Shear Jamming and Fragility of Suspensions in a Continuum Model with Elastic Constraints.

Under an applied traction, highly concentrated suspensions of solid particles in fluids can turn from a state in which they flow to a state in which they counteract the traction as an elastic solid: a shear-jammed state. Remarkably, the suspension can turn back to the flowing state simply by inverting the traction. A tensorial model is presented and tested in paradigmatic cases. We show that, to reproduce the phenomenology of shear jamming in generic geometries, it is necessary to link this effect to the elastic response supported by the suspension microstructure rather than to a divergence of the viscosity.

Shear Thickening and Jamming of Dense Suspensions: The "Roll" of Friction.

Particle-based simulations of discontinuous shear thickening (DST) and shear jamming (SJ) suspensions are used to study the role of stress-activated constraints, with an emphasis on resistance to gearlike rolling. Rolling friction decreases the volume fraction required for DST and SJ, in quantitative agreement with real-life suspensions with adhesive surface chemistries and "rough" particle shapes. It sets a distinct structure of the frictional force network compared to only sliding friction, and from a dynamical perspective leads to an increase in the velocity correlation length, in part responsible for the increased viscosity. The physics of rolling friction is thus a key element in achieving a comprehensive understanding of strongly shear-thickening materials.

Force transmission and the order parameter of shear thickening.

The origin of the abrupt shear thickening observed in some dense suspensions has been recently argued to be a transition from frictionless (lubricated) to frictional interactions between immersed particles. The Wyart-Cates rheological model, built on this scenario, introduced the concept of the fraction of frictional contacts f as the relevant order parameter for the shear thickening transition. Central to the model is the "equation-of-state" relating f to the applied stress σ, which is directly linked to the distribution of the normal components of non-hydrodynamic interparticle forces. Here, we develop a model for this force distribution, based on the so-called q-model, which we borrow from granular physics. This model explains the known f(σ) in the simple case of sphere contacts displaying only sliding friction, but also predicts strong deviation from this "usual" form when stronger kinds of constraints are applied on the relative motion. We verify these predictions in the case of contacts with rolling friction, in particular a broadening of the stress range over which shear thickening occurs. We finally discuss how a similar approach can be followed to predict f(σ) in systems with other variations from the canonical system of monodisperse spheres with sliding friction, in particular the case of large bidispersity.

Discontinuous shear thickening in Brownian suspensions by dynamic simulation.

Dynamic particle-scale numerical simulations are used to show that the shear thickening observed in dense colloidal, or Brownian, suspensions is of a similar nature to that observed in noncolloidal suspensions, i.e., a stress-induced transition from a flow of lubricated near-contacting particles to a flow of a frictionally contacting network of particles. Abrupt (or discontinuous) shear thickening is found to be a geometric rather than hydrodynamic phenomenon; it stems from the strong sensitivity of the jamming volume fraction to the nature of contact forces between suspended particles. The thickening obtained in a colloidal suspension of purely hard frictional spheres is qualitatively similar to experimental observations. However, the agreement cannot be made quantitative with only hydrodynamics, frictional contacts, and Brownian forces. Therefore, the role of a short-range repulsive potential mimicking the stabilization of actual suspensions on the thickening is studied. The effects of Brownian and repulsive forces on the onset stress can be combined in an additive manner. The simulations including Brownian and stabilizing forces show excellent agreement with experimental data for the viscosity η and the second normal stress difference N2.

Crystallization kinetics of binary colloidal monolayers.

Experiments and simulations are used to study the kinetics of crystal growth in a mixture of magnetic and nonmagnetic particles suspended in ferrofluid. The growth process is quantified using both a bond order parameter and a mean domain size parameter. The largest single crystals obtained in experiments consist of approximately 1000 particles and form if the area fraction is held between 65-70% and the field strength is kept in the range of 8.5-10.5 Oe. Simulations indicate that much larger single crystals containing as many as 5000 particles can be obtained under impurity-free conditions within a few hours. If our simulations are modified to include impurity concentrations as small as 1-2%, then the results agree quantitatively with the experiments. These findings provide an important step toward developing strategies for growing single crystals that are large enough to enable follow-on investigations across many subdisciplines in condensed matter physics.

Odd Response-Induced Phase Separation of Active Spinners.

Due to the breaking of time-reversal and parity symmetries and the presence of non-conservative microscopic interactions, active spinner fluids and solids respectively exhibit nondissipative odd viscosity and nonstorage odd elasticity, engendering phenomena unattainable in traditional passive or active systems. Here, we study the effects of odd viscosity and elasticity on phase behaviors of active spinner systems. We find the spinner fluid under a simple shear experiences an anisotropic gas-liquid phase separation driven by the odd-viscosity stress. This phase separation exhibits equilibrium-like behavior, with both binodal-like and spinodal curves and critical point. However, the formed dense liquid phase is unstable, since the odd elasticity instantly takes over the odd viscosity to condense the liquid into a solid-like phase. The unusual phase behavior essentially arises from the competition between thermal fluctuations and the odd response-induced effective attraction. Our results demonstrate that the cooperation of odd viscosity and elasticity can lead to exotic phase behavior, revealing their fundamental roles in phase transition.

Discontinuous shear thickening of frictional hard-sphere suspensions.

Discontinuous shear thickening (DST) observed in many dense athermal suspensions has proven difficult to understand and to reproduce by numerical simulation. By introducing a numerical scheme including both relevant hydrodynamic interactions and granularlike contacts, we show that contact friction is essential for having DST. Above a critical volume fraction, we observe the existence of two states: a low viscosity, contactless (hence, frictionless) state, and a high viscosity frictional shear jammed state. These two states are separated by a critical shear stress, associated with a critical shear rate where DST occurs. The shear jammed state is reminiscent of the jamming phase of granular matter. Continuous shear thickening is seen as a lower volume fraction vestige of the jamming transition.

Colloidal gelation with non-sticky particles.

Colloidal gels are widely applied in industry due to their rheological character-no flow takes place below the yield stress. Such property enables gels to maintain uniform distribution in practical formulations; otherwise, solid components may quickly sediment without the support of gel matrix. Compared with pure gels of sticky colloids, therefore, the composites of gel and non-sticky inclusions are more commonly encountered in reality. Through numerical simulations, we investigate the gelation process in such binary composites. We find that the non-sticky particles not only confine gelation in the form of an effective volume fraction, but also introduce another lengthscale that competes with the size of growing clusters in gel. The ratio of two key lengthscales in general controls the two effects. Using different gel models, we verify such a scenario within a wide range of parameter space, suggesting a potential universality in all classes of colloidal composites.

How surface roughness affects the interparticle interactions at a liquid interface.

HYPOTHESIS: Colloidal particles can be trapped at a liquid interface, which reduces the energetically costly interfacial area. Once at an interface, colloids undergo various self-assemblies and structural transitions due to shape-dependent interparticle interactions. Particles with rough surfaces receive increasing attention and have been applied in material design, such as Pickering emulsions and shear-thickening materials. However, the roughness effects on the interactions at a liquid interface remain less understood. EXPERIMENTS: Experimentally, particles with four surface roughnesses were designed and compared via isotherm measurements upon a uniaxial compression. At each stage of the compression, micrographic observations were conducted via the Blodgett method. Numerically, the compression of monolayer was simulated by using Langevin dynamics. Rough colloids were modelled as particles with capillary attraction and tangential constraints. FINDINGS: Sufficiently rough systems exhibit a non-trivial intermediate state between a gas-like state and a close-packed jamming state. This state is understood as a gel state due to roughness-induced capillary attraction. Roughness-induced friction lowers the jamming point. Furthermore, the tangential contact force owing to surface asperities can cause a gradual off-plane collapse of the compressed monolayer.

Restructuring of colloidal aggregates in shear flow: coupling interparticle contact models with Stokesian dynamics.

A method to couple interparticle contact models with Stokesian dynamics (SD) is introduced to simulate colloidal aggregates under flow conditions. The contact model mimics both the elastic and plastic behavior of the cohesive connections between particles within clusters. Owing to this, clusters can maintain their structures under low stress while restructuring or even breakage may occur under sufficiently high stress conditions. SD is an efficient method to deal with the long-ranged and many-body nature of hydrodynamic interactions for low Reynolds number flows. By using such a coupled model, the restructuring of colloidal aggregates under shear flows with stepwise increasing shear rates was studied. Irreversible compaction occurs due to the increase of hydrodynamic stress on clusters. Results show that the greater part of the fractal clusters are compacted to rod-shaped packed structures, while the others show isotropic compaction.

Nonmonotonic flow curves of shear thickening suspensions.

The discontinuous shear thickening (DST) of dense suspensions is a remarkable phenomenon in which the viscosity can increase by several orders of magnitude at a critical shear rate. It has the appearance of a first-order phase transition between two hypothetical "states" that we have recently identified as Stokes flows with lubricated or frictional contacts, respectively. Here we extend the analogy further by means of stress-controlled simulations and show the existence of a nonmonotonic steady-state flow curve analogous to a nonmonotonic equation of state. While we associate DST with an S-shaped flow curve, at volume fractions above the shear jamming transition the frictional state loses flowability and the flow curve reduces to an arch, permitting the system to flow only at small stresses. Whereas a thermodynamic transition leads to phase separation in the coexistence region, we observe a uniform shear flow all along the thickening transition. A stability analysis suggests that uniform shear may be mechanically stable for the small Reynolds numbers and system sizes in a rheometer.

Hydrodynamic stress on small colloidal aggregates in shear flow using Stokesian dynamics.

The hydrodynamic properties of rigid fractal aggregates have been investigated by considering their motion in shear flow in the Stokesian dynamics approach. Due to the high fluid viscosity and small particle inertia of colloidal systems, the total force and torque applied to the aggregate reach equilibrium values in a short time. Obtaining equilibrating motions for a number of independent samples, one can extract the average hydrodynamic characteristics of the given fractal aggregates. Despite the geometry of these objects being essentially disordered, the average drag-force distributions for aggregates show symmetric patterns. Moreover, these distributions collapse on a single master curve, characteristic of the nature of the aggregates, provided the positions of the particles are rescaled with the geometric radius of gyration. This result can be used to explain the reason why the stress acting on an aggregate and moments of the forces acting on contact points between particles follow power-law behaviors with the aggregate size. Moreover, the values of the exponents can be explained. As a consequence, considering cohesive force typical for colloidal particles, we find that even aggregates smaller than a few dozen particles must experience restructuring when typical shear flow is applied.