First Order Alignment Transition in an Interfaced Active Nematic Fluid.

We investigate experimentally the dynamic phase transition of a two-dimensional active nematic layer interfaced with a passive liquid crystal. Under a temperature ramp that leads to the transition of the passive liquid into a highly anisotropic lamellar smectic-A phase, and in the presence of a magnetic field, the coupled active nematic reorganizes its flow and orientational patterns from the turbulent into a quasilaminar regime aligned perpendicularly to the field. Remarkably, while the phase transition of the passive fluid is known to be continuous, or second order, our observations reveal intermittent dynamics of the order parameter and the coexistence of aligned and turbulent regions in the active nematic, a signature of discontinuous, or first order, phase transitions, similar to what is known to occur in relation to flocking in dry active matter. Our results suggest that alignment transitions in active systems are intrinsically discontinuous, regardless of the symmetry and momentum-damping mechanisms.

Collective chemomechanical oscillations in active hydrogels.

We report on the collective response of an assembly of chemomechanical Belousov-Zhabotinsky (BZ) hydrogel beads. We first demonstrate that a single isolated spherical BZ hydrogel bead with a radius below a critical value does not oscillate, whereas an assembly of the same BZ hydrogel beads presents chemical oscillation. A BZ chemical model with an additional flux of chemicals out of the BZ hydrogel captures the experimentally observed transition from oxidized nonoscillating to oscillating BZ hydrogels and shows this transition is due to a flux of inhibitors out of the BZ hydrogel. The model also captures the role of neighboring BZ hydrogel beads in decreasing the critical size for an assembly of BZ hydrogel beads to oscillate. We finally leverage the quorum sensing behavior of the collective to trigger their chemomechanical oscillation and discuss how this collective effect can be used to enhance the oscillatory strain of these active BZ hydrogels. These findings could help guide the eventual fabrication of a swarm of autonomous, communicating, and motile hydrogels.

Measuring the counterion cloud of soft microgels using SANS with contrast variation.

The behavior of microgels and other soft, compressible colloids depends on particle concentration in ways that are absent in their hard-particulate counterparts. For instance, poly-N-isopropylacrylamide (pNIPAM) microgels can spontaneously deswell and reduce suspension polydispersity when concentrated enough. Despite the pNIPAM network in these microgels is neutral, the key to understanding this distinct behavior relies on the existence of peripheric charged groups, responsible for providing colloidal stability when deswollen, and the associated counterion cloud. When in close proximity, clouds of different particles overlap, effectively freeing the associated counterions, which are then able to exert an osmotic pressure that can potentially cause the microgels to decrease their size. Up to now, however, no direct measurement of such an ionic cloud exists, perhaps even also for hard colloids, where it is referred to as an electric double layer. Here, we use small-angle neutron scattering with contrast variation with different ions to isolate the change in the form factor directly related to the counterion cloud, and obtain its radius and width. Our results highlight that the modeling of microgel suspensions must unavoidably and explicitly consider the presence of this cloud, which exists for nearly all microgels synthesized today.

Physically informed data-driven modeling of active nematics.

A continuum description is essential for understanding a variety of collective phenomena in active matter. However, building quantitative continuum models of active matter from first principles can be extremely challenging due to both the gaps in our knowledge and the complicated structure of nonlinear interactions. Here, we use a physically informed data-driven approach to construct a complete mathematical model of an active nematic from experimental data describing kinesin-driven microtubule bundles confined to an oil-water interface. We find that the structure of the model is similar to the Leslie-Ericksen and Beris-Edwards models, but there are appreciable and important differences. Rather unexpectedly, elastic effects are found to play no role in the experiments considered, with the dynamics controlled entirely by the balance between active stresses and friction stresses.

Long term phase separation dynamics in liquid crystal-enriched microdroplets obtained from binary fluid mixtures.

The dynamics of long term phase separation in binary liquid mixtures remains a subject of fundamental interest. Here, we study a binary liquid mixture, where the minority phase is confined to a liquid crystal (LC)-rich droplet, by investigating the evolution of size, defect and mesogen alignment over time. We track the binary liquid mixture evolving towards equilibrium by visualising the configuration of the liquid crystal droplet through polarisation microscopy. We compare our experimental findings with computational simulations and elucidate differences between bulk phases and confined droplets based on the respective thermodynamics of phase separation. Our work provides insights on how phase transitions on the microscale can deviate from bulk phase diagrams with relevance to other material systems, such as the liquid-liquid phase separation of polymer and protein solutions.

Ant waves-Spontaneous activity waves in fire-ant columns.

Active matter, which includes crowds of organisms, is composed of constituents that independently consume and dissipate energy. Some active matter systems have been shown to sustain the propagation of various types of waves, resulting from the interplay between density and alignment. Here, we examine a type of solitary wave in dense two-dimensional columns of Solenopsis invicta, fire ants, in which the local activity, density and alignment all play a key role. We demonstrate that these waves are nonlinear and that they are composed of aligned ants that are constrained at the top by the time it takes disordered ants to activate and align and at the bottom by a density minimum enforced by gravity. Our results suggest that intrinsically switchable activity can be a productive framework to understand and trigger a broad range of wave-like behaviors, including stampedes in crowds and herds.

Social interactions lead to motility-induced phase separation in fire ants.

Collections of fire ants are a form of active matter, as the ants use their internal metabolism to self-propel. In the absence of aligning interactions, theory and simulations predict that active matter with spatially dependent motility can undergo motility-induced phase separation. However, so far in experiments, the motility effects that drive this process have come from either crowding or an external parameter. Though fire ants are social insects that communicate and cooperate in nontrivial ways, we show that the effect of their interactions can also be understood within the framework of motility-induced phase separation. In this context, the slowing down of ants when they approach each other results in an effective attraction that can lead to space-filling clusters and an eventual formation of dynamical heterogeneities. These results illustrate that motility-induced phase separation can provide a unifying framework to rationalize the behavior of a wide variety of active matter systems.

Janssen effect in columns of fire ants.

We study fire-ant columns, an active version of passive granular columns, and find that, despite the inherent activity of the ants and their natural tendency to rearrange, the ants develop force-chain structures that help support the weight of the column. Hence, the apparent mass at the bottom of the column saturates with added mass in a Janssen-like fashion, reminiscent of what is seen in passive-grain columns in wide containers. Activity-induced rearrangements within the column, however, lead to changes in the force-chain structure that slightly reduce the supportive nature of the force-chains over time and to fluctuations in the pressure at the bottom of the column that scale like the law of large numbers. We capture the experimental results in simulations that include not only friction with the walls, but also a fluctuating force that introduces activity and that effectively affects the force-chain structure of the ant collective.

Resolving the different bulk moduli within individual soft nanogels using small-angle neutron scattering.

The bulk modulus, K, quantifies the elastic response of an object to an isotropic compression. For soft compressible colloids, knowing K is essential to accurately predict the suspension response to crowding. Most colloids have complex architectures characterized by different softness, which additionally depends on compression. Here, we determine the different values of K for the various morphological parts of individual nanogels and probe the changes of K with compression. Our method uses a partially deuterated polymer, which exerts the required isotropic stress, and small-angle neutron scattering with contrast matching to determine the form factor of the particles without any scattering contribution from the polymer. We show a clear difference in softness, compressibility, and evolution of K between the shell of the nanogel and the rest of the particle, depending on the amount of cross-linker used in their synthesis.

Glass-Based Devices to Generate Drops and Emulsions.

In this manuscript, three different step-by-step protocols to generate highly monodisperse emulsion drops using glass-based microfluidics are described. The first device is built for the generation of simple drops driven by gravity. The second device is designed to generate emulsion drops in a coflowing scheme. The third device is an extension of the coflowing device with the addition of a third liquid that acts as an electric ground, allowing the formation of electrified drops that subsequently discharge. In this setup, two of the three liquids have an appreciable electrical conductivity. The third liquid mediates between these two and is a dielectric. A voltage difference applied between the two conducting liquids creates an electric field that couples with hydrodynamic stresses of the coflowing liquids, affecting the jet and drop formation process. The addition of the electric field provides a path to generate smaller drops than in simple coflow devices and for generating particles and fibers with a wide range of sizes.

From nematic shells to nematic droplets: energetics and defect transitions.

In this work, we investigate the possibility of inducing valence transitions, i.e. transitions between different defect configurations, by transforming a nematic shell into a nematic droplet. Our shells are liquid crystal droplets containing a smaller aqueous droplet inside, which are suspended in an aqueous phase. When osmotically de-swelling the inner droplet, the shell progressively increases its thickness until it eventually becomes a single droplet. During the process, the shell energy landscape evolves, triggering a response in the system. We observe two different scenarios. Either the inner droplet progressively shrinks and disappears, inducing a defect reorganization, or it is expelled from the shell at a critical radius of the inner droplet, abruptly changing the geometry of the system. We use numerical simulations and modeling to investigate the origin of these behaviors. We find that the selected route depends on the defect structure and the energetics of the system as it evolves. The critical inner radius and time for expulsion depend on the osmotic pressure of the outer phase, suggesting that the flow through the shell plays a role in the process.

Polymer-chain configurations in active and passive baths.

The configurations taken by polymers embedded in out-of-equilibrium baths may have broad implications in a variety of biological systems. As such, they have attracted considerable interest, particularly in simulation studies. Here we analyze the distribution of configurations taken by a passive flexible chain in a bath of hard, self-propelled, vibrated disks and systematically compare it to that of the same flexible chain in a bath of hard, thermal-like, vibrated disks. We demonstrate experimentally that the mean length and mean radius of gyration of both chains agree with Flory's law. However, the Kuhn length associated with the number of correlated monomers is smaller in the case of the active bath, corresponding to a higher effective temperature. Importantly, the active bath does not just simply map on a hot equilibrium bath. Close examination of the chains' configurations indicates a marked bias, with the chain in the active bath more likely assuming configurations with a single prominent bend.

Internal structure of ultralow-crosslinked microgels: From uniform deswelling to phase separation.

We perform small angle neutron scattering on ultralow-crosslinked microgels and find that while in certain conditions both the particle size and the characteristic internal length scale change in unison, in other instances this is not the case. We show that nonuniform deswelling depends not only on particle size, but also on the particular way the various contributions to the free energy combine to result in a given size. Only when polymer-solvent demixing strongly competes with ionic or electrostatic effects do we observe nonuniform behavior, reflecting internal microphase separation. The results do not appreciably depend on particle number density; even in concentrated suspensions, we find that at relatively low temperature, where demixing is not very strong, the deswelling behavior is uniform, and that only at sufficiently high temperature, where demixing is very strong, does the microgel structure change akin to internal microphase separation.

Behavior and mechanics of dense microgel suspensions.

Suspensions of soft and highly deformable microgels can be concentrated far more than suspensions of hard colloids, leading to their unusual mechanical properties. Microgels can accommodate compression in suspensions in a variety of ways such as interpenetration, deformation, and shrinking. Previous experiments have offered insightful, but somewhat conflicting, accounts of the behavior of individual microgels in compressed suspensions. We develop a mesoscale computational model to probe the behavior of compressed suspensions consisting of microgels with different architectures at a variety of packing fractions and solvent conditions. We find that microgels predominantly change shape and mildly shrink above random close packing. Interpenetration is only appreciable above space filling, remaining small relative to the mean distance between cross-links. At even higher packing fractions, microgels solely shrink. Remarkably, irrespective of the single-microgel properties, and whether the suspension concentration is changed via changing the particle number density or the swelling state of the particles, which can even result in colloidal gelation, the mechanics of the suspension can be quantified in terms of the single-microgel bulk modulus, which thus emerges as the correct mechanical measure for these type of soft-colloidal suspensions. Our results rationalize the many and varied experimental results, providing insights into the relative importance of effects defining the mechanics of suspensions comprising soft particles.

Activity effects on the nonlinear mechanical properties of fire-ant aggregations.

Individual fire ants are inherently active as they are living organisms that convert stored chemical energy into motion. However, each individual ant is not equally disposed to motion at any given time. In an active aggregation, most of the constituent ants are active, and vice versa for an inactive aggregation. Here we look at the role activity plays on the nonlinear mechanical behavior of the aggregation through large amplitude oscillatory shear measurements. We find that the level of viscous nonlinearity can be decreased by increasing the activity or by increasing the volume fraction. In contrast, the level of elastic nonlinearity is not affected by either activity or volume fraction. We interpret this in terms of a transient network with equal rates of linking and unlinking but with varying number of linking and unlinking events.

Rheology of capillary foams.

Aqueous foams are ubiquitous; they appear in products and processes that span the cosmetics, food, and energy industries. The versatile applicability of foams comes as a result of their intrinsic viscous and elastic properties; for example, foams are exploited as drilling fluids in enhanced oil recovery for their high viscosity. Recently, so-called capillary foams were discovered: a class of foams that have excellent stability under static conditions and whose flow properties have so far remained unexplored. The unique architecture of these foams, containing oil-coated bubbles and a gelled network of oil-bridged particles, is expected to affect foam rheology. In this work, we report the first set of rheological data on capillary foams. We study the viscoelastic properties of capillary foams by conducting oscillatory and steady shear tests. We compare our results on the rheological properties of capillary foams to those reported for other aqueous foams. We find that capillary foams, which have low gas volume fractions, exhibit long lasting rheological stability as well as a yielding behavior that is reminiscent of surfactant foams with high gas volume fractions.

Polarized epifluorescence microscopy and the imaging of nematic liquid crystals in highly curved geometries.

We develop polarized epifluorescence microscopy (PFM), a technique to qualitatively determine a director field, even when refraction effects are too strong to use optical polarized microscopy. We present the basic theory behind the technique and cover in detail the experimental setup. We validate PFM on the well-studied cases of a planar nematic cell, spherical nematic droplets, and a cylindrical capillary filled with nematic liquid crystal. Last, we use nematic capillary bridges to demonstrate that PFM can indeed provide measurements of the director field, even when refraction effects are large.

Complexation of Pluronic L62 (EO6)-(PO34)-(EO6)/aerosol-OT (sodium bis(2-ethylhexyl)sulfosuccinate) in aqueous solutions investigated by small angle neutron scattering.

We investigate the phase behaviours of Pluronic L62 in aqueous solution in the presence of aerosol-OT (AOT) molecules by small angle neutron scattering (SANS). The presence of AOT significantly changes the micellization phenomenon of L62 micelles in aqueous solution, including their critical micelle temperature (CMT), global size, and asphericity. The origin of these observations is attributed to the complexation between the neutral L62 surfactants and the ionic AOT molecules, which additionally provides charge to the mixed micelles: we analyse the data and extract meaningful information using the Ornstein-Zernike integral formalism. As a result, we observe that the co-micellization of L62 and AOT is very stable across a wide temperature range.

Reverse Janssen Effect in Narrow Granular Columns.

When grains are added to a cylinder, the weight at the bottom is smaller than the total weight of the column, which is partially supported by the lateral walls through frictional interactions with the grains. This is known as the Janssen effect. Via a combined experimental and numerical investigation, here we demonstrate a reverse Jansen effect whereby the fraction of the weight supported by the base overcomes one. We characterize the dependence of this phenomenon on the various control parameters involved, rationalize the physical process causing the emergence of the compressional frictional forces responsible for the anomaly, and introduce a model to reproduce our findings. Contrary to prior assumptions, our results demonstrate that the constitutive relation on a material element can depend on the applied stress.

Capillary-Based Microfluidics-Coflow, Flow-Focusing, Electro-Coflow, Drops, Jets, and Instabilities.

Capillary-based microfluidics is a great technique to produce monodisperse and complex emulsions and particulate suspensions. In this review, the current understanding of drop and jet formation in capillary-based microfluidic devices for two primary flow configurations, coflow and flow-focusing is summarized. The experimental and theoretical description of fluid instabilities is discussed and conditions for controlled drop breakup in different modes of drop generation are provided. Current challenges in drop breakup with low interfacial tension systems and recent progress in overcoming drop size limitations using electro-coflow are addressed. In each scenario, the physical mechanisms for drop breakup are revisited, and simple scaling arguments proposed in the literature are introduced.