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Soft amorphous materials are viscoelastic solids ubiquitously found around us, from clays and cementitious pastes to emulsions and physical gels encountered in food or biomedical engineering. Under an external deformation, these materials undergo a noteworthy transition from a solid to a liquid state that reshapes the material microstructure. This yielding transition was the main theme of a workshop held from January 9 to 13, 2023 at the Lorentz Center in Leiden. The manuscript presented here offers a critical perspective on the subject, synthesizing insights from the various brainstorming sessions and informal discussions that unfolded during this week of vibrant exchange of ideas. The result of these exchanges takes the form of a series of open questions that represent outstanding experimental, numerical, and theoretical challenges to be tackled in the near future.

We study the local dynamics of a thixotropic yield stress fluid that shows a pronounced non-monotonic flow curve. This mechanically unstable behavior is generally not observable from standard rheometry tests, resulting in a stress plateau that stems from the coexistence of a flowing band with an unyielded region below a critical shear rate  c . Combining ultrasound velocimetry with standard rheometry, we discover an original shear-banding scenario in the decreasing branch of the flow curve of model paraffin gels, in which the velocity profile of the flowing band is set by the applied shear rate  instead of  c . As a consequence, the material slips at the walls with a velocity that shows a non-trivial dependence on the applied shear rate. To capture our observations, we propose a differential version of the so-called lever rule, describing the extent of the flowing band and the evolution of wall slip with shear rate. This phenomenological model holds down to very low shear rates, at which the dimension of the flowing band becomes comparable to the size of the individual wax particles that constitute the gel microstructure, leading to cooperative effects. Our approach provides a framework where constraints imposed in the classical shear-banding scenario can be relaxed, with wall slip acting as an additional degree of freedom.

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 at an applied shear rate  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  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 of 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  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 to 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.

We couple rheometry and ultrasonic velocimetry to study experimentally the flow behavior of gels of colloidal calcite particles dispersed in water, while tuning the strength of the interparticle attraction through physico-chemistry. We unveil, for the first time in a colloidal gel, a direct connection between attractive interactions and the occurrence of shear bands, as well as stress fluctuations.

We study the motion of a sphere of diameter 330 μm embedded in a Carbopol microgel under the effect of the acoustic radiation pressure exerted by a focused ultrasonic field. The sphere motion within the microgel is tracked using videomicroscopy and compared to conventional creep and recovery measurements performed with a rheometer. We find that under moderate ultrasonic intensities, the sphere creeps as a power law of time with an exponent α ≃ 0.2 that is significantly smaller than the one inferred from global creep measurements below the yield stress of the microgel (α ≃ 0.4). Moreover, the sphere relaxation motion after creep and the global recovery are respectively consistent with these two different exponents. By allowing a rheological characterization at the scale of the sphere with forces of the order of micronewtons, the present experiments pave the way for acoustic "mesorheology" which probes volumes and forces an intermediate between standard macroscopic rheology and classical microrheology. They also open new questions about the effects of the geometry of the deformation field and of the sphere size and surface properties on the creep behaviour of soft materials.

Soft materials may break irreversibly upon applying sufficiently large shear oscillations, a process whose 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.

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.

We demonstrated recently that polyelectrolytes with cationic moieties along the chain and a single anionic head are able to form physical hydrogels due to the reversible nature of the head-to-body ionic bond. Here we generate a variety of such polyelectrolytes with various cationic moieties and counterion combinations starting from a common polymeric platform. We show that the rheological properties (shear modulus, critical strain) of the final hydrogels can be modulated over three orders of magnitude depending on the cation/anion pair. Our data fit remarkably well within a scaling model involving a supramolecular head-to-tail single file between cross-links, akin to the behaviour of pine-processionary caterpillar. This model allows the quantitative measure of the amount of counterion condensation from standard rheology procedure.

We report experimental results on the dynamics of a granular packing submitted to high-intensity focused ultrasound. Acoustic radiation pressure is shown to remotely induce local rearrangements within a pile as well as global motion around the focal spot in an initially jammed system. We demonstrate that this fluidization process is intermittent for a range of acoustic pressures and hysteretic when the pressure is cycled. Such a first-order-like unjamming transition is reproduced in numerical simulations in which the acoustic pressure field is modeled by a localized external force. Further analysis of the simulated packings suggests that in the intermittent regime unjamming is not associated with any noticeable prior structural signature. A simple two-state model based on effective temperatures is proposed to account for these findings.

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 σ0. The data are compatible with both exponential and power-law scalings with σ0, which hints at two possible interpretations of delayed yielding in terms of 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.

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 for a time tw before being subjected to a constant shear rate [small gamma, Greek, dot above]. We investigate in detail the effects of both tw and [small gamma, Greek, dot above] on the fluidization dynamics and build a detailed state diagram of the gel response to shear startup flows. The gel may display either 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 until 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 tw and [small gamma, Greek, dot above] values, although the very details of the fluidization scenario vary with [small gamma, Greek, dot above]. Finally, the critical shear rate [small gamma, Greek, dot above]* that separates steady-state shear-banding from steady-state homogeneous flow depends on the width of the shear cell and exhibits a nonlinear dependence with tw. Our work brings about valuable experimental data on transient flows of attractive dispersions, highlighting the subtle interplay between shear, wall slip and aging whose modeling constitutes a major challenge that has not been met yet.

Homogeneous polymer solutions are well known to exhibit viscoelastic flow instabilities: purely elastic when inertia is negligible and inertio-elastic otherwise. Recently, shear-banding wormlike micelle solutions were also discovered to follow a similar phenomenology. In the shear-banding regime, inertia is usually negligible so only purely elastic flows have been reported. Here, we investigate a non-shear-banding solution where inertia becomes significant, leading to flow patterns akin to the inertio-elastic regime of dilute polymer solutions. We show that the instability follows a supercritical bifurcation and we investigate the structure of the inertio-elastic vortices that develop above the onset.

The stress-induced yielding scenario of colloidal gels is investigated under rough boundary conditions by means of rheometry coupled with local velocity measurements. Under an applied shear stress σ, the fluidization of gels made of attractive carbon black particles dispersed in a mineral oil is shown to involve a previously unreported shear rate response γ dot above(t) characterized by two well-defined and separated timescales τc and τf. First γ dot above 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 whether plastic events take place or whether any shear transformation zone exists, such phenomena occur at a smaller scale. As a key result of this paper, the duration τc 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 σc, i.e. τc ∼ (σ - σc)(-β), with β = 2-3 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 with the full fluidization of the material which ends up being homogeneously sheared. The corresponding fluidization time τf robustly follows an exponential decay with the applied shear stress, i.e. τf = τ0 exp(-σ/σ0), as already reported for smooth boundary conditions. Varying the gel concentration C in a systematic fashion shows that the parameter σ0 and the yield stress σc exhibit similar power-law dependences with C. 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).