In periodically sheared suspensions there is a dynamical phase transition characterized by a critical strain amplitude $γ_c$ between an absorbing state where particle trajectories are reversible and an active state where trajectories are chaotic and diffusive. Repulsive non-hydrodynamic interactions between "colliding" particles' surfaces have been proposed as a source of this broken time reversal symmetry. A simple toy model called Random Organization qualitatively reproduces the dynamical features of this transition. Random Organization and other absorbing state models exhibit hyperuniformity, a strong suppression of density fluctuations on long length-scales quantified by a structure factor $S(q \rightarrow 0) \sim q^α$ with $α> 0$, at criticality. Here we show experimentally that the particles in periodically sheared suspensions organize into structures with anisotropic short-range order but isotropic, long-range hyperuniform order when oscillatory shear amplitudes approach $γ_c$.
The creation of disordered hyperuniform materials with potentially extraordinary optical properties requires a capacity to synthesize large samples that are effectively hyperuniform down to the nanoscale. Motivated by this challenge, we propose a fabrication protocol using binary superparamagnetic colloidal particles confined in a 2D plane. The strong and long-ranged dipolar interaction induced by a tunable magnetic field is free from screening effects that attenuates long-ranged electrostatic interactions in charged colloidal systems. Specifically, we find a family of optimal size ratios that…
The emergence of particle irreversibility in periodically driven colloidal suspensions has been interpreted as resulting either from a nonequilibrium phase transition to an absorbing state or from the chaotic nature of particle trajectories. Using a simple model of a driven suspension we show that a nonequilibrium phase transition is accompanied by hyperuniform static density fluctuations in the vicinity of the transition, where we also observe strong dynamic heterogeneities reminiscent of dynamics in glassy materials. We find that single particle dynamics becomes intermittent and strongly non…
We poorly understand the macroscopic properties of complex fluids and of amorphous bodies in general. This is mainly due to the interplay between phenomena at different levels and length-scales. In particular, it is not necessarily true that the microscopic level (dominated by direct interactions) coincides with the level where the continuum description comes into play. This is typically the case in the presence of structural inhomogeneities which are inherent to all structurally disordered states of matter below close packing. As a consequence, the macroscopic response to external fields of e…
We study the effect of shear flow on homogeneous crystal nucleation, using Brownian Dynamics simulations in combination with an umbrella sampling like technique. The symmetry breaking due to shear results in anisotropic radial distribution functions. The homogeneous shear rate suppresses crystal nucleation and leads to an increase of the size of the critical nucleus. These observations can be described by a simple, phenomenological extension of classical nucleation theory. In addition, we find that nuclei have a preferential orientation with respect to the direction of shear. On average the lo…
We examine the dynamics of two-dimensional colloidal systems using numerical simulations of a system with a drive applied to a thin region in the middle of the sample to produce a local shear. For a monodisperse colloidal assembly, we find a well defined decoupling transition separating a regime of elastic motion from a plastic phase where the particles in the driven region break away or decouple from the particles in the bulk, producing a shear band. For a bidisperse assembly, we find that the onset of a bulk disordering transition coincides with the broadening of the shear band. We identify …
We use confocal microscopy to study a random close packed sample of colloidal particles. We introduce an algorithm to estimate the size of each particle. Taking into account their sizes, we compute the compressibility of the sample as a function of wave vector $q$, and find that this compressibility vanishes linearly as $q \rightarrow 0$. The particle sizes must be considered to calculate the compressibility properly. These results also suggest that the experimental packing is hyperuniform.
We examine microstructural and mechanical changes which occur during oscillatory shear flow and reformation after flow cessation of an intermediate volume fraction colloidal gel using rheometry and Brownian Dynamics (BD) simulations. A model depletion colloid-polymer mixture is used, comprising of a hard sphere colloidal suspension with the addition of non-adsorbing linear polymer chains. Results reveal three distinct regimes depending on the strain amplitude of oscillatory shear. Large shear strain amplitudes fully break the structure which results into a more homogenous and stronger gel afte…
We show that the shear-induced solidification of dilute charge-stabilized (DLVO) colloids is due to the interplay between the shear-induced formation and breakage of large non-Brownian clusters. While their size is limited by breakage, their number density increases with the shearing-time. Upon flow cessation, the dense packing of clusters interconnects into a rigid state by means of grainy bonds, each involving a large number of primary colloidal bonds. The emerging picture of shear-driven solidification in dilute colloidal suspensions combines the gelation of Brownian systems with the jammin…
Structural defects are ubiquitous in condensed matter, and not always a nuisance. For example, they underlie phenomena such as Anderson localization and hyperuniformity, and they are now being exploited to engineer novel materials. Here, we show experimentally that the density of structural defects in a 2D binary colloidal crystal can be engineered with a random potential. We generate the random potential using an optical speckle pattern, whose induced forces act strongly on one species of particles (strong particles) and weakly on the other (weak particles). Thus, the strong particles are mor…
Jamming is a geometric phase transition occurring in dense particle systems in the absence of temperature. We use computer simulations to analyse the effect of thermal fluctuations on several signatures of the transition. We show that scaling laws for bulk and shear moduli only become relevant when thermal fluctuations are extremely small, and propose their relative ratio as a quantitative signature of jamming criticality. Despite the nonequilibrium nature of the transition, we find that thermally induced fluctuations and mechanical responses obey equilibrium fluctuation-dissipation relations …
Shear history plays an important role in determining the linear and nonlinear rheological response of colloidal gels and can be used for tuning their structure and flow properties. Increasing colloidal particle aspect ratio lowers the critical volume fraction for gelation due to an increase of the particle excluded volume. Using a combination of rheology and confocal microscopy we investigate the effect of steady and oscillatory pre-shear history on the structure and rheology of colloidal gels formed by silica spheres and rods of length L and diameter D (L/D = 10) dispersed in 11 M CsCl soluti…
The effects of thermal noise on particle rearrangements in colloidal suspensions undergoing cyclic shear are experimentally investigated using particle tracking methods. The experimental model system consists of polystyrene particles adsorbed at an oil- water interface, in which the particles exhibit small but non-negligible Brownian motion. We perform experiments on bidisperse (1 and 1.2 $μ$m in size) colloidal samples with area fractions ($ϕ$ ) of 0.20 and 0.32. Reversibility of particle rearrangements are characterized, and we show that unlike dense athermal systems, reversible clusters are…
The flow curves, viz. the curves of stationary stress under steady shearing, are obtained close to the glass transition in dense colloidal dispersions using asymptotic expansions in a schematic model of mode coupling theory. The shear thinning of the viscosity in fluid states and the yielding of glassy states is discussed. At the transition between fluid and shear-molten glass, simple and generalized Herschel-Bulkley laws are derived with power law exponents that can be computed for different particle interactions from the equilibrium structure factor.
We consider the nonlinear rheology of dense colloidal suspensions under a time-dependent simple shear flow. Starting from the Smoluchowski equation for interacting Brownian particles advected by shearing (ignoring fluctuations in fluid velocity) we develop a formalism which enables the calculation of time-dependent, far-from-equilibrium averages. Taking shear-stress as an example we derive exactly a generalized Green-Kubo relation, and an equation of motion for the transient density correlator, involving a three-time memory function. Mode coupling approximations give a closed constitutive equa…
Strongly confined colloidal dispersions under shear can exhibit a variety of dynamical phenomena, including depinning transitions and complex structural changes. Here, we investigate the behaviour of such systems under pure oscillatory shearing with shear rate $\dotγ(t) = \dotγ_0 \cos(ωt)$, as it is a common scenario in rheological experiments. The colloids' depinning behaviour is assessed from a particle level based on trajectories, obtained from overdamped Brownian Dynamics simulations. The numerical approach is complemented by an analytic one based on an effective single-particle model in t…
Granulation is a process whereby a dense colloidal suspension is converted into pasty granules (surrounded by air) by application of shear. Central to the stability of the granules is the capillary force arising from the interfacial tension between solvent and air. This force appears capable of maintaining a solvent granule in a jammed solid state, under conditions where the same amount of solvent and colloid could also exist as a flowable droplet. We argue that in the early stages of granulation the physics of dilatancy, which requires that a powder expand on shearing, is converted by capilla…
Langevin Dynamics simulations are used to study the effect of shear on a two-dimensional colloidal crystal confined by structured parallel walls. When walls are sheared very slowly, only two or three crystalline layers next to the walls move along with them, while the inner layers of the crystal are only slightly tilted. At higher shear velocities, this inner part of the crystal breaks into several pieces with different orientations. The velocity profile across the slit is reminiscent of shear-banding in flowing soft materials, where liquid and solid regions coexist; the difference, however, i…
Dense, disordered packings of particles are useful models of low-temperature amorphous phases of matter, biological systems, granular media, and colloidal systems. The study of dense packings of nonspherical particles enables one to ascertain how rotational degrees of freedom affect packing behavior. Here, we study superballs, a large family of deformations of the sphere, defined in three dimensions by $|x_1|^{2p}+|x_2|^{2p}+|x_3|^{2p}\leq1$, where $p>0$ is a deformation parameter indicating to what extent the shape deviates from a sphere. As $p$ increases from the sphere point ($p=1$), the su…
We present an experiment on crystallization of packings of macroscopic granular spheres. This system is often considered to be a model for thermally driven atomic or colloidal systems. Cyclically shearing a packing of frictional spheres, we observe a first order phase transition from a disordered to an ordered state. The ordered state consists of crystallites of mixed FCC and HCP symmetry that coexist with the amorphous bulk. The transition, initiated by homogeneous nucleation, overcomes a barrier at 64.5% volume fraction. Nucleation consists predominantly of the dissolving of small nuclei and…
The rheology of non-colloidal suspensions under cyclic shear is studied numerically. The main findings are a strain amplitude ($γ_0$) dependent response in the shear stress and second normal stress difference ($N_2$). Specifically, we find a reduced viscosity, an enhanced intracycle shear thinning, the onset of a finite $N_2$ and its frequency doubling, all near a critical strain amplitude $γ_c$ that scales with the volume fraction $ϕ$ as $γ_c \sim ϕ^{-2}$. These rheological changes also signify a reversible-irreversible transition (RIT), dividing stroboscopic particle dynamics into a reversib…
We have studied the effect of an external DC electric field (~kV/mm) on the rheological properties of colloidal suspensions consisting of aggregates of laponite particles in a silicone oil. Microscopy observations show that under application of an electric field greater than a triggering electric field E_c~0.6 kV/mm, laponite aggregates assemble into chain- and/or column-like structures in the oil. Without an applied electric field, the steady state shear behavior of such suspensions is Newtonian-like. Under application of an electric field larger than E_c, it changes dramatically as a result …
