Recovery of ground-state degeneracy in two-dimensional square ice is a significant challenge in the field of geometric frustration with far-reaching fundamental implications, such as realization of vertex models and understanding the effect of dimensionality reduction. We combine experiments, theory, and numerical simulations to demonstrate that sheared square colloidal ice partially recovers the ground-state degeneracy for a wide range of field strengths and lattice shear angles. Our method opens an avenue to engineer a novel class of frustrated micro- and nano-structures based on sheared magnetic lattices in a wide range of soft- and condensed-matter systems.
Using memory-function formalism we show that in sheared colloidal suspensions the fluctuation-dissipation theorem for self-diffusion, i.e. Einstein's relation between self-diffusion and mobility tensors, is violated and propose a new way to measure this violation in Brownian Dynamics simulations. We derive mode-coupling expressions for the tagged particle friction tensor and for an effective, shear-rate dependent temperature.
The nonlinear rheological properties of dense suspensions are discussed within simplified models, suggested by a recent first principles approach to the model of Brownian particles in a constant-velocity-gradient solvent flow. Shear thinning of colloidal fluids and dynamical yielding of colloidal glasses arise from a competition between a slowing down of structural relaxation, because of particle interactions, and enhanced decorrelation of fluctuations, caused by the shear advection of density fluctuations. A mode coupling approach is developed to explore the shear-induced suppression of parti…
We study numerically the crystallization process in a supersaturated suspension of repulsive colloidal particles driven by simple shear flow. The effect of the shear flow on crystallization is two-fold: while it suppresses the initial nucleation, once a large enough critical nucleus has formed its growth is enhanced by the shear flow. Combining both effects implies an optimal strain rate at which the overall crystallization rate has a maximum. To gain insight into the underlying mechanisms, we employ a discrete state model describing the transitions between the local structural configurations …
When amorphous solids are strained they display elastic deformation at small strain, however, beyond a critical strain they yield and begin to flow plastically. The origin of this plasticity lies in the irreversible rearrangement of particles. Such rearrangements have been shown to give rise to a long-ranged quadrupolar strain field, similar to Eshebly's spherical inclusions. However, their spatio-temporal organisation at finite temperatures and finite shear rate remains unclear. Here, we have investigated the strain field in sheared colloidal glasses. We show that the strain field in homogene…
A Landau theory is presented for the structural transition of electrically stabilized colloidal crystals under shear. The model suggests that a structural transition from an ordered layered colloidal crystal into a disordered structure occurs at a critical shear stress. The shear induced structural transition is related to a change of the rheological properties caused by the variation of the microstructure which can be verified by scattering experiments. The theory is used to establish the shape of the flow curves. A good qualitative agreement with experimental results can be achieved, while a…
We develop a free energy framework to describe the response of glasses to applied stress. Unlike crystals, for which the free energy increases quadratically with strain due to affine displacements, for glasses, the nonequilibrium free energy decreases due to complex interplay of non-affine displacements and dissipation. We measure this free energy directly in strained colloidal glasses, and use mean-field theory to relate it to affine and nonaffine displacements. Nonaffine displacements grow with applied shear due to shear-induced loss of structural connectivity. Our mean-field model allows fo…
The rheology of dense amorphous materials under large shear strain is not fully understood, partly due to the difficulty of directly viewing the microscopic details of such materials. We use a colloidal suspension to simulate amorphous materials, and study the shear-induced structural relaxation with fast confocal microscopy. We quantify the plastic rearrangements of the particles in several ways. Each of these measures of plasticity reveals spatially heterogeneous dynamics, with localized regions where many particles are strongly rearranging by these measures. We examine the shapes of these r…
The microscopic deformation mechanism of charged colloidal glasses with extended-range interactions under shear is investigated by in-situ small-angle neutron scattering, and a dynamically correlated region (DCR) is identified. This short-lived region provides the resistance to the configurational rearrangement imposed by the external deformation, as evidenced by the evolution of the size of DCR in the shear thinning regime and the quantitative agreement between the local stress sustained by DCR and the macroscopic stress from rheological measurements at low and mediate shear rates. This findi…
By means of classical density functional theory and its dynamical extension, we consider a colloidal fluid with spherically-symmetric competing interactions, which are well known to exhibit a rich bulk phase behavior. This includes complex three-dimensional periodically ordered cluster phases such as lamellae, two-dimensional hexagonally packed cylinders, gyroid structures or spherical micelles. While the bulk phase behavior has been studied extensively in earlier work, in this paper we focus on such structures confined between planar repulsive walls under shear flow. For sufficiently high she…
The mechanical non-linear response of dense Brownian suspensions of polymer gel particles is studied experimentally and by means of numerical simulations. It is shown that the response to the application of a constant shear rate depends on the previous history of the suspension. When the flow starts from a suspension at rest, it exhibits an elastic response followed by a stress overshoot and then a plastic flow regime. Conversely, after flow reversal, the stress overshoot does not occur, and the apparent elastic modulus is reduced while numerical simulations reveal that the anisotropy of the l…
We investigate the dynamics and rheological properties of a circular colloidal cluster that is continuously sheared by magnetic and optical torques in a two-dimensional (2D) Taylor-Couette geometry. By varying the two driving fields, we obtain the system flow diagram and report the velocity profiles along the colloidal structure. We then use the inner magnetic trimer as a microrheometer, and observe continuous thinning of all particle layers followed by thickening of the third one above a threshold field. Experimental data are supported by Brownian dynamics simulations. Our approach gives a un…
Using high-speed confocal microscopy, we measure the particle positions in a colloidal suspension under large amplitude oscillatory shear. Using the particle positions we quantify the in situ anisotropy of the pair-correlation function -- a measure of the Brownian stress. From these data, we find two distinct types of responses as the system crosses over from equilibrium to far-from-equilibrium states. The first is a nonlinear amplitude saturation that arises from shear-induced advection, while the second is a linear frequency saturation due to competition between suspension relaxation and she…
Recent computational and theoretical studies have shown that the deformation of colloidal suspensions under a steady shear is highly heterogeneous at the particle level and demonstrate a critical influence on the macroscopic deformation behavior. Despite its relevance to a wide variety of industrial applications of colloidal suspensions, scattering studies focusing on addressing the heterogeneity of the non-equilibrium colloidal structure are scarce thus far. Here, we report the first experimental result using small-angle neutron scattering. From the evolution of strain heterogeneity, we concl…
Glasses behave as solids on experimental time scales due to their slow relaxation. Growing dynamic length scales due to cooperative motion of particles are believed to be central to this slow response. For quiescent glasses, however, the size of the cooperatively rearranging regions has never been observed to exceed a few particle diameters, and the observation of long-range correlations that are signatures of an elastic solid has remained elusive. Here, we provide direct experimental evidence of long-range correlations during the deformation of a dense colloidal glass. By imposing an external…
The pair correlation function of charge stabilized colloidal particles under strongly sheared conditions is studied using the analytical intermediate asymptotics method recently developed in [L. Banetta and A. Zaccone, Phys. Rev. E 99, 052606 (2019)] to solve the steady-state Smoluchowski equation for medium to high values of the Péclet number; the analytical theory works for dilute conditions. A rich physical behaviour is unveiled for the pair correlation function of colloids interacting via the repulsive Yukawa (or Debye-Hückel) potential, in both the extensional and compressional sectors of…
Crystalline bilayers of charged colloidal suspensions which are confined between two parallel plates and sheared via a relative motion of the two plates are studied by extensive Brownian dynamics computer simulations. The charge-stabilized suspension is modeled by a Yukawa pair potential. The unsheared equilibrium configuration are two crystalline layers with a nested quadratic in-plane structure. For increasing shear rates $\dot γ$, we find the following steady states: first, there is a static solid which is elastically sheared until a yield-stress limit is reached. Then there are two crystal…
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 hyperuniformit…
We study the rheological properties of colloidal microphases in two dimensions simulating a model of colloidal particles with competing interactions. Due to the competition between short-range attraction and long-range repulsion, as a function of the density the model exhibits a variety of microphases such as clusters, stripes or crystals with bubbles. We prepare the system in a confined microphase employing Monte-Carlo simulations and then quench the system at T=0. The resulting configurations are then sheared by applying a drag force profile. We integrate numerically the equation of motion f…
The constituents of soft matter systems such as colloidal suspensions, emulsions, polymers, and biological tissues undergo microscopic random motion, due to thermal energy. They may also experience drift motion correlated over mesoscopic or macroscopic length scales, \textit{e.g.} in response to an internal or applied stress or during flow. We present a new method for measuring simultaneously both the microscopic motion and the mesoscopic or macroscopic drift. The method is based on the analysis of spatio-temporal cross-correlation functions of speckle patterns taken in an imaging configuratio…
