arXiv subjects

Thibaut Divoux

Publications and source records attributed to Thibaut Divoux.

At least 55 records · Page 3Linked to original sources

arXiv2017

Yield Stress Materials in Soft Condensed Matter

We present a comprehensive review of the physical behavior of yield stress materials in soft condensed matter, which encompass a broad range of materials from colloidal assemblies and gels to emulsions and non-Brownian suspensions. All these disordered materials display a nonlinear flow behavior in response to external mechanical forces, due to the existence of a finite force threshold for flow to occur: the yield stress. We discuss both the physical origin and rheological consequences associated with this nonlinear behavior, and give an overview of experimental techniques available to measure the yield stress. We discuss recent progress concerning a microscopic theoretical description of the flow dynamics of yield stress materials, emphasizing in particular the role played by relaxation time scales, the interplay between shear flow and aging behavior, the existence of inhomogeneous shear flows and shear bands, wall slip, and non-local effects in confined geometries.

cond-mat.soft↗

arXiv2017

Understanding rheological hysteresis in soft glassy materials

Motivated by recent experimental studies of rheological hysteresis in soft glassy materials, we study numerically strain rate sweeps in simple yield stress fluids and viscosity bifurcating yield stress fluids. Our simulations of downward followed by upward strain rate sweeps, performed within fluidity models and the soft glassy rheology model, successfully capture the experimentally observed monotonic decrease of the area of the rheological hysteresis loop with sweep time in simple yield stress fluids, and the bell shaped dependence of hysteresis loop area on sweep time in viscosity bifurcating fluids. We provide arguments explaining these two different functional forms in terms of differing tendencies of simple and viscosity bifurcating fluids to form shear bands during the sweeps, and show that the banding behaviour captured by our simulations indeed agrees with that reported experimentally. We also discuss the difference in hysteresis behaviour between inelastic and viscoelastic fluids. Our simulations qualitatively agree with the experimental data discussed here for four different soft glassy materials.

cond-mat.soft↗

arXiv2017

Nonlinear viscoelasticity and generalized failure criterion for polymer gels

Polymer gels behave as soft viscoelastic solids and exhibit a generic nonlinear mechanical response characterized by pronounced stiffening prior to irreversible failure, most often through macroscopic fractures. Here, we aim at capturing the latter scenario for a protein gel using a nonlinear integral constitutive equation built upon ($i$) the linear viscoelastic response of the gel, here well described by a power-law relaxation modulus, and ($ii$) the nonlinear viscoelastic properties of the gel, encoded into a "damping function". Such formalism predicts quantitatively the gel mechanical response to a shear start-up experiment, up to the onset of macroscopic failure. Moreover, as the gel failure involves the irreversible growth of macroscopic cracks, we couple the latter stress response with Bailey's durability criterion for brittle solids in order to predict the critical values of the stress $σ_c$ and strain $γ_c$ at the failure point, and how they scale with the applied shear rate. The excellent agreement between theory and experiments suggests that the crack growth in this soft viscoelastic gel is a Markovian process, and that Baileys' criterion extends well beyond hard materials such as metals, glasses, or minerals.

cond-mat.soft↗

arXiv2016

Drying of agarose gels monitored by in-situ interferometry

Hydrogels behave as viscoelastic soft solids and display a porous microstructure filled with water with typical amounts of 90\%~w/w or more. As such, these materials are highly sensitive to water loss through evaporation, which impacts their mechanical properties. Yet, aside from scattered empirical observations, little is known about the gel drying kinetics for which there is a lack of temporally and spatially resolved measurements. Here we report a benchmark study of the slow drying of agarose gels cast in cylindrical Petri dishes. The weak adhesion of the gel to the lateral wall of the dish guarantees that the gel diameter remains constant during the drying process and that the gel shrinkage is purely vertical. The thinning rate is monitored by in-situ interferometry using a Michelson interferometer. The displacement of interference fringes are analyzed using an original spatiotemporal filtering method, which allows us to measure local thinning rates of about 10~nm/s with high accuracy. Experiments conducted at different positions along the gel radius show that the gel thins locally with a constant velocity before experiencing a sudden collapse at the end of the drying process. We further use the thinning rate measured at the center of the dish during the early stage of the drying process as a robust observable to quantify the role of additives on the gel drying kinetics and compare gels of different compositions. Our work exemplifies interferometry as a powerful tool to quantify the impact of minute amounts of additives on the drying of biopolymer gels.

cond-mat.soft↗

arXiv2016

Simultaneous rheo-electric measurements of strongly conductive complex fluids

We introduce a novel apparatus designed for stress-controlled rheometers to perform simultaneous rheological and electrical measurements on strongly conductive complex fluids under shear. By means of a non-toxic liquid metal at room temperature, the electrical connection to the rotating shaft is completed with minimal additional mechanical friction, allowing for simultaneous stress measurements as low as 1 Pa. We use the capabilities of this design to perform an extensive set of rheo-electric experiments on gels formulated from attractive carbon black particles, at concentrations ranging from 4 to 15% wt. First, experiments on gels at rest prepared with different shear history show a robust power-law scaling between the elastic modulus $G'_0$ and the conductivity $σ_0$ of the gels, i.e. $G'_0 \sim σ_0^α$, with $α=1.65 \pm 0.04$ independently of the gel concentration. Second, conductivity measurements performed simultaneously with creep experiments reveal for the first time that plastic events take place in the bulk while the shear rate decreases as a weak power law of time in the early stage of the experiment. The subsequent evolution of the conductivity and shear rate allows us to propose a local yielding scenario that is in agreement with previous velocimetry measurements. Finally, we determine the constitutive rheological and electrical behavior of carbon black gels. Corrections first introduced for mechanical measurements are carefully extended to electrical measurements to accurately distinguish between bulk and surface contributions to the conductivity. As an illustrative example, we examine the constitutive rheo-electric properties of five carbon black gels of different grades, and demonstrate the relevance of the novel rheo-electric apparatus as a versatile characterization tool for strongly conductive complex fluids and their applications.

cond-mat.mtrl-sci↗

arXiv2016

Overcooked agar solutions: impact on the structural and mechanical properties of agar gels

Thermoreversible hydrogels are commonly prepared by cooling down to ambient temperature, aqueous polymer solutions first brought to a boil. The incubation time of the polymer solution at such a high temperature is traditionally kept to a minimum to minimize its impact on the subsequent gelation. Here we study the effect of a prolonged heating of a 1.5\% w/w agar solution at $T=80^{\circ}$C, well above the gelling temperature. The incubation time $\mathcal{T}$ of the polysaccharide solution is varied from a few hours up to five days. We show that the agar solution ages as the result of both the hydrolysis and the intramolecular oxidation of the polysaccharides. As a consequence, both the viscosity and the pH of the solution decrease continuously during the incubation period. Furthermore, samples withdrew at different incubation times are cooled down to form gels which structure and mechanical properties are systematically determined. Cryo-microscopy and X-ray diffraction experiments reveal that agar gels formed from solutions of increasing incubation times, display a coarser microstructure composed of micron-sized foils which result from the condensation of the polysaccharides and contrast with the fibrous-like microstructure of gels prepared from a fresh agar solution. Along with structural changes, a prolonged incubation time of the polymer solution at $T=80^{\circ}$C leads to weaker agar gels of significantly lower shear elastic modulus. Moreover, extensive macro-indentation experiments coupled to direct visualization show that increasing the incubation time of the agar solution up to a few days decreases the yield strain of the gel, while the rupture scenario turns continuously from brittle to ductile-like. Our study suggests that the incubation time of agar solutions at high temperature could be used to tune the mechanical properties of agar-based gels.

cond-mat.mtrl-sci↗

arXiv2016

Normal force controlled rheology applied to agar gelation

A wide range of thermoreversible gels are prepared by cooling down to ambient temperature hot aqueous polymer solutions. During the sol-gel transition, such materials may experience a volume contraction which is traditionally overlooked as rheological measurements are usually performed in geometries of constant volume. In this article, we revisit the formation of 1.5\% wt. agar gels through a series of benchmark rheological experiments performed with a plate-plate geometry. We demonstrate on that particular gel of polysaccharides that the contraction associated with the sol/gel transition cannot be neglected. Indeed, imposing a constant gap width during the gelation results in the strain hardening of the sample, as evidenced by the large negative normal force that develops. Such hardening leads to the slow drift in time of the gel elastic modulus $G'$ towards ever larger values, and thus to an erroneous estimate of $G'$. As an alternative, we show that imposing a constant normal force equals to zero during the gelation, instead of a constant gap width, suppresses the hardening as the decrease of the gap compensates for the sample contraction. Using normal force controlled rheology, we then investigate the impact of thermal history on 1.5\% wt. agar gels. We show that neither the value of the cooling rate, nor the introduction of a constant temperature stage during the cooling process influence the gel elastic properties. Instead, $G'$ only depends on the terminal temperature reached at the end of the cooling ramp, as confirmed by direct imaging of the gel microstructure by cryoelectron microscopy. The present work offers an extensive review of the technical difficulties associated with the rheology of hydrogels and paves the way for a systematic use of normal force controlled rheology to monitor non-isochoric processes.

cond-mat.soft↗

arXiv2015

Avalanche-like fluidization of a non-Brownian particle gel

We report on the fluidization dynamics of an attractive gel composed of non-Brownian particles made of fused silica colloids. Extensive rheology coupled to ultrasonic velocimetry allows us to characterize the global stress response together with the local dynamics of the gel during shear startup experiments. In practice, after being rejuvenated by a preshear, the gel is left to age during a time $t_w$ before being submitted to a constant shear rate $\dot γ$. We investigate in detail the effects of both $t_w$ and $\dot γ$ on the fluidization dynamics and build a detailed state diagram of the gel response to shear startup flows. The gel may either display transient shear banding towards complete fluidization, or steady-state shear banding. In the former case, we unravel that the progressive fluidization occurs by successive steps that appear as peaks on the global stress relaxation signal. Flow imaging reveals that the shear band grows up to complete fluidization of the material by sudden avalanche-like events which are distributed heterogeneously along the vorticity direction and correlated to large peaks in the slip velocity at the moving wall. These features are robust over a wide range of values of $t_w$ and $\dot γ$, although the very details of the fluidization scenario vary with $\dot γ$. Finally, the critical shear rate $\dot γ^*$ that separates steady-state shear-banding from steady-state homogeneous flow depends on the width on the shear cell and exhibits a nonlinear dependence with $t_w$. Our work brings about valuable experimental data on transient flows of attractive dispersions, highlighting the subtle interplay between shear, wall slip and aging which modeling constitutes a major challenge that has not been met yet.

cond-mat.soft↗

arXiv2015

Wall slip across the jamming transition of soft thermoresponsive particles

Flows of suspensions are often affected by wall slip, that is the fluid velocity $v_{f}$ in the vicinity of a boundary differs from the wall velocity $v_{w}$ due to the presence of a lubrication layer. While the slip velocity $v_s=\vert v_{f}-v_{w}\vert$ robustly scales linearly with the stress $σ$ at the wall in dilute suspensions, there is no consensus regarding denser suspensions that are sheared in the bulk, for which slip velocities have been reported to scale as a $v_s\proptoσ^p$ with exponents $p$ inconsistently ranging between 0 and 2. Here we focus on a suspension of soft thermoresponsive particles and show that $v_s$ actually scales as a power law of the viscous stress $σ-σ_c$, where $σ_c$ denotes the yield stress of the bulk material. By tuning the temperature across the jamming transition, we further demonstrate that this scaling holds true over a large range of packing fractions $ϕ$ on both sides of the jamming point and that the exponent $p$ increases continuously with $ϕ$, from $p=1$ in the case of dilute suspensions to $p=2$ for jammed assemblies. These results allow us to successfully revisit inconsistent data from the literature and paves the way for a continuous description of wall slip above and below jamming.

cond-mat.soft↗

arXiv2015

Shear Banding of Complex Fluids

Even in simple geometries many complex fluids display non-trivial flow fields, with regions where shear is concentrated. The possibility for such shear banding has been known since several decades, but the recent years have seen an upsurge of studies offering an ever more precise understanding of the phenomenon. The development of new techniques to probe the flow on multiple scales and with increasing spatial and temporal resolution has opened the possibility for a synthesis of the many phenomena that could only have been thought of separately before. In this review, we bring together recent research on shear banding in polymeric and on soft glassy materials, and highlight their similarities and disparities.

cond-mat.soft↗

arXiv2015

Syneresis and delayed detachment in agar plates

Biogels made of crosslinked polymers such as proteins or polysaccharides behave as porous soft solids and store large amount of solvent. These gels undergo spontaneous aging, called syneresis that consists in the shrinkage of the gel matrix and the progressive expulsion of the solvent. As a result, a biogel originally casted in a container often lose contact with the container sidewalls, and the detachment time is a priori difficult to anticipate since it may occur over variable time spans (from hours to days). Here we report on the syneresis phenomena in agar plates that consist in Petri dishes filled with a gel mainly composed of agar. Direct observations and speckle pattern correlation analysis allow us to rationalize the delayed detachment of the gel from the sidewall of the Petri dish. The detachment time $t^*$ is surprisingly not controlled by the mass loss as one would intuitively expect. Instead, $t^*$ is strongly correlated to the gel minimum thickness $e_{min}$ measured along the sidewall of the plate, and increases as a robust function of $e_{min}$ independently of the prior mass-loss history. Time-resolved correlation spectroscopy atypically applied to such weakly diffusive media gives access to the local thinning rate of the gel. This technique also allows us to detect the gel micro-displacements that are triggered by the water evaporation prior to the detachment, and even to anticipate the latter from a few hours. Our work provides observables to predict the detachment time of agar gels in dishes, and highlights the relevance of speckle pattern correlation analysis for the quantitative investigation of the syneresis dynamics in biopolymer gels.

cond-mat.soft↗

arXiv2014

Creep and Fracture of a Protein Gel under Stress

Biomaterials such as protein or polysaccharide gels are known to behave qualitatively as soft solids and to rupture under an external load. Combining optical and ultrasonic imaging to shear rheology we show that the failure scenario of a protein gel is reminiscent of brittle solids: after a primary creep regime characterized by a power-law behavior which exponent is fully accounted for by linear viscoelasticity, fractures nucleate and grow logarithmically perpendicularly to shear, up to the sudden rupture of the gel. A single equation accounting for those two successive processes nicely captures the full rheological response. The failure time follows a decreasing power law with the applied shear stress, similar to the Basquin law of fatigue for solids. These results are in excellent agreement with recent fiber-bundle models that include damage accumulation on elastic fibers and exemplify protein gels as model, brittle-like soft solids.

cond-mat.soft↗

arXiv2013

Timescales in creep and yielding of attractive gels

The stress-induced yielding scenario of colloidal gels is investigated under rough boundary conditions by means of rheometry coupled to local velocity measurements. Under an applied shear stress, the fluidization of gels made of attractive carbon black particles suspended in a mineral oil is shown to involve a previously unreported shear rate response $\dot γ(t)$ characterized by two well-defined and separated timescales $τ_c$ and $τ_f$. First $\dot γ(t)$ decreases as a weak power law strongly reminiscent of the primary creep observed in numerous crystalline and amorphous solids, coined the "Andrade creep." We show that the bulk deformation remains homogeneous at the micron scale, which demonstrates that if plastic events take place or if any shear transformation zone exists, such phenomena occur at a smaller scale. As a key result of this paper, the duration $τ_c$ of this creep regime decreases as a power law of the viscous stress, defined as the difference between the applied stress and the yield stress with an exponent ranging between 2 and 3 depending on the gel concentration. The end of this first regime is marked by a jump of the shear rate by several orders of magnitude, while the gel slowly slides as a solid block experiencing strong wall slip at both walls, despite rough boundary conditions. Finally, a second sudden increase of the shear rate is concomitant to the full fluidization of the material which ends up being homogeneously sheared. The corresponding fluidization time $τ_f$ robustly follows an exponential decay with the applied shear stress as already reported for smooth boundary conditions. Finally, we highlight a few features that are common to attractive colloidal gels and to solid materials by discussing our results in the framework of theoretical approaches of solid rupture (kinetic, fiber bundle, and transient network models).

cond-mat.soft↗

arXiv2013

Yielding dynamics of a Herschel-Bulkley fluid: a critical-like fluidization behaviour

The shear-induced fluidization of a carbopol microgel is investigated during long start-up experiments using combined rheology and velocimetry in Couette cells of varying gap widths and boundary conditions. As already described in [Divoux et al., {\it Phys. Rev. Lett.}, 2010, {\bf 104}, 208301], we show that the fluidization process of this simple yield stress fluid involves a transient shear-banding regime whose duration $τ_f$ decreases as a power law of the applied shear rate $\gp$. Here we go one step further by an exhaustive investigation of the influence of the shearing geometry through the gap width $e$ and the boundary conditions. While slip conditions at the walls seem to have a negligible influence on the fluidization time $τ_f$, different fluidization processes are observed depending on $\gp$ and $e$: the shear band remains almost stationary for several hours at low shear rates or small gap widths before strong fluctuations lead to a homogeneous flow, whereas at larger values of $\gp$ or $e$, the transient shear band is seen to invade the whole gap in a much smoother way. Still, the power-law behaviour appears as very robust and hints to critical-like dynamics. To further discuss these results, we propose (i) a qualitative scenario to explain the induction-like period that precedes full fluidization and (ii) an analogy with critical phenomena that naturally leads to the observed power laws if one assumes that the yield point is the critical point of an underlying out-of-equilibrium phase transition.

cond-mat.soft↗

arXiv2013

Insights on the local dynamics induced by thermal cycling in granular matter

In this letter, we report results on the effect of temperature variations on a granular assembly through Molecular Dynamic simulations of a 2D granular column. Periodic dilation of the grains are shown to perfectly mimic such thermal cycling, and allows to rationalize the link between the compaction process, the local grains dynamics and finite size effects. Here we show that the individual grain properties, namely their roughness and elastic modulus define a minimal cycling amplitude of temperature ΔTc below which the dynamics is intermittent and spatially heterogeneous while confined into localized regions recently coined "hot spot" [Amon et al., Phys. Rev. Lett. 108, 135502 (2012)]. Above ΔTc, the whole column flows while the grains dynamics ranges continuously from cage-like at the bottom of the column to purely diffusive at the top. Our results provide a solid framework for the futur use of thermal cycling as an alternate driving method for soft glassy materials.

cond-mat.soft↗

arXiv2012

Rheological hysteresis in soft glassy materials

The nonlinear rheology of a soft glassy material is captured by its constitutive relation, shear stress vs shear rate, which is most generally obtained by sweeping up or down the shear rate over a finite temporal window. For a huge amount of complex fluids, the up and down sweeps do not superimpose and define a rheological hysteresis loop. By means of extensive rheometry coupled to time-resolved velocimetry, we unravel the local scenario involved in rheological hysteresis for various types of well-studied soft materials. We introduce two observables that quantify the hysteresis in macroscopic rheology and local velocimetry respectively, as a function of the sweep rate δt^{-1}. Strikingly, both observables present a robust maximum with δt, which defines a single material-dependent timescale that grows continuously from vanishingly small values in simple yield stress fluids to large values for strongly time-dependent materials. In line with recent theoretical arguments, these experimental results hint at a universal timescale-based framework for soft glassy materials, where inhomogeneous flows characterized by shear bands and/or pluglike flow play a central role.

cond-mat.soft↗

arXiv2011

Degassing cascades in a shear-thinning viscoelastic fluid

We report the experimental study of the degassing dynamics through a thin layer of shear-thinning viscoelastic fluid (CTAB/NaSal solution), when a constant air flow is imposed at its bottom. Over a large range of parameters, the air is periodically released through series of successive bubbles, hereafter named {\it cascades}. Each cascade is followed by a continuous degassing, lasting for several seconds, corresponding to an open channel crossing the fluid layer. The periodicity between two cascades does not depend on the injected flow-rate. Inside one cascade, the properties of the overpressure signal associated with the successive bubbles vary continuously. The pressure threshold above which the fluid starts flowing, fluid deformation and pressure drop due to degassing through the thin fluid layer can be simply described by a Maxwell model. We point out that monitoring the evolution inside the cascades provides a direct access to the characteristic relaxation time associated with the fluid rheology.

physics.flu-dyn↗

arXiv2011

Influence of Non-Newtonian rheology on magma degassing

Many volcanoes exhibit temporal changes in their degassing process, from rapid gas puffing to lava fountaining and long-lasting quiescent passive degassing periods. This range of behaviors has been explained in terms of changes in gas flux and/or magma input rate. We report here a simple laboratory experiment which shows that the non- Newtonian rheology of magma can be responsible, alone, for such intriguing behavior, even in a stationary gas flux regime. We inject a constant gas flow-rate Q at the bottom of a non-Newtonian fluid column, and demonstrate the existence of a critical flow rate Q* above which the system spontaneously alternates between a bubbling and a channeling regime, where a gas channel crosses the entire fluid column. The threshold Q* depends on the fluid rheological properties which are controlled, in particular, by the gas volume fraction (or void fraction) ϕ. When ϕ increases, Q* decreases and the degassing regime changes. Non-Newtonian properties of magma might therefore play a crucial role in volcanic eruption dynamics.

physics.geo-ph↗