arXiv subjects

Arnaud Poulesquen

Publications and source records attributed to Arnaud Poulesquen.

6 recordsLinked to original sources

arXiv2025

Anti-thixotropic dynamics in attractive colloidal dispersions: a shear restructuring driven by elastic stresses

Due to rich rheological properties, dispersions of attractive colloidal particles are ubiquitous in industries. Specifically, upon experiencing a sudden reduction in shear rate, these dispersions may exhibit transient behaviors such as thixotropy-where viscosity increases over time-and anti-thixotropy, characterized by an initial viscosity decrease before reaching a steady state. While thixotropy has been described as a competition between structure buildup and disruption, the mechanisms of anti-thixotropy remain poorly understood. Here, we investigate the anti-thixotropic dynamics of carbon black particles dispersed in oil-a system known for exhibiting anti-thixotropy-through flow step-down experiments. Using a multi-technique approach combining rheology with velocimetry and structural characterizations, we show that viscosity decrease results from a decrease in wall slip concomitant to shear-induced structural rearrangements, indicating a transition from a dynamical network of fractal clusters into a network of loosely connected dense agglomerates. Additionally, after a characteristic anti-thixotropic time $τ$, a steady flow is reached. This time $τ$ diverges with increasing shear rate at a critical value corresponding to a Mason number of one, indicating that anti-thixotropy occurs only when colloidal attraction outweighs viscous forces. More precisely, we show that the structural rearrangement underpinning the viscosity decrease is mediated by elastic stresses $σ_e$, such that $τ\propto σ_e^{-3}$. Finally, on long time scales, the steady state is linked to a microstructure with nearly zero yield stress, indicating a loss of flow memory. These findings provide a mechanism for anti-thixotropy and suggest pathways for controlling viscosity and yield stress in attractive colloidal dispersions.

cond-mat.soft↗

arXiv2024

Wall slip and bulk flow heterogeneity in a sludge under shear

We investigate the shear flow of a sludge mimicking slurries produced by the nuclear industry and constituted of a dispersion of non-Brownian particles into an attractive colloidal dispersion at a total solid volume fraction of about 10%. Combining rheometry and ultrasound flow imaging, we show that, upon decreasing the shear rate, the flow transitions from a homogeneous shear profile in the bulk to a fully arrested plug-like state with total wall slip, through an oscillatory regime where strong fluctuations of the slip velocity propagate along the vorticity direction. When the shear stress is imposed close to the yield stress, the shear rate presents large, quasi-periodic peaks, associated with the propagation of local stick-and-slip events along the vorticity direction. Such complex dynamics, reminiscent of similar phenomena reported in much denser suspensions, highlight the importance of local flow characterization to fully understand sludge rheology.

cond-mat.soft↗

arXiv2024

Attractive carbon black dispersions: structural and mechanical responses to shear

The rheological behavior of colloidal dispersions is of paramount importance in a wide range of applications, including construction materials, energy storage systems and food industry products. These dispersions consistently exhibit non-Newtonian behaviors, a consequence of intricate interplays involving colloids morphology, volume fraction, and inter-particle forces. Understanding how colloids structure under flow remains a challenge, particularly in the presence of attractive forces leading to clusters formation. In this study, we adopt a synergistic approach, combining rheology with ultra small-angle X-ray scattering (USAXS), to probe the flow-induced structural transformations of attractive carbon black (CB) dispersions and their effects on the viscosity. Our key findings can be summarized as follow. First, testing different CB volume fractions, in the high shear rate hydrodynamic regime, CB particles aggregate to form fractal clusters. Their size conforms to a power law of the shear rate, $ξ_c \propto \dotγ^{-m}$, with $m\simeq 0.5$. Second, drawing insights from the fractal structure of clusters, we compute an effective volume fraction $ϕ_{\mathrm{eff}}$ and find that microstructural models adeptly account for the hydrodynamic stress contributions. We identify a critical shear rate $\dot{γ^*}$ and a critical volume fraction $ϕ_{\mathrm{eff}}^{*}$, at which the clusters percolate to form a dynamical network.

cond-mat.soft↗

arXiv2022

Interpenetration of fractal clusters drives elasticity in colloidal gels formed upon flow cessation

Colloidal gels are out of equilibrium soft solids composed of attractive Brownian particles that form a space-spanning network at low volume fractions. The elastic properties of these systems result from the network microstructure, which is very sensitive to shear history. Here, we take advantage of such sensitivity to tune the viscoelastic properties of a colloidal gel made of carbon black nanoparticles. Starting from a fluidized state under an applied shear rate $\dot γ_0$, we use an abrupt flow cessation to trigger a liquid-to-solid transition. We observe that the resulting gel is all the more elastic when the shear rate $\dot γ_0$ is low and that the viscoelastic spectra can be mapped on a master curve. Moreover, coupling rheometry to small angle X-ray scattering allows us to show that the gel microstructure is different from gels solely formed by thermal agitation where only two length scales are observed: the dimension of the colloidal and the dimension the fractal aggregates. Competition between shear and thermal energy leads to gels with three characteristic length scales. Such gels structure in a percolated network of fractal clusters that interpenetrate each other. Experiments on gels prepared with various shear histories reveal that cluster interpenetration increases with decreasing values of the shear rate $\dot γ_0$ applied before flow cessation. These observations strongly suggest that cluster interpenetration drives the gel elasticity, which we confirm using a structural model. Our results, which are in stark contrast with previous literature, where gel elasticity was either linked to cluster connectivity or to bending modes, highlight a novel local parameter controlling the macroscopic viscoelastic properties of colloidal gels.

cond-mat.soft↗

arXiv2022

Aggregation and disaggregation processes in clusters of particles: simple numerical and theoretical insights of the competition in 2D geometries

Aggregation and disaggregation of clusters of attractive particles under flow are studied from numerical and theoretical points of view. Two-dimensional molecular dynamics simulations of both Couette and Poiseuille flows highlight the growth of the average steady-state cluster size as a power law of the adhesion number, a dimensionless number that quantifies the ratio of attractive forces to shear stress. Such a power-law scaling results from the competition between aggregation and disaggregation processes, as already reported in the literature. Here, we rationalize this behavior through a model based on an energy function, which minimization yields the power-law exponent in terms of the cluster fractal dimension, in good agreement with the present simulations and with previous works.

cond-mat.soft↗

arXiv2020

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↗