By combining aspects of the coherent and self intermediate scattering functions, measured by dynamical light scattering on a suspension of hard sphere-like particles, we show that the arrest of particle number density fluctuations spreads from the position of the main structure factor peak. Taking the velocity auto-correlation function into account we propose that as density fluctuations are arrested the system's ability to respond to diffusing momentum currents is impaired and, accordingly, the viscosity increases. From the stretching of the coherent intermediate scattering function we read a quantitative manifestation of the undissipated thermal energy, the source of those, ergodicity restoring, processes that short-circuit the sharp transition to a perfect glass.
We study the rheological response of dense suspensions of elliptical particles, with an aspect ratio equal to 3, under oscillatory shear flows and imposed pressure by numerical simulations. Like for the isotropic particles, we find that the oscillatory shear flows respect the Cox-Merz rule at large oscillatory strains but differ at low strains, with a lower viscosity than the steady shear and higher shear jamming packing fractions. However, unlike the isotropic cases (i.e., discs and spheres), frictionless ellipses get dynamically arrested in their initial orientational configuration at small …
We formulate a microscopic, force-level, activated dynamics-based statistical-mechanical theory for the continuous startup nonlinear shear-rheology of ultra-dense glass-forming hard-sphere fluids and colloidal suspensions in the context of the ECNLE approach. Activated structural relaxation is described as a coupled local-nonlocal event involving caging and longer-range collective elasticity which controls the characteristic stress relaxation time. Theoretical predictions for the deformation-induced mobility enhancement, onset of relaxation acceleration at low values of stress, strain, or shea…
Interfacially arrested melting in thin films: capillarity-driven suspension of phase transitions
Zhejiang Key Laboratory of Extreme Environment Functional Materials, Yiwu Research Institute of Fudan University（复旦大学义乌研究院极端环境功能材料浙江省重点实验室）；Shanghai Frontiers Science Research Base of Intelligent Optoelectronics and Perception, Institute of Optoelectronics, Fudan University（复旦大学光电研究院上海智能光电子与感知前沿科学基地）；Max Planck Institute of Colloids and Interfaces（马克斯·普朗克胶体与界面研究所）
A remarkable property of dense suspensions is that they can transform from liquid-like at rest to solid-like under sudden impact. Previous work showed that this impact-induced solidification involves rapidly moving jamming fronts; however, details of this process have remained unresolved. Here we use high-speed ultrasound imaging to probe non-invasively how the interior of a dense suspension responds to impact. Measuring the speed of sound we demonstrate that the solidification proceeds without a detectable increase in packing fraction, and imaging the evolving flow field we find that the shea…
Yield stress fluids are widely used in industrial application to arrest dense solid particles, which can be studied by using a concentrated emulsion as a model fluid. We show in experiments that particle sedimentation in emulsions cannot be predicted by the classical criterion for spheres embedded in a yield stress fluid. Phase separation processes take place, where a liquid layer forms and particle sedimentation is enhanced by the emulsion drainage. In addition, emulsion drainage can be arrested or enhanced by the amount of particles embedded in the emulsion. A minimal mathematical model is d…
At the surfaces of autophoretic colloids, slip velocities arise from local chemical gradients that are many-body functions of particle configuration and activity. For rapid chemical diffusion, coupled with slip-induced hydrodynamic interactions, we deduce the chemohydrodynamic forces and torques between colloids. Near a no-slip wall, the forces can be expressed as gradients of a non-equilibrium potential which, by tuning the type of activity, can be varied from repulsive to attractive. When this potential has a barrier, we find arrested phase separation with a mean cluster size set by competin…
A dilute non-interacting suspension of micro-swimmers exhibits a finite velocity variance and short-ranged correlations that decay over a swimmer length. For a suspension of interacting straight swimmers, however, pair-interactions leads to a non-decaying velocity covariance, and a variance that diverges logarithmically with system size. The divergence is arrested on inclusion of orientation decorrelation mechanisms. Results for suspensions of run-and-tumble particles (RTPs) are presented, where the underlying straight-swimmer divergence leads to a broad cross-over between the ballistic and di…
Dispersing small particles in a liquid can produce surprising behaviors when the solids fraction becomes large: rapid shearing drives these systems out of equilibrium and can lead to dramatic increases in viscosity (shear-thickening) or even solidification (shear jamming). These phenomena occur above a characteristic onset stress when particles are forced into frictional contact. Here we show via simulations how this can be understood within a framework that abstracts details of the forces acting at particle-particle contacts into general stress-activated constraints on relative particle movem…
We theoretically study the effect of external deformation on activated structural relaxation and elementary aspects of the nonlinear mechanical response of glassy hard sphere fluids in the context of the nonequilibrium version of the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory. ECNLE theory describes activated relaxation as a coupled local-nonlocal event involving local caging and longer range collective elasticity, with the latter becoming more important with increasing packing fraction. The central new question is how this physical picture, and the relative importance o…
Coalescence event in pendant and sessile drop is distinguished by the formation and evolution of the liquid bridge created upon singular contact. The bridge radius, $R$, is known to evolve as $R\sim t^b$, with power-law exponent, $b$, signifying the dominant governing forces. In this work, we experimentally explore the phenomenon in sub-classes of complex fluids namely, colloidal and non-colloidal suspensions that have particle hydrodynamic interactions as origin of viscoelasticity. Our observations suggest that such fluids have flow dependent thinning response with finite elasticity in shear …
The rotational Brownian motion of colloidal spheres in dense suspensions reflects local hydrodynamics and friction, both key to non-linear rheological phenomena such as shear-thickening and jamming, and transport in crowded environments, including intracellular migration and blood flow. To fully elucidate the role of rotational dynamics experimentally, it is crucial to measure the translational and rotational motion of all spheres simultaneously. Here, we develop compositionally uniform colloidal spheres with an off-centre, fully embedded core with a different fluorophore to the particle body,…
We theoretically study the non-monotonic (re-entrant) activated dynamics associated with a repulsive glass to fluid to attractive glass transition in high density particle suspensions interacting via strong short range attractive forces. The classic theoretical projection approximation that replaces all microscopic forces by a single effective force determined solely by equilibrium pair correlations is revisited based on the projectionless dynamic theory (PDT) that avoids force projection. A hybrid-PDT is formulated that explicitly quantifies how attractive forces induce dynamical constraints,…
We analyse the experimental particle current auto correlation function (CAF) of suspensions of hard spheres. Interactions between the particles are mediated by thermally activated acoustic excitations in the solvent. Those acoustic modes are tantamount to the system's (energy) microstates and by their orthogonality, each of those modes can be identified with an independent Brownian particle current. Accordingly, partitioning of the system's energy states is impressed on the CAF. This impression provides a novel measure of the entropy and location of a partitioning/entropy limit at a packing fr…
In this work we, study shear reversals of dense non-Brownian suspensions composed of cohesionless elliptical particles. By numerical simulations, we show that a new fragility appears for frictionless ellipses in the flowing states, where particles can flow indefinitely in one direction at applied shear stresses but shear-jams in the other direction upon shear stress reversal. This new fragility, absent in the isotropic particle case, is linked to the directional order of the elongated particles at steady shear and its reorientation at shear stress reversal, which forces the suspensions to pass…
We describe and summarize a class of minimal numerical models emerged from recent development of simulation methods for dense particle suspensions in overdamped linear flows. The main ingredients include (i) a frame-invariant, short-range lubrication model for spherical particles, and (ii) a soft-core, stick/slide frictional contact model activated when particles overlap. We implement a version of the model using a modified velocity-Verlet algorithm that explicitly solves the $N$-body dynamical system in $\mathcal{O}(cN)$ operations, where $c$ is a kernel constant depending on the cutoff of pa…
Forcing dense suspensions of non-cohesive particles through constrictions might either result in a continuous flow, an intermittent one, or indefinite interruption of flow, i.e., a clog. While one of the most important (and obvious) controlling parameters in such a system is the neck-to-particle size ratio, the role of the liquid driving method is not so obvious. On the one hand, wide-spread volume-controlled systems result in pressure and local liquid velocity increases upon eventual clogs. On the other hand, pressure-controlled systems result in a decrease of the flow through the constrictio…
Dense suspensions of hard particles in a liquid can exhibit strikingly counter-intuitive behavior, such as discontinuous shear thickening (DST) [1-8] and reversible shear jamming (SJ) into a state with finite yield stress [9-13]. Recent studies identified a stress-activated crossover from hydrodynamic interactions to frictional particle contacts to be key for these behaviors [2-4, 6-8, 10, 14]. However, many suspensions exhibit only DST and not SJ. Here we show that particle surface chemistry can play a central role in creating conditions that allow for SJ. We find the system's ability to form…
The sudden arrest of motion due to confinement is commonly observed via the clogging transition in the flow of particles through a constriction. We present results of a simple experiment to elucidate a similar transition in the bidirectional flow of two species in which two species of macroscopic particles with different densities are confined in a tube and suspended in a fluid of intermediate density. Counterflowing grains serve as mobile obstacles and clogging occurs without arch formation due to confinement. We measure the clogging or jamming probability $J$ as a function of number of parti…
We use 2D numerical simulations to study dense suspensions of non-Brownian hard particles using the Critical Load Model (CLM) under constant confining pressures. This simple model shows discontinuous shear thickening (DST) as the tangential forces get activated upon increased shear stresses. By parameterizing a simple binary system of frictional and non-frictional particles of different proportions we show that the jamming packing fraction, at which the viscosity diverges, is controlled by the fraction of frictional contacts. The viscosity of dense suspensions can thereby be expressed as a fun…
Colloidal suspensions have long been studied as a model for atomic and molecular systems, due to the ability to fluorescently label and individually track each particle, yielding particle-resolved structural information. This allows various local order parameters to be probed that are otherwise inaccessible for a comparable molecular system. For phase transitions such as crystallisation, appropriate order parameters which emphasise 6-fold symmetry are a natural choice, but for vitrification the choice of order parameter is less clear cut. Previous work has highlighted the importance of icosahe…
The aggregation of attractive colloids has been extensively studied from both theoretical and experimental perspectives as the fraction of solid particles is changed, and the range, type and strength of attractive or repulsive forces between particles varies. The resulting gels consisting of disordered assemblies of attractive colloidal particles, have also been investigated with regards to percolation, phase separation, and the mechanical characteristics of the resulting fractal networks. Despite tremendous progress in our understanding of the gelation process, and the exploration of differen…
When suspended particles are pushed by liquid flow through a constricted channel they might either pass the bottleneck without trouble or encounter a permanent clog that will stop them forever. However, they may also flow intermittently with great sensitivity to the neck-to-particle size ratio D/d. In this work, we experimentally explore the limits of the intermittent regime for a dense suspension through a single bottleneck as a function of this parameter. To this end, we make use of high time- and space-resolution experiments to obtain the distributions of arrest times T between successive b…
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 gear-like 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 res…
Shear thickening of suspensions is studied by discrete-particle simulation, accounting for hydrodynamic, repulsive, and contact forces. The contact forces, including friction, are activated when the imposed shear stress $σ$ is able to overcome the repulsive force. The simulation method captures strong continuous and discontinuous shear thickening (CST and DST) in the range of solid volume fraction $0.54 \le ϕ\le 0.56$ studied here. This work presents characteristics of the contact force network developed in the suspension under shear. The number of frictional contacts per particle $Z$ is shown…
The dynamical arrest of attractive colloidal particles into out-of-equilibrium structures, known as gelation, is central to biophysics, materials science, nanotechnology, and food and cosmetic applications, but a complete understanding is lacking. In particular, for intermediate particle density and attraction, the structure formation process remains unclear. Here, we show that the gelation of short-range attractive particles is governed by a nonequilibrium percolation process. We combine experiments on critical Casimir colloidal suspensions, numerical simulations, and analytical modeling with…
Fine particle suspensions (such as cornstarch mixed with water) exhibit dramatic changes in viscosity when sheared, producing fascinating behaviors that captivate children and rheologists alike. Recent examination of these mixtures in simple flow geometries suggests inter-granular repulsion is central to this effect --- for mixtures at rest or shearing slowly, repulsion prevents frictional contacts from forming between particles, whereas, when sheared more forcefully, granular stresses overcome the repulsion allowing particles to interact frictionally and form microscopic structures that resis…
