particulate colloidal gels, which behave as solids but can also flow under stress, have emerged as promising candidates. Resulting from the attractive interaction between their constituents, their network architecture exhibit solid-like properties even at very low volume fractions. This structural flexibility allows them to adopt various configurations and store structural information making them highly susceptible to memory effects. Shear flow, applied through rheometry, offers a simple and effective way to tune their properties and imprint a ``rheological memory'' of the flow history. However, the precise relationship between flow history and viscoelastic response remains elusive, largely due to the limited structural characterization of these systems during flow and after flow cessation. Here, we use ultra-small angle X-ray scattering (USAXS) to reveal a strong structural memory in the solid state, where the microstructure formed under shear is retained after flow cessation. We identify two distinct mechanisms of structural memory, as governed by the ratio of viscous to attractive forces, namely, the Mason number. Using recently developed fractal scaling laws, we show that the rheology is fully determined by the gel microstructure. Notably, these gels exhibit a double-fractal architecture, highlighting the remarkably broad range of length scales over which these disordered materials are structured. By clarifying how memory is encoded, our results offer strategies to tune shear sensitivity of colloidal gels and design smart materials.
Imprintable membranes from incomplete chiral coalescence
2014
Coalescence is an essential phenomenon that governs the equilibrium behaviour in a variety of systems from intercellular transport to planetary formation. In this report, we study coalescence pathways of circularly shaped two-dimensional colloidal membranes, which are one rod-length-thick liquid-like monolayers of aligned rods. The chirality of the constituent rods leads to three atypical coalescence pathways that are not found in other simple or complex fluids. In particular, we characterize two pathways that do not proceed to completion but instead produce partially joined membranes connected by line defects—
π
-wall defects or alternating arrays of twisted bridges and pores. We elucidate the structure and energetics of these defects and ascribe their stability to a geometrical frustration inherently present in chiral colloidal membranes. Furthermore, we induce the coalescence process with optical forces, leading to a robust on-demand method for imprinting networks of channels and pores into colloidal membranes.
Conventional coalescence at fluid drop and bubble interfaces follows the all-or-none rule. Zakhary
et al
. show that the coalescence between colloidal membranes composed of aligned rod-like viruses does not follow this rule, but exhibits an intermediate state induced by topological defects.
Journal Article
Photoredox Processes in the Aggregation and Gelation of Electron-Responsive Supramolecular Polymers Based on Viologen
by
Reynard-Feytis, Quentin
,
Chevallier, Floris
,
Bucher, Christophe
in
Dimerization
,
Electron transfer
,
Gelation
2022
Viologen-based ditopic bis-pyridinyl-triazole bidentate ligands self-assemble in the presence of palladium ions into supramolecular polymers whose structure is imposed by the directed formation of coordination bonds. Light-irradiation of these electron-responsive supramolecular materials triggers a photo-induced electron transfer yielding isolated π-radicals and dimers of radicals. The photoreduction events and the associated dimerization steps trigger a large-scale reorganization occurring within the supramolecular network yielding aggregates or gels depending on the irradiation conditions (power, duration). Detailed electrochemical, spectro-electrochemical and photochemical analyses were conducted to understand the mechanisms at stakes in these light-induced aggregation and gelation.
Journal Article