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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.

We investigate the emergence of orientational order among +1/2 disclinations in active nematic liquid crystals. Using a combination of theoretical and experimental methods, we show that +1/2 disclinations have short-range antiferromagnetic alignment, as a consequence of the elastic torques originating from their polar structure. The presence of intermediate -1/2 disclinations, however, turns this interaction from anti-aligning to aligning at scales that are smaller than the typical distance between like-sign defects. No long-range orientational order is observed. Strikingly, these effects are insensitive to material properties and qualitatively similar to what is found for defects in passive nematic liquid crystals., 6 pages, 4 figures

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.

We determine the osmotic pressure of microgel suspensions using membrane osmometry and dialysis, for microgels with different softnesses. Our measurements reveal that the osmotic pressure of solutions of both ionic and neutral microgels is determined by the free ions that leave the microgel periphery to maximize their entropy and not by the translational degrees of freedom of the microgels themselves. Furthermore, up to a given concentration it is energetically favorable for the microgels to maintain a constant volume without appreciable deswelling. The concentration where deswelling starts weakly depends on the crosslinker concentration, which affects the microgel dimension; we explain this by considering the dependence of the osmotic pressure and the microgel bulk modulus on the particle size.

We confine a nematic liquid crystal with homeotropic anchoring to stable toroidal droplets and study how geometry affects the equilibrium director configuration. In contrast to the case of cylindrical confinement, we find that the equilibrium state is chiral-a twisted and escaped radial director configuration. Furthermore, we find that the magnitude of the twist distortion increases as the ratio of the ring radius to the tube radius decreases; we confirm this with computer simulations of optically polarized microscopy textures. In addition, numerical calculations also indicate that the local geometry indeed affects the magnitude of the twist distortion. We further confirm this curvature-induced twisting using bent cylindrical capillaries.

We use toroidal droplets to study the breakup dynamics of a Newtonian liquid jet in the presence of rheologically nonlinear materials. We find that the droplets resist breakup for times that are longer than those in the presence of Newtonian liquids. More importantly, we show that our experiments can be explained by incorporating the nonlinearities into the linear treatment of the problem through the strain-rate-dependent viscosity. Finally, we show that the scaling factor required to relate the viscosity to the growth rate associated to unstable modes is given by the elastic modulus of the outside material, illustrating that both the viscoelastic and shear-thinning nature of the outside material play a crucial role in the dynamics of the problem.

Fire ant aggregations are active materials composed of individual constituents that are able to transform internal energy into work. We find using rheology and direct visualization that the aggregation undergoes activity cycles that affect the mechanical properties of the system. When the activity is high, the aggregation approximately equally stores and dissipates energy, it is more homogeneous, and exerts a high outward force. When the activity is low, the aggregation is predominantly elastic, it is more heterogeneous, and it exerts a small outward force. We rationalize our results using a simple kinetic model where the number of active ants within the aggregation is the essential quantity.

We investigate the phase behavior of suspensions of poly($N$-isopropylacrylamide) (pNIPAM) microgels with either bimodal or polydisperse size distribution. We observe a shift of the fluid-crystal transition to higher concentrations depending on the polydispersity or the fraction of large particles in suspension. Crystallization is observed up to polydispersities as high as 18.5%, and up to a number fraction of large particles of 29% in bidisperse suspensions. The crystal structure is random hexagonal close-packed as in monodisperse pNIPAM microgel suspensions. We explain our experimental results by considering the effect of bound counterions. Above a critical particle concentration, these cause deswelling of the largest microgels, which are the softest, changing the size distribution of the suspension and enabling crystal formation in conditions where incompressible particles would not crystallize.

Neutral toroidal droplets can break via the surface-tension-driven Rayleigh-Plateau instability. They can additionally exhibit a shrinking instability, which is also driven by surface tension, whereby the handle progressively disappears. We find that charging a toroidal droplet can qualitatively change the behavior and cause the droplet to expand. We successfully model the transition from shrinking to expanding, considering the pressure balance across the interface of the torus. However, despite the change in behavior, charged toroidal droplets end up breaking into spherical droplets. We quantify how the wavelength of the fastest unstable mode associated to this breakup depends on the applied voltage and compare the results with theoretical expectations for charged cylindrical jets.

We investigate microgels synthesized from $N$-isopropylacrylamide (NIPAM) copolymerized with a large mol% of acrylic acid, finding that when the acid groups are partially ionized at high temperatures, competition between ion-induced swelling and hydrophobic deswelling of poly(NIPAM) chains results in microphase separation. In cross-linked microgels, this manifests as a dramatic decrease in the ratio between the radius of gyration and the hydrodynamic radius to $\ensuremath{\sim}0.2$, indicating that almost all the mass of the microgel is concentrated near the particle center. We also observe a concurrent decrease of the polymer network length scale via small-angle neutron scattering, confirming the presence of a dense, deswollen core surrounded by a diffuse, charged periphery. We compare these results to those obtained for a system of charged ultralow-cross-linked microgels; the form factor shows a distinct peak at high $q$ when the temperature exceeds a threshold value. We successfully fit the form factor to theory developed to describe scattering from weakly charged gels in poor solvents, and we tie this behavior to charge segregation in the case of the cross-linked microgels.

International audience; We introduce the idea of transformation trajectories to describe the evolution of nematic shells in terms of defect locations and director field when the elastic anisotropy and the shell thickness heterogeneity vary. Experiments are compared to numerical results to clarify the exact role played by these two parameters. We demonstrate that heterogeneity in thickness is a result of a symmetry breaking initiated by buoyancy and enhanced by liquid crystal elasticity, and is irrespective of the elastic anisotropy. In contrast, elastic anisotropy--in particular, disfavored bend distortion--drives an asymmetric defect reorganization. These shell states can be both stable or metastable.

We independently determine the bulk and shear moduli of compressed microgel suspensions and the bulk modulus of individual microgel particles and find that the elastic behavior of the suspension reflects the degree of compression of the particles. This feature, which is distinct from other soft materials such as emulsions or foams, can give rise to an unusually large difference between the bulk and shear moduli of the suspension. Our results extend our understanding of soft materials to systems based on compressible objects, opening up possibilities for engineering materials with drastically different responses to shear and compression.

4 páginas, 4 figuras.-- PACS numbers: 47.65.-d, 47.55.db, 47.60.Kz, We use a glass-based microfluidic device to study the electric current behavior of an electrospray process in the presence of a coflowing liquid. The current shows strong voltage dependence and weak flow rate dependence, in stark contrast to classical electrospray. By considering that the current is dominated by convection near the apex of the conical meniscus and driven by tangential electric stresses, we quantitatively capture the voltage and flow rate dependence of the current. Our results elucidate the influence of external field strength and open the way to achieve robust electric control of the current and of the drop size in microfluidics., We thank DPI2008-06624-C03-03 and NSF (DMR- 0847304 and CBET-0967293).

We present a small-angle x-ray scattering study of the crystal structure formed by pH -sensitive poly(2-vinylpyridine) microgel particles with 5 wt % of cross-linker. We focus on highly swollen particles and explore concentrations ranging from below close packing to well above close packing, where the particles are forced to shrink and/or interpenetrate. The crystal structure found from poly- as well as monocrystalline domains is random hexagonally close packed, as also observed in hard spheres.

We use a simple method to generate toroidal droplets and study how they transform into spherical droplets. The method relies on the viscous forces exerted by a rotating continuous phase over a liquid which is extruded from an injection needle; the resultant jet is forced to close into a torus due to the imposed rotation. Once formed, the torus transforms into single or multiple spheres. Interestingly, we find there are two routes for this process depending on the aspect ratio of the torus. For thin tori, classical hydrodynamic instabilities induce its breakup into a precise number of droplets. By contrast, for sufficiently fat tori, unstable modes are unable to grow, and the torus evolves through a different route; it shrinks towards its center to coalesce onto itself, to finally form a single spherical droplet.

We investigate the effect of confinement on drop formation in microfluidic devices. The presence or absence of drop formation is studied for two immiscible coflowing liquids in a microfluidic channel, where the channel width is considerably larger than the channel height. We show that stability of the inner fluid thread depends on the channel geometry: when the width of the inner fluid is comparable to or larger than the channel height, hydrodynamic instabilities are suppressed, and a stable jet that does not break into drops results; otherwise, the inner fluid breaks into drops, in either a dripping or jetting regime. We present a model that accounts for the data and experimentally exploit this effect of geometric confinement to induce the breakup of a jet at a spatially defined location.

We investigate how defects in bipolar shells of liquid crystal evolve when the boundary conditions for the nematic director n at the outer surface of the shell are changed from tangential to homeotropic. When the boundary conditions for n are tangential, these bipolar shells are characterized by the presence of two pairs of boojums, one pair on each spherical surface. However, when n is tangential at the inner surface and perpendicular at the outer surface, only the innermost pair of defects remains. Interestingly, there are two possible routes from one shell to the other and both involve the generation of a disclination ring that shrinks with time, eventually disappearing. Although the process is reminiscent of that encountered in bulk nematic droplets, in the case of nematic shells the two defects on the inner surface play a relevant role in the overall evolution process.

Cylindrical liquid jets are inherently unstable and eventually break into drops due to the Rayleigh-Plateau instability, characterized by the growth of disturbances that are either convective or absolute in nature. Convective instabilities grow in amplitude as they are swept along by the flow, while absolute instabilities are disturbances that grow at a fixed spatial location. Liquid jets are nearly always convectively unstable. Here we show that two-phase jets can breakup due to an absolute instability that depends on the capillary number of the outer liquid, provided the Weber number of the inner liquid is $gO(1)$. We verify our experimental observations with a linear stability analysis.

We study the structure of charged colloidal suspensions under confinement and determine a state diagram for the occurrence of electrostatic adsorption onto the confining walls, an effect that results in the accumulation of particles on the bounding surfaces and that could be relevant in experiments. We use Monte Carlo simulations to quantify this structural transition and perform theoretical calculations based on integral equations. Overall, our results provide a guide for experimentalists dealing with charged colloidal systems to determine the relevance of this purely electrostatic effect.

We use double-emulsion drops to experimentally investigate the defect structures of spherical shells of nematic liquid crystals. We uncover a rich scenario of coexisting defect structures dictated by the unavoidable finite thickness of even the thinnest shell and by the thickness variation around the sphere. These structures are characterized by a varying number of disclination lines and pairs of surface point defects on the inner and outer surfaces of the nematic shell. In the limit of very thick shells the defect structure ultimately merges with that of a bulk nematic liquid crystal drop.

Bipolar liquid crystal drops moving inside microchannels exhibit periodic director field transformations due to induced circulating flows inside them. These modifications are characterized by changes in the type of point surface disclinations; they periodically change from splay to bend disclinations, implying the drop changes between bipolar and escaped concentric configurations. Upon stopping the flow, this structure does not relax to the lower energy bipolar configuration; we argue this is due to drop flattening inside the channels.

Polymeric microgels are very interesting systems to study polymer-solvent interactions since they react to changes in the solvent properties by swelling or deswelling to reach a final equilibrium state of minimal free energy. Accordingly, factors such as pH, temperature, or salt concentration can induce size changes. While the volume phase transition undergone by ionic microgels with addition of salt is reasonably well understood in terms of Donnan effects, the origin of these transitions in neutral microgels is devoid of such understanding. In this paper, the effects of electrolytes on the swelling behavior of neutral thermosensitive microgels are interpreted within the Flory-Rehner theory for the swelling of neutral gels, by considering that ionic concentration affects the entropic contribution to the Flory solvency $\ensuremath{\chi}$ parameter; this manifests macroscopically as particle deswelling. The entropic changes depend on the ability of the electrolyte to disrupt the neighboring water structure and result in increasing values of $\ensuremath{\chi}$ with salt concentration. In this sense, we find a clear correlation between the deswelling ability of the ions and their chaotropic (structure breaking) or kosmotropic (structure making) nature as classified in the Hofmeister series.

We confine charged spheres in cells with the smallest dimension along the direction of gravity $\stackrel{\ifmmode \hat{}\else \^{}\fi{}}{g}$. The particles are density mismatched with the surrounding medium and sediment along $\stackrel{\ifmmode \hat{}\else \^{}\fi{}}{g}$ with typical P\'eclet numbers of $\mathrm{Pe}\ensuremath{\approx}{10}^{\ensuremath{-}3}$. After a certain time, we find that the number of particles $N$ increases near both upper and lower plates until a characteristic time $\ensuremath{\tau}$ is reached; above this time $N$ plateaus. We attribute the observed phenomenology to collective particle motions driven by gravity and mediated by hydrodynamic interactions; these could yield formation of swirls made of particles with correlated velocities that could eventually drive the particles towards the upper plate. The characteristic time for these migrations scales with plate-to-plate separation ${L}_{z}$ as $\ensuremath{\tau}\ensuremath{\sim}{L}_{z}^{1.2}$, exactly as the characteristic decay time of velocity fluctuations in sedimentation processes [S. Y. Tee et al., Phys. Rev. Lett. 89, 054501 (2002)], despite that in these experiments the smallest cell dimension is perpendicular to $\stackrel{\ifmmode \hat{}\else \^{}\fi{}}{g}$ and $7l\mathrm{Pe}l50$. In the absence of gravitational field, the observed particle migrations disappear, emphasizing the key role played by gravity in these experiments.

Small-angle neutron scattering and dynamic light scattering have been used to study the thermodynamics of swelling and the associated structure modifications of highly cross-linked temperature-sensitive poly $(N$-isopropylacrylamide) [poly(NIPAM)] microgels in ${\mathrm{D}}_{2}\mathrm{O}.$ A particle core-shell model is proposed, with the core containing most of the cross-linker molecules. The Flory-Rehner theory, with the inclusion of a concentration dependent Flory solvency parameter, successfully describes the experimental swelling, despite the inhomogeneous character of the particles. Interestingly, the shell evolution with temperature controls the whole particle swelling, exerting an external pressure over the core, which in turn influences its size during the swelling process. Scaling laws for the correlation lengths were found with respect to temperature and polymer concentration. Finally, it has been encountered that for the collapsed microgel states, the particle surface seems to have a fractal character.

We investigate the nonlinear effects related to the formation of particle-counterion clusters in highly charged asymmetric colloidal suspensions. The ocurrence of such clustering is experimentally probed by studying the stability of the colloidal system. The results demonstrate that a renormalized charge is needed in order to explain the observed critical coagulation concentrations. This renormalization is predicted by an extension of the Debye-Hückel-Bjerrum liquid state theory [A. Diehl, M. C. Barbosa, and Y. Levin, Europhys. Lett. 53, 86 (2001)]. Therefore, counterion condensation seems to become apparent in particle aggregation processes through control of the repulsive barrier that keeps the system stable. As a consequence of the agreement, new insights into the microscopic state of highly charged complex fluids follow.