arXiv subjects

Thomas Gibaud

Publications and source records attributed to Thomas Gibaud.

47 records · Page 3Linked to original sources

arXiv2014

Time dependence in large amplitude oscillatory shear: a rheo-ultrasonic study of fatigue dynamics in a colloidal gel

We report on the response of a yield stress material, namely a colloidal gel made of attractive carbon black particles, submitted to large amplitude oscillatory shear stress (LAOStress). At a constant stress amplitude well below its apparent yield stress, the gel displays fatigue and progressively turns from an elastic solid to a viscous fluid. The time-resolved analysis of the strain response, of the Fourier spectrum, and of Lissajous plots allows one to define two different timescales $τ_w<τ_f$ associated with the yielding and fluidization of the gel. Coupling rheology to ultrasonic imaging further leads to a local picture of the LAOStress response in which the gel first fails at the walls at $τ_w$ and then undergoes a slow heterogeneous fluidization involving solid--fluid coexistence until the whole sample is fluid at $τ_f$. Spatial heterogeneities are observed in both the gradient and vorticity directions and suggest a fragmentation of the initially solidlike gel into macroscopic domains eroded by the surrounding fluidized suspension.

cond-mat.soft↗

arXiv2013

Intrinsic curvature determines the crinkled edges of "crenellated disks"

Elastic curvature constants determine many structural and functional properties of fluid membranes. Methods to measure the mean curvature modulus have proved to be robust. In contrast, Gaussian curvature is an intrinsic property of a surface. Thus, measuring the relevant modulus $\bar{k}$ in fluid membranes remains a challenging task. Inspired from colloidal "crenellated disks" observed in a model system composed of hard rods, we propose a concise relation between the two curvature moduli and the parameters associated with the free, crinkled edges. Our approach offers a straightforward way to determine $\bar{k}$ of these reconfigurable membranes, where various complex topologies can be nanosculpted. Further, we reveal the structure and stability of the "crenellated disks."

cond-mat.soft↗

arXiv2013

Unexpected decoupling of stretching and bending modes in protein gels

We show that gels formed by arrested spinodal decomposition of protein solutions exhibit elastic properties in two distinct frequency domains, both elastic moduli exhibiting a remarkably strong dependence on volume fraction. Considering the large difference between the protein size and the characteristic length of the network we model the gels as porous media and show that the high and low frequency elastic moduli can be respectively attributed to stretching and bending modes. The unexpected decoupling of the two modes in the frequency domain is attributed to the length scale involved: while stretching mainly relates to the relative displacement of two particles, bending involves the deformation of a strand with a thickness of the order of a thousand particle diameters.

cond-mat.soft↗

arXiv2011

Phase separation and dynamical arrest for particles interacting with mixed potentials--the case of globular proteins revisited

We examine the applicability of the extended law of corresponding states (ELCS) to equilibrium and non equilibrium features of the state diagram of the globular protein lysozyme. We provide compelling evidence that the ELCS correctly reproduces the location of the binodal for different ionic strengths, but fails in describing the location of the arrest line. We subsequently use Mode Coupling Theory (MCT) to gain additional insight into the origin of these observations. We demonstrate that while the critical point and the connected binodal and spinodal are governed by the integral features of the interaction potential described by the normalized second virial coefficient, the arrest line is mainly determined by the attractive well depth or bond strength. This article is published in Soft Matter. The reference is: DOI: 10.1039/c0sm01175d

cond-mat.soft↗

arXiv2009

The yielding dynamics of a colloidal gel

Attractive colloidal gels display a solid-to-fluid transition as shear stresses above the yield stress are applied. This shear-induced transition is involved in virtually any application of colloidal gels. It is also crucial for controlling material properties. Still, in spite of its ubiquity, the yielding transition is far from understood, mainly because rheological measurements are spatially averaged over the whole sample. Here, the instrumentation of creep and oscillatory shear experiments with high-frequency ultrasound opens new routes to observing the local dynamics of opaque attractive colloidal gels. The transition proceeds from the cell walls and heterogeneously fluidizes the whole sample with a characteristic time whose variations with applied stress suggest the existence of an energy barrier linked to the gelation process. The present results provide new test grounds for computer simulations and theoretical calculations in the attempt to better understand the yielding transition. The versatility of the technique should also allow extensive mesoscopic studies of rupture mechanisms in soft solids ranging from crystals to glassy materials.

cond-mat.soft↗

arXiv2009

A closer look at arrested spinodal decomposition in protein solutions

Concentrated aqueous solutions of the protein lysozyme undergo a liquid solid transition upon a temperature quench into the unstable spinodal region below a characteristic arrest temperature of Tf=15C. We use video microscopy and ultra-small angle light scattering in order to investigate the arrested structures as a function of initial concentration, quench temperature and rate of the temperature quench. We find that the solid-like samples show all the features of a bicontinuous network that is formed through an arrested spinodal decomposition process. We determine the correlation length Xi and demonstrate that Xi exhibits a temperature dependence that closely follows the critical scaling expected for density fluctuations during the early stages of spinodal decomposition. These findings are in agreement with an arrest scenario based on a state diagram where the arrest or gel line extends far into the unstable region below the spinodal line. Arrest then occurs when during the early stage of spinodal decomposition the volume fraction phi2 of the dense phase intersects the dynamical arrest threshold phi2Glass, upon which phase separation gets pinned into a space-spanning gel network with a characteristic length Xi.

cond-mat.soft↗

arXiv2009

Shear-induced fragmentation of Laponite suspensions

Simultaneous rheological and velocity profile measurements are performed in a smooth Couette geometry on Laponite suspensions seeded with glass microspheres and undergoing the shear-induced solid-to-fluid (or yielding) transition. Under these slippery boundary conditions, a rich temporal behaviour is uncovered, in which shear localization is observed at short times, that rapidly gives way to a highly heterogeneous flow characterized by intermittent switching from plug-like flow to linear velocity profiles. Such a temporal behaviour is linked to the fragmentation of the initially solid sample into blocks separated by fluidized regions. These solid pieces get progressively eroded over time scales ranging from a few minutes to several hours depending on the applied shear rate $\dotγ$. The steady-state is characterized by a homogeneous flow with almost negligible wall slip. The characteristic time scale for erosion is shown to diverge below some critical shear rate $\dotγ^\star$ and to scale as $(\dotγ-\dotγ^\star)^{-n}$ with $n\simeq 2$ above $\dotγ^\star$. A tentative model for erosion is discussed together with open questions raised by the present results.

cond-mat.soft↗

arXiv2009

Interplay between Spinodal Decomposition and Glass Formation in Proteins Exhibiting Short-Range Attractions

We investigate the competition between spinodal decomposition and dynamical arrest using aqueous solutions of the globular protein lysozyme as a model system for colloids with short-range attractions. We show that quenches below a temperature Ta lead to gel formation as a result of a local arrest of the proteindense phase during spinodal decomposition. The rheological properties of these gels allow us to use centrifugation experiments to determine the local densities of both phases and to precisely locate the gel boundary and the attractive glass line close to and within the unstable region of the phase diagram.

cond-mat.soft↗

arXiv2009

A simple patchy colloid model for the phase behavior of lysozyme dispersions

We propose a minimal model for spherical proteins with aeolotopic pair interactions to describe the equilibrium phase behavior of lysozyme. The repulsive screened Coulomb interactions between the particles are taken into account assuming that the net charges are smeared out homogeneously over the spherical protein surfaces. We incorporate attractive surface patches, with the interactions between patches on different spheres modeled by an attractive Yukawa potential. The parameters entering the attractive Yukawa potential part are determined using information on the experimentally accessed gas-liquid-like critical point. The Helmholtz free energy of the fluid and solid phases is calculated using second-order thermodynamic perturbation theory. Our predictions for the solubility curve are in fair agreement with experimental data. In addition, we present new experimental data for the gas-liquid coexistence curves at various salt concentrations and compare these with our model calculations. In agreement with earlier findings, we observe that the strength and the range of the attractive potential part only weakly depend on the salt content.

cond-mat.soft↗

arXiv2009

Engineering solid-like structures via an arrested spinodal decomposition

The possibilities to tune the structure of solid like material resulting from arrested spinodal decomposition is investigated using a system composed of lysozyme, a globular protein, dispersed in a water solution as model system for colloids with short range attraction. It is shown that the resulting arrested spinodal decomposition is driven by the interplay between the early kinetics of the spinodal decomposition and the dynamical arrest. The initial concentration, the quench depth and speed from the fluid state to the arrested state enable to tailor the mesh size of the solid network of the arrested spinodal decomposition.

cond-mat.soft↗

arXiv2009

Influence of boundary conditions on yielding in a soft glassy material

The yielding behavior of a sheared Laponite suspension is investigated within a 1 mm gap under two different boundary conditions. No-slip conditions, ensured by using rough walls, lead to shear localization as already reported in various soft glassy materials. When apparent wall slip is allowed using a smooth geometry, the sample is shown to break up into macroscopic solid pieces that get slowly eroded by the surrounding fluidized material up to the point where the whole sample is fluid. Such a drastic effect of boundary conditions on yielding suggests the existence of some macroscopic characteristic length that could be connected to cooperativity effects in jammed materials under shear.

cond-mat.soft↗