Michael E. Cates

Flow-induced phase transitions in rod-like micelles

The authors study the dynamics of self-assembling rod-like micelles under both shear and elongational flow. They assume a simple reaction scheme in which two micelles can fuse only if they are collinear. This results in a positive feedback mechanism between micellar alignment and growth. They define tau break as the reaction time for a typical micelle and tau rot as its rotational diffusion time. They consider both the limiting case of tau break > tau rot. By matching these limiting results they are able to make some predictions for the general case. In elongational flow they predict a gelation transition, at some critical flow rate, to a phase of extremely long rods which are fully aligned with the flow axis. It is shown that these rods can be of a length which is very much greater than the mean micellar length in the absence of flow but which is still stable with respect to the tension produced in a flow. It is found that the analogous transition in shear flow is absent although the mean micellar size near the flow axis is still expected to increase sharply at high flow rates. The authors briefly discuss the relevance of the calculations to experiments on shear-induced structures in micellar systems.

Light-induced self-assembly of active rectification devices

Self-propelled particles that swim in response to light can self-assemble microfluidic rectification devices under nonuniform illumination. Self-propelled colloidal objects, such as motile bacteria or synthetic microswimmers, have microscopically irreversible individual dynamics—a feature they share with all living systems. The incoherent behavior of individual swimmers can be harnessed (or “rectified”) by microfluidic devices that create systematic motions that are impossible in equilibrium. We present a computational proof-of-concept study showing that such active rectification devices could be created directly from an unstructured “primordial soup” of light-controlled motile particles, solely by using spatially modulated illumination to control their local propulsion speed. Alongside both microscopic irreversibility and speed modulation, our mechanism requires spatial symmetry breaking, such as a chevron light pattern, and strong interactions between particles, such as volume exclusion, which cause a collisional slowdown at high density. Together, we show how these four factors create a novel, many-body rectification mechanism. Our work suggests that standard spatial light modulator technology might allow the programmable, light-induced self-assembly of active rectification devices from an unstructured particle bath.

Clustering and Pattern Formation in Chemorepulsive Active Colloids.

We demonstrate that migration away from self-produced chemicals (chemorepulsion) generates a generic route to clustering and pattern formation among self-propelled colloids. The clustering instability can be caused either by anisotropic chemical production, or by a delayed orientational response to changes of the chemical environment. In each case, chemorepulsion creates clusters of a self-limiting area which grows linearly with self-propulsion speed. This agrees with recent observations of dynamic clusters in Janus colloids (albeit not yet known to be chemorepulsive). More generally, our results could inform design principles for the self-assembly of chemorepulsive synthetic swimmers and/or bacteria into nonequilibrium patterns.

Celebrating Soft Matter's 10th anniversary: Testing the foundations of classical entropy: colloid experiments

Defining the entropy of classical particles raises a number of paradoxes and ambiguities, some of which have been known for over a century. Several, such as Gibbs paradox, involve the fact that classical particles are distinguishable, and in textbooks these are often resolved by appeal to the quantum-mechanical indistinguishability of atoms or molecules of the same type. However, questions then remain of how to correctly define the entropy of large poly-atomic particles such as colloids in suspension, of which no two are exactly alike. By performing experiments on such colloids, one can establish that certain definitions of the classical entropy fit the data, while others in the literature do not. Specifically, the experimental facts point firmly to an informatic interpretation that dates back to Gibbs: entropy is determined by the number of microstates that we as observers choose to treat as equivalent when we identify a macrostate. This approach, unlike some others, can account for the existence of colloidal crystals, and for the observed abundances of colloidal clusters of different shapes. We also address some lesser-known paradoxes whereby the physics of colloidal assemblies, which ought to be purely classical, seems to involve quantum mechanics directly. The experimental symptoms of such involvement are predicted to be isotope effects in which colloids with different inertial masses, but otherwise identical sizes and properties, show different aggregation statistics. These paradoxes are caused by focussing ones attention on some classical degrees while neglecting others; when all are treated equally, all isotope effects are found to vanish.

Pattern formation in chemically interacting active rotors with self-propulsion

We demonstrate that active rotations in chemically signalling particles, such as autochemotactic E. coli close to walls, create a route for pattern formation based on a nonlinear yet deterministic instability mechanism. For slow rotations, we find a transient persistence of the uniform state, followed by a sudden formation of clusters contingent on locking of the average propulsion direction by chemotaxis. These clusters coarsen, which results in phase separation into a dense and a dilute region. Faster rotations arrest phase separation leading to a global travelling wave of rotors with synchronized roto-translational motion. Our results elucidate the physics resulting from the competition of two generic paradigms in active matter, chemotaxis and active rotations, and show that the latter provides a tool to design programmable self-assembly of active matter, for example to control coarsening.

Tunable shear thickening in suspensions

Significance When a concentrated suspension is strained, its viscosity can increase radically. This behavior, known as shear thickening, can be very useful to technological applications or highly problematic in industrial processes. Suspension flow properties are typically specified at the formulation stage, meaning that they are fixed in advance rather than controlled in situ during application. Here, we report a biaxial shear strategy eradicating the flow-induced structures responsible for thickening and tuning the suspension viscosity on demand during flow. This protocol enables us to regulate the thickening viscosity over 2 orders of magnitude. The tuning capability is a foundational step toward using dense suspensions in 3D printing, energy storage, and robotics. Shear thickening, an increase of viscosity with shear rate, is a ubiquitous phenomenon in suspended materials that has implications for broad technological applications. Controlling this thickening behavior remains a major challenge and has led to empirical strategies ranging from altering the particle surfaces and shape to modifying the solvent properties. However, none of these methods allows for tuning of flow properties during shear itself. Here, we demonstrate that by strategic imposition of a high-frequency and low-amplitude shear perturbation orthogonal to the primary shearing flow, we can largely eradicate shear thickening. The orthogonal shear effectively becomes a regulator for controlling thickening in the suspension, allowing the viscosity to be reduced by up to 2 decades on demand. In a separate setup, we show that such effects can be induced by simply agitating the sample transversely to the primary shear direction. Overall, the ability of in situ manipulation of shear thickening paves a route toward creating materials whose mechanical properties can be controlled.

Nonequilibrium dynamics of mixtures of active and passive colloidal particles

We develop a mesoscopic field theory for the collective nonequilibrium dynamics of multicomponent mixtures of interacting active (i.e., motile) and passive (i.e., nonmotile) colloidal particles with isometric shape in two spatial dimensions. By a stability analysis of the field theory, we obtain equations for the spinodal that describes the onset of a motility-induced instability leading to cluster formation in such mixtures. The prediction for the spinodal is found to be in good agreement with particle-resolved computer simulations. Furthermore, we show that in active-passive mixtures the spinodal instability can be of two different types. One type is associated with a stationary bifurcation and occurs also in one-component active systems, whereas the other type is associated with a Hopf bifurcation and can occur only in active-passive mixtures. Remarkably, the Hopf bifurcation leads to moving clusters. This explains recent results from simulations of active-passive particle mixtures, where moving clusters and interfaces that are not seen in the corresponding one-component systems have been observed. (Less)

Random bilayer phases of dilute surfactant solutions

Surfactant molecules in dilute solution may aggregate reversibly into extended structures. For suitably chosen molecules, the preferred packing involves a locally flat bilayer which tends to wander entropically at large distances. At low temperatures (and/or high concentrations) the system forms a stack of flat sheets with one-dimensional quasi-long range order (a smectic liquid crystal), but at high temperatures or low concentrations, the stack can melt into a random surface structure that resembles a multiply connected labyrinth or sponge of bilayer in a sea of solvent. Recent theoretical and experimental progress in understanding the properties of the sponge is reviewed. The authors argue that the sponge phase may provide a good system for the study of various liquid-state critical phenomena.

Theories of binary fluid mixtures: from phase-separation kinetics to active emulsions

Binary fluid mixtures are examples of complex fluids whose microstructure and flow are strongly coupled. For pairs of simple fluids, the microstructure consists of droplets or bicontinuous demixed domains and the physics is controlled by the interfaces between these domains. At continuum level, the structure is defined by a composition field whose gradients which are steep near interfaces drive its diffusive current. These gradients also cause thermodynamic stresses which can drive fluid flow. Fluid flow in turn advects the composition field, while thermal noise creates additional random fluxes that allow the system to explore its configuration space and move towards the Boltzmann distribution. This article introduces continuum models of binary fluids, first covering some well-studied areas such as the thermodynamics and kinetics of phase separation, and emulsion stability. We then address cases where one of the fluid components has anisotropic structure at mesoscopic scales creating nematic (or polar) liquid-crystalline order; this can be described through an additional tensor (or vector) order parameter field. We conclude by outlining a thriving area of current research, namely active emulsions, in which one of the binary components consists of living or synthetic material that is continuously converting chemical energy into mechanical work.

Contractile and chiral activities codetermine the helicity of swimming droplet trajectories

Significance Active fluids include bacterial suspensions, biological tissues, and the cytoskeleton. They are far from equilibrium because the fluid is continuously stirred by constituent particles themselves. A model droplet of active fluid can show swimming or crawling motilities resembling those in real biological cells despite the simplifications entailed. Here, we consider the effects of microscopic chirality on the motility of these active droplets. We find a rich phase diagram including oscillatory dynamics, run and tumble, and helical swimming with either the same or opposite sign to the microscopic one. Active fluids are a class of nonequilibrium systems where energy is injected into the system continuously by the constituent particles themselves. Many examples, such as bacterial suspensions and actomyosin networks, are intrinsically chiral at a local scale, so that their activity involves torque dipoles alongside the force dipoles usually considered. Although many aspects of active fluids have been studied, the effects of chirality on them are much less known. Here, we study by computer simulation the dynamics of an unstructured droplet of chiral active fluid in three dimensions. Our model considers only the simplest possible combination of chiral and achiral active stresses, yet this leads to an unprecedented range of complex motilities, including oscillatory swimming, helical swimming, and run-and-tumble motion. Strikingly, whereas the chirality of helical swimming is the same as the microscopic chirality of torque dipoles in one regime, the two are opposite in another. Some of the features of these motility modes resemble those of some single-celled protozoa, suggesting that underlying mechanisms may be shared by some biological systems and synthetic active droplets.