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Addition of particles to a viscoelastic suspension dramatically alters the properties of the mixture, particularly when it is sheared or otherwise processed. Shear-induced stretching of the polymers results in elastic stress that causes a substantial increase in measured viscosity with increasing shear, and an attractive interaction between particles, leading to their chaining. At even higher shear rates, the flow becomes unstable, even in the absence of particles. This instability makes it very difficult to determine the properties of a particle suspension. Here we use a fully immersed parallel plate geometry to measure the high-shear-rate behavior of a suspension of particles in a viscoelastic fluid. We find an unexpected separation of the particles within the suspension resulting in the formation of a layer of particles in the center of the cell. Remarkably, monodisperse particles form a crystalline layer which dramatically alters the shear instability. By combining measurements of the velocity field and torque fluctuations, we show that this solid layer disrupts the flow instability and introduces a new, single-frequency component to the torque fluctuations that reflects a dominant velocity pattern in the flow. These results highlight the interplay between particles and a suspending viscoelastic fluid at very high shear rates., Comment: SI Videos and future data sharing are available at https://doi.org/10.7910/DVN/K0XZ6N

Despite significant advances in particle imaging technologies over the past two decades, few advances have been made in particle tracking, i.e. linking individual particle positions across time series data. The state-of-the-art tracking algorithm is highly effective for systems in which the particles behave mostly independently. However, these algorithms become inaccurate when particle motion is highly correlated, such as in dense or strongly interacting systems. Accurate particle tracking is essential in the study of the physics of dense colloids, such as the study of dislocation formation, nucleation, and shear transformations. Here, we present a new method for particle tracking that incorporates information about the correlated motion of the particles. We demonstrate significant improvement over the state-of-the-art tracking algorithm in simulated data on highly correlated systems., Comment: 6 pages, 5 figures

Elastomeric materials when sliding on clean and rough surfaces generate wrinkles at the interface due to tangential stress gradients. These interfacial folds travel along the bottom of elastomer as surface detachment waves to facilitate the apparent sliding motion of elastomer. At very low sliding speed compared to elastic surface waves, the process is dominated by surface adhesion and relaxation effects, and the phenomenon is historically referred to as Schallamach waves. We report in this letter the observation of fast-traveling intersonic detachment waves exceeding the Rayleigh and shear wave velocities of the soft material in contact. The spatio-temporal analysis revealed the accelerating nature of the detachment wave, and the scaling of wave speed with the elastic modului of the material suggests that this process is governed by elasticity and inertia. Multiple wave signatures on the plot were connected to different stages of surface wrinkles, as they exhibited distinctive slopes (from which velocities were derived) in the generation, propagation and rebound phases. We also characterized the frequencies of wrinkle generation in addition to the speeds and found a consistent scaling law of these two wave characteristics as the stiffness of elastomer increased. Physical implications of this new finding may further promote our understanding of elastomer noise generation mechanisms, as at macroscopic sliding velocity, the frequency of elastomer instability readily enters human audible ranges and interacts with other vibratory frequencies to cooperatively create harsh and detrimental noises in disc braking, wiper blade and shoe squeaking among many other elastomer applications.

We demonstrate a new class of elastic waves in the bulk: When longitudinal and transverse components propagate at the same speed, rolling waves with a spin that is not parallel to the wave vector can emerge. First, we give a general definition of spin for traveling waves. Then, since rolling waves cannot exist in isotropic solids, we derive conditions for anisotropic media and proceed to design architected materials capable of hosting rolling waves. Numerically, we show spin manipulations by reflection. Structures reported in this work can be fabricated using available techniques, opening new possibilities for spin technologies in acoustics, mechanics and phononics.

Three-dimensional, time-dependent direct simulations of step emulsification micro-devices highlight two essential mechanisms for droplet formation: first, the onset of an adverse pressure gradient driving a back-flow of the continuous phase from the external reservoir to the micro-channel. Second, the striction of the flowing jet which leads to its subsequent rupture. It is also shown that such a rupture is delayed and eventually suppressed by increasing the flow speed of the dispersed phase within the channel, due to the stabilising effect of dynamic pressure. This suggests a new criterion for dripping-jetting transition, based on local values of the Capillary and Weber numbers., Comment: 8 pages, 6 figures

Fully three-dimensional, time-dependent, direct simulations of the non-ideal Navier-Stokes equations for a two-component fluid, shed light into the mechanism which inhibits droplet breakup in step emulsifiers below a critical threshold of the the width-to-height ($w/h$) ratio of the microfluidic nozzle. Below $w/h \sim 2.6$, the simulations provide evidence of a smooth topological transition of the fluid from the confined rectangular channel geometry to an isotropic (spherical) expansion of the fluid downstream the nozzle step. Above such threshold, the transition from the inner to the outer space involves a series of dynamical rearrangements which keep the free surface in mechanical balance. Such rearrangements also induce a backflow of the ambient fluid which, in turn, leads to jet pinching and ultimately to its rupture, namely droplet formation. The simulations show remarkable agreement with the experimental value of the threshold, which is found around $w/h \sim 2.56$., Comment: 12 pages, 5 figures

Series of short contributions that are part of Nobel Symposium 162 - Microfluidics arXiv:1712.08369., Comment: Nobel Symposium 162, Stockholm, Sweden, 2017 arXiv:1712.08369v1 Report-no: Nobel162/2017/00

Solid-state transformation is often accompanied by mechanical expansion/compression, due to their volume change and structural evolution at interfaces at the atomic scale. However, these two types of dynamics are usually difficult to monitor in the same time. In this work, we use in-situ transmission electron microscopy to directly study the reduction transformation at the AgCl-Ag interface. Three stages of lattice fluctuations were identified and correlated to the structural evolution. During the steady state, a quasi-layered growth mode of Ag in both vertical and lateral directions were observed due to the confinement of AgCl lattices. The development of planar defects and depletion of AgCl are respectively associated with lattice compression and relaxation. Topography and structure of decomposing AgCl was further monitored by in-situ scanning transmission electron microscopy. Silver species are suggested to originate from both the surface and the interior of AgCl, and be transported to the interface. Such mass transport may have enabled the steady state and lattice compression in this volume-shrinking transformation., Comment: 21 pages, 5 figures; accepted for publication in J. Phys. Chem. Lett

We present a regularized version of the color gradient lattice Boltzmann (LB) scheme for the simulation of droplet formation in microfluidic devices of experimental relevance. The regularized version is shown to provide computationally efficient access to Capillary number regimes relevant to droplet generation via microfluidic devices, such as flow-focusers and the more recent microfluidic step emulsifier devices., Comment: 9 pages, 5 figures

The relationship between the microstructure of a porous medium and the observed flow distribution is still a puzzle. We resolve it with an analytical model, where the local correlations between adjacent pores, which determine the distribution of flows propagated from one pore downstream, predict the flow distribution. Numerical simulations of a two-dimensional porous medium verify the model and clearly show the transition of flow distributions from $\delta$-function-like via Gaussians to exponential with increasing disorder. Comparison to experimental data further verifies our numerical approach., Comment: 5 pages, 3 figures, supplemental material

Self-healing polymers crosslinked by solely reversible bonds are intrinsically weaker than common covalently crosslinked networks. Introducing covalent crosslinks into a reversible network would improve mechanical strength. It is challenging, however, to apply this design concept to dry elastomers, largely because reversible crosslinks such as hydrogen bonds are often polar motifs, whereas covalent crosslinks are non-polar motifs, and these two types of bonds are intrinsically immiscible without co-solvents. Here we design and fabricate a hybrid polymer network by crosslinking randomly branched polymers carrying motifs that can form both reversible hydrogen bonds and permanent covalent crosslinks. The randomly branched polymer links such two types of bonds and forces them to mix on the molecular level without co-solvents. This allows us to create a hybrid dry elastomer that is very tough with a fracture energy $13,500J/m^2$ comparable to that of natural rubber; moreover, the elastomer can self-heal at room temperature with a recovered tensile strength 4 MPa similar to that of existing self-healing elastomers. The concept of forcing covalent and reversible bonds to mix at molecular scale to create a homogenous network is quite general and should enable development of tough, self-healing polymers of practical usage.

As an injury heals, an embryo develops, or a carcinoma spreads, epithelial cells systematically change their shape. In each of these processes cell shape is studied extensively, whereas variation of shape from cell-to-cell is dismissed most often as biological noise. But where do cell shape and variation of cell shape come from? Here we report that cell shape and shape variation are mutually constrained through a relationship that is purely geometrical. That relationship is shown to govern maturation of the pseudostratified bronchial epithelial layer cultured from both non-asthmatic and asthmatic donors as well as formation of the ventral furrow in the epithelial monolayer of the Drosophila embryo in vivo. Across these and other vastly different epithelial systems, cell shape variation collapses to a family of distributions that is common to all and potentially universal. That distribution, in turn, is accounted for quantitatively by a mechanistic theory of cell-cell interaction showing that cell shape becomes progressively less elongated and less variable as the layer becomes progressively more jammed. These findings thus uncover a connection between jamming and geometry that is generic -spanning jammed living and inert systems alike- and demonstrate that proximity of the cell layer to the jammed state is the principal determinant of the most primitive features of epithelial cell shape and shape variation., Comment: First three authors had equal contribution | Video links are given in the Supplementary Videos section (pages 31-32)

Crystals with low latent heat are predicted to melt from an entropically stabilized body-centered cubic symmetry. At this weakly first-order transition, strongly correlated fluctuations are expected to emerge, which could change the nature of the transition. Here we show how large fluctuations stabilize bcc crystals formed from charged colloids, giving rise to strongly power-law correlated heterogeneous dynamics. Moreover, we find that significant nonaffine particle displacements lead to a vanishing of the nonaffine shear modulus at the transition. We interpret these observations by reformulating the Born-Huang theory to account for nonaffinity, illustrating a scenario of ordered solids reaching a state where classical lattice dynamics fail.

Cells actively probe and respond to the stiffness of their surroundings. Since mechanosensory cells in connective tissue are surrounded by a disordered network of biopolymers, their in vivo mechanical environment can be extremely heterogeneous. Here, we investigate how this heterogeneity impacts mechanosensing by modeling the cell as an idealized local stiffness sensor inside a disordered fiber network. For all types of networks we study, including experimentally-imaged collagen and fibrin architectures, we find that measurements applied at different points throughout a given network yield a strikingly broad range of local stiffnesses, spanning roughly two decades. We verify via simulations and scaling arguments that this broad range of local stiffnesses is a generic property of disordered fiber networks, and show that the range can be further increased by tuning specific network features, including the presence of long fibers and the proximity to elastic transitions. These features additionally allow for a highly tunable dependence of stiffness on probe length. Finally, we show that to obtain optimal, reliable estimates of global tissue stiffness, a cell must adjust its size, shape, and position to integrate multiple stiffness measurements over extended regions of space., Comment: 30 pages, 14 figures

Collagen is the main structural and load-bearing element of various connective tissues, where it forms the extracellular matrix that supports cells. It has long been known that collagenous tissues exhibit a highly nonlinear stress-strain relationship (Fung YC, Am J Physiol 213(6),1967; Humphrey JD, Proc R Soc Lond A: Math Phys Eng Sci 459(2029),2003), although the origins of this nonlinearity remain unknown (McMahon TA, Lec Math Life Sci 13,1980). Here, we show that the nonlinear stiffening of reconstituted type I collagen networks is controlled by the applied stress, and that the network stiffness becomes surprisingly insensitive to network concentration. We demonstrate how a simple model for networks of elastic fibers can quantitatively account for the mechanics of reconstituted collagen networks. Our model points to the important role of normal stresses in determining the nonlinear shear elastic response, which can explain the approximate exponential relationship between stress and strain reported for collagenous tissues (Fung YC, Am J Physiol 213(6),1967). This further suggests new principles for the design of synthetic fiber networks with collagen-like properties, as well as a mechanism for the control of the mechanics of such networks., Comment: manuscript: 9 pages, 3 figures, supporting information: 5 pages, 7 figures

We use confocal microscopy to directly visualize the simultaneous flow of both a wetting and a non-wetting fluid through a model three-dimensional (3D) porous medium. We find that, for small flow rates, both fluids flow through unchanging, distinct, connected 3D pathways; in stark contrast, at sufficiently large flow rates, the non-wetting fluid is broken up into discrete ganglia. By performing experiments over a range of flow rates, using fluids of different viscosities, and with porous media having different geometries, we show that this transition can be characterized by a state diagram that depends on the capillary numbers of both fluids, suggesting that it is controlled by the competition between the viscous forces exerted on the flowing oil and the capillary forces at the pore scale. Our results thus help elucidate the diverse range of behaviors that arise in two-phase flow through a 3D porous medium., Comment: Physics of Fluids (2014)

We use confocal microscopy to directly visualize the formation and complex morphologies of trapped non-wetting fluid ganglia within a model 3D porous medium. The wetting fluid continues to flow around the ganglia after they form; this flow is characterized by a capillary number, Ca. We find that the ganglia configurations do not vary for small Ca; by contrast, as Ca is increased above a threshold value, the largest ganglia start to become mobilized and are ultimately removed from the medium. By combining our 3D visualization with measurements of the bulk transport, we show that this behavior can be quantitatively understood by balancing the viscous forces exerted on the ganglia with the pore-scale capillary forces that keep them trapped within the medium. Our work thus helps elucidate the fluid dynamics underlying the mobilization of a trapped non-wetting fluid from a 3D porous medium.

We study the deformations of pH-responsive spherical microcapsules -- micrometer-scale liquid drops surrounded by thin, solid shells -- under the influence of electrostatic forces. When exposed to a large concentration of NaOH, the microcapsules become highly charged, and expand isotropically. We find that the extent of this expansion can be understood by coupling electrostatics with shell theory; moreover, the expansion dynamics is well described by Darcy's law for fluid flow through the microcapsule shell. Unexpectedly, however, below a threshold NaOH concentration, the microcapsules begin to disintegrate, and eventually rupture; they then expand non-uniformly, ultimately forming large, jellyfish-like structures. Our results highlight the fascinating range of behaviors exhibited by pH-responsive microcapsules, driven by the interplay between electrostatic and mechanical forces., Comment: Supplementary information available online at journal webpage

We use confocal microscopy to directly visualize the spatial fluctuations in fluid flow through a three-dimensional porous medium. We find that the velocity magnitudes and the velocity components both along and transverse to the imposed flow direction are exponentially distributed, even with residual trapping of a second immiscible fluid. Moreover, we find pore-scale correlations in the flow that are determined by the geometry of the medium. Our results suggest that, despite the considerable complexity of the pore space, fluid flow through it is not completely random., Comment: In press, Physical Review Letters

We show that when a non-wetting fluid drains a stratified porous medium at sufficiently small capillary numbers Ca, it flows only through the coarsest stratum of the medium; by contrast, above a threshold Ca, the non-wetting fluid is also forced laterally, into part of the adjacent, finer strata. The spatial extent of this partial invasion increases with Ca. We quantitatively understand this behavior by balancing the stratum-scale viscous pressure driving the flow with the capillary pressure required to invade individual pores. Because geological formations are frequently stratified, we anticipate that our results will be relevant to a number of important applications, including understanding oil migration, preventing groundwater contamination, and sub-surface CO$_{2}$ storage.

We report an approach to fully visualize the flow of two immiscible fluids through a model three-dimensional (3D) porous medium at pore-scale resolution. Using confocal microscopy, we directly image the drainage of the medium by the non-wetting oil and subsequent imbibition by the wetting fluid. During imbibition, the wetting fluid pinches off threads of oil in the narrow crevices of the medium, forming disconnected oil ganglia. Some of these ganglia remain trapped within the medium. By resolving the full 3D structure of the trapped ganglia, we show that the typical ganglion size, and the total amount of residual oil, decreases as the capillary number Ca increases; this behavior reflects the competition between the viscous pressure in the wetting fluid and the capillary pressure required to force oil through the pores of the medium. This work thus shows how pore-scale fluid dynamics influence the trapped fluid configurations in multiphase flow through 3D porous media.

Colloidal capsules can sustain an external osmotic pressure; however, for a sufficiently large pressure, they will ultimately buckle. This process can be strongly influenced by structural inhomogeneities in the capsule shells. We explore how the time delay before the onset of buckling decreases as the shells are made more inhomogeneous; this behavior can be quantitatively understood by coupling shell theory with Darcy's law. In addition, we show that the shell inhomogeneity can dramatically change the folding pathway taken by a capsule after it buckles., Comment: In press; Physical Review Letters (2012)

We present a simple method for accessing the elastic properties of microscopic deformable particles. This method is based on measuring the pressure-induced deformation of soft particles as they are forced through a tapered glass microcapillary. It allows us to determine both the compressive and the shear modulus of a deformable object in one single experiment. Measurements on a model system of poly-acrylamide microgel particles exhibit excellent agreement with measurements on bulk gels of identical composition. Our approach is applicable over a wide range of mechanical properties and should thus be a valuable tool for the characterization of a variety of soft and biological materials.

Microfluidic devices can be used to produce highly controlled and monodisperse double or multiple emulsions. The presence of inner drops inside a jet of the middle phase introduces deformations in the jet, which leads to breakup into monodisperse double emulsions. However, the ability to generate double emulsions can be compromised when the interfacial tension between the middle and outer phases is low, leading to flow with high capillary and Weber numbers. In this case, the interface between the fluids is initially deformed by the inner drops but the jet does not break into drops. Instead, the jet becomes highly corrugated, which prevents formation of controlled double emulsions. We show using numerical calculations that the corrugations are caused by the inner drops perturbing the interface and the perturbations are then advected by the flow into complex shapes.

We show how attractive interactions dramatically influence emulsion rheology. Unlike the repulsive case, attractive emulsions below random close packing, RCP, can form soft gel-like elastic solids. However, above RCP, attractive and repulsive emulsions have similar elasticities. Such compressed attractive emulsions undergo an additional shear-driven relaxation process during yielding. Our results suggest that attractive emulsions begin to yield at weak points through the breakage of bonds, and, above RCP, also undergo droplet configurational rearrangements.

Drops impacting on a surface are ubiquitous in our everyday experience. This impact is understood within a commonly accepted hydrodynamic picture: it is initiated by a rapid shock and a subsequent ejection of a sheet leading to beautiful splashing patterns. However, this picture ignores the essential role of the air that is trapped between the impacting drop and the surface. Here we describe a new imaging modality that is sensitive to the behavior right at the surface. We show that a very thin film of air, only a few tens of nanometers thick, remains trapped between the falling drop and the surface as the drop spreads. The thin film of air serves to lubricate the drop enabling the fluid to skate on the air film laterally outward at surprisingly high velocities, consistent with theoretical predictions. Eventually this thin film of air must break down as the fluid wets the surface. We suggest that this occurs in a spinodal-like fashion, and causes a very rapid spreading of a wetting front outwards; simultaneously the wetting fluid spreads inward much more slowly, trapping a bubble of air within the drop. Our results show that the dynamics of impacting drops are much more complex than previously thought and exhibit a rich array of unexpected phenomena that require rethinking classical paradigms., Comment: 4 pages, 4 figures

We introduce a new experimental approach to study the structural transitions of large numbers of nanoparticle-coated droplets as their volume is reduced. We use an emulsion system where the dispersed phase is slightly soluble in the continuous phase. By adding a fixed amount of unsaturated continuous phase, the volume of the droplets can be controllably reduced, causing them to buckle or crumple, thereby becoming nonspherical. The resultant morphologies depend both on the extent of volume reduction and the average droplet size. The buckling and crumpling behavior implies that the droplet surfaces are solid., Comment: Supporting information (pictures, text, movie) available free of charge online at http://pubs.acs.org/doi/abs/10.1021/la103874z

Cytoskeletal networks of biopolymers are cross-linked by a variety of proteins. Experiments have shown that dynamic cross-linking with physiological linker proteins leads to complex stress relaxation and enables network flow at long times. We present a model for the mechanical properties of transient networks. By a combination of simulations and analytical techniques we show that a single microscopic timescale for cross-linker unbinding leads to a broad spectrum of macroscopic relaxation times, resulting in a weak power-law dependence of the shear modulus on frequency. By performing rheological experiments, we demonstrate that our model quantitatively describes the frequency behavior of actin network cross-linked with $\alpha$-Actinin-$4$ over four decades in frequency., Comment: 4 pages

We investigate the 3D structure and drying dynamics of complex mixtures of emulsion droplets and colloidal particles, using confocal microscopy. Air invades and rapidly collapses large emulsion droplets, forcing their contents into the surrounding porous particle pack at a rate proportional to the square of the droplet radius. By contrast, small droplets do not collapse, but remain intact and are merely deformed. A simple model coupling the Laplace pressure to Darcy's law correctly estimates both the threshold radius separating these two behaviors, and the rate of large-droplet evacuation. Finally, we use these systems to make novel hierarchical structures., Comment: 4 pages, 4 figures

We present a technique to locally and rapidly heat water drops in microfluidic devices with microwave dielectric heating. Water absorbs microwave power more efficiently than polymers, glass, and oils due to its permanent molecular dipole moment that has a large dielectric loss at GHz frequencies. The relevant heat capacity of the system is a single thermally isolated picoliter drop of water and this enables very fast thermal cycling. We demonstrate microwave dielectric heating in a microfluidic device that integrates a flow-focusing drop maker, drop splitters, and metal electrodes to locally deliver microwave power from an inexpensive, commercially available 3.0 GHz source and amplifier. The temperature of the drops is measured by observing the temperature dependent fluorescence intensity of cadmium selenide nanocrystals suspended in the water drops. We demonstrate characteristic heating times as short as 15 ms to steady-state temperatures as large as 30 degrees C above the base temperature of the microfluidic device. Many common biological and chemical applications require rapid and local control of temperature, such as PCR amplification of DNA, and can benefit from this new technique., Comment: 6 pages, 4 figures

We present further evidence that gelation is an arrested phase separation in attractive colloid-polymer mixtures, based on a method combining confocal microscopy experiments with numerical simulations recently established in {\bf Nature 453, 499 (2008)}. Our results are independent of the form of the interparticle attractive potential, and therefore should apply broadly to any attractive particle system with short-ranged, isotropic attractions. We also give additional characterization of the gel states in terms of their structure, inhomogeneous character and local density., Comment: 6 figures, to be published in J. Phys. Condens. Matter, special issue for EPS Liquids Conference 2008

The drying dynamics in three dimensional porous media are studied with confocal microscopy. We observe abrupt air invasions in size from single particle to hundreds of particles. We show that these result from the strong flow from menisci in large pores to menisci in small pores during drying. This flow causes air invasions to start in large menisci and subsequently spread throughout the entire system. We measure the size and structure of the air invasions and show that they are in accord with invasion percolation. By varying the particle size and contact angle we unambiguously demonstrate that capillary pressure dominates the drying process., Comment: 5 pages, 4 figures

We study the micromechanics of collagen-I gel with the goal of bridging the gap between theory and experiment in the study of biopolymer networks. Three-dimensional images of fluorescently labeled collagen are obtained by confocal microscopy and the network geometry is extracted using a 3d network skeletonization algorithm. Each fiber is modeled as a worm-like-chain that resists stretching and bending, and each cross-link is modeled as torsional spring. The stress-strain curves of networks at three different densities are compared to rheology measurements. The model shows good agreement with experiment, confirming that strain stiffening of collagen can be explained entirely by geometric realignment of the network, as opposed to entropic stiffening of individual fibers. The model also suggests that at small strains, cross-link deformation is the main contributer to network stiffness whereas at large strains, fiber stretching dominates. Since this modeling effort uses networks with realistic geometries, this analysis can ultimately serve as a tool for understanding how the mechanics of fibers and cross-links at the microscopic level produce the macroscopic properties of the network. While the focus of this paper is on the mechanics of collagen, we demonstrate a framework that can be applied to many biopolymer networks.

Vorticity aligned cylindrical flocs of carbon black particles are coincident with a primary shear thickening transition in steady flow and also appear as transient structures in the flow response of gels produced by a secondary shear thickening at high shear rates., Comment: 6 pages, 7 figures v2: Added normal stress data; Added optical micrograph of structures under steady shear Published in Soft Matter

Dilute oil dispersions of fractal carbon black particles with attractive Van der Waals interactions display continuous shear thickening followed by shear thinning at high shear rates. The shear thickening transition occurs at $\dot\gamma_{c}\approx 10^{2}-10^{3}s^{-1}$ and is driven by hydrodynamic breakup of clusters. Pre-shearing dispersions at shear rates $\dot\gamma>\dot\gamma_{c}$ produces enhanced-modulus gels where $G' \sim \sigma_{pre-shear}^{1.5-2}$ and is directly proportional to the residual stress in the gel measured at a fixed sample age. The observed data can be accounted for using a simple scaling model for the breakup of fractal clusters under shear stress., Comment: 5 pages, 5 figures; v2: treating low shear rate date separately; edited title; reworked figures

We use a confocal microscope to examine the motion of individual particles in a dense colloidal suspension. Close to the glass transition, particle motion is strongly spatially correlated. The correlations decay exponentially with particle separation, yielding a dynamic length scale of O(2-3 sigma) (in terms of particle diameter sigma). This length scale grows modestly as the glass transition is approached. Further, the correlated motion exhibits a strong spatial dependence on the pair correlation function g(r). Motion within glassy samples is weakly correlated, but with a larger spatial scale for this correlation., Comment: Submitted to J Phys: Cond Mat; for Workshop on Nonequilibrium Phenomena in Glasses (Pisa, September 2006)

The rheological properties of soft materials often exhibit surprisingly universal linear and non-linear features. Here we show that these properties can be unified by considering the effect of the strain-rate amplitude on the structural relaxation of the material. We present a new form of oscillatory rheology, Strain-Rate Frequency Superposition (SRFS), where the strain-rate amplitude is fixed as the frequency is varied. We show that SRFS can isolate the response due to structural relaxation, even when it occurs at frequencies too low to be accessible with standard techniques., Comment: 4 pages, 4 figures

While the important role of electrostatic interactions in aqueous colloidal suspensions is widely known and reasonably well-understood, the relevance of charge in nonpolar suspensions remains mysterious. We demonstrate that particles can have surprisingly strong electrostatic interactions in low dielectric constant environments when ions are solubilized by reverse micelles. A simple thermodynamic model, relating the structure of the micelles to the equilibrium ionic strength, is in good agreement with both conductivity and interaction measurements. Since dissociated ions are solubilized by reverse micelles, the entropic incentive to charge a particle surface is qualitatively changed, and surface entropy plays a important role., Comment: 4 pages, three figures

We show that geometric confinement dramatically affects the shear-induced configurations of dense mono-disperse colloidal suspensions; a new structure emerges, where layers of particles buckle to stack in a more efficient packing. The volume fraction in the shear zone is controlled by a balance between the viscous stresses and the osmotic pressure of a contacting reservoir of unsheared particles. We present a model that accounts for our observations and helps elucidate the complex interplay between particle packing and shear stress for confined suspensions., Comment: 10 pages, 4 figures

Increment 53 - 54 Science Symposium presentation of Advanced Colloids Experiment (ACE-H-2) to RPO. The purpose of this event is for Principal Investigators to present their science objectives, testing approach, and measurement methods to agency scientists, managers, and other investigators.

This invention generally relates to systems and methods for the formation and/or control of fluidic species, and articles produced by such systems and methods. In some cases, the invention involves unique fluid channels, systems, controls, and/or restrictions, and combinations thereof. In certain embodiments, the invention allows fluidic streams (which can be continuous or discontinuous, i.e., droplets) to be formed and/or combined, at a variety of scales, including microfluidic scales. In one set of embodiments, a fluidic stream may be produced from a channel, where a cross-sectional dimension of the fluidic stream is smaller than that of the channel, for example, through the use of structural elements, other fluids, and/or applied external fields, etc. In some cases, a Taylor cone may be produced. In another set of embodiments, a fluidic stream may be manipulated in some fashion, for example, to create tubes (which may be hollow or solid), droplets, nested tubes or droplets, arrays of tubes or droplets, meshes of tubes, etc. In some cases, droplets produced using certain embodiments of the invention may be charged or substantially charged, which may allow their further manipulation, for instance, using applied external fields. Non-limiting examples of such manipulations include producing charged droplets, coalescing droplets (especially at the microscale), synchronizing droplet formation, aligning molecules within the droplet, etc. In some cases, the droplets and/or the fluidic streams may include colloids, cells, therapeutic agents, and the like.

The Advanced Colloids Experiment is being conducted on the International Space Station (ISS) using the Light Microscopy Module (LMM) in the Fluids Integrated Rack (FIR). Work to date will be discussed and future plans and opportunities will be highlighted. The LMM is a microscope facility designed to allow scientists to process, manipulate, and characterize colloidal samples in micro-gravity where the absence of gravitational settling and particle jamming enables scientists to study such things as:a.The role that disordered and ordered-packing of spheres play in the phase diagram and equation of state of hard sphere systems,b.crystal nucleation and growth, growth instabilities, and the glass transition, c.gelation and phase separation of colloid polymer mixtures,d.crystallization of colloidal binary alloys,e.competition between crystallization and phase separation,f.effects of anisotropy and specific interactions on packing, aggregation, frustration and crystallization,g.effects of specific reversible and irreversible interactions mediated in the first case by hybridization of complementary DNA strands attached to separate colloidal particles,h.Lock and key interactions between colloids with dimples and spheres which match the size and shape of the dimples,i.finding the phase diagrams of isotropic and interacting particles,j.new techniques for complex self-assembly including scenarios for self-replication, k.critical Casimir forces,l.biology (real and model systems) in microgravity,m.etc. By adding additional microscopy capabilities to the existing LMM, NASA will increase the tools available for scientists that fly experiments on the ISS enabling scientists to observe directly what is happening at the particle level. Presently, theories are needed to bridge the gap between what is being observed (at a macroscopic level when photographing samples) with what is happening at a particle (or microscopic) level. What is happening at a microscopic level will be directly accessible with the availability of the Light Microscopy Module (LMM) on ISS. To meet these goals, the ACE experiment is being built-up in stages, with the availability of confocal microscopy being the ultimate objective. Supported by NASAs Physical Sciences Research Program, ESAESTEC, and the authors respective governments.

The Binary Colloidal Alloy Test - 5: Phase Separation (BCAT-5-PhaseSep) experiment will photograph initially randomized colloidal samples onboard the ISS to determine their resulting structure over time. This allows the scientists to capture the kinetics (evolution) of their samples, as well as the final equilibrium state of each sample. BCAT-5-PhaseSep studies collapse (phase separation rates that impact product shelf-life); in microgravity the physics of collapse is not masked by being reduced to a simple top and bottom phase as it is on Earth.

The Binary Colloidal Alloy Test - 5: Compete (BCAT-5-Compete) investigation will photograph andomized colloidal samples onboard the International Space Station (ISS) to determine their resulting structure over time. The use of EarthKAM software and hardware will allow the scientists to capture the kinetics (evolution) of their samples, as well as the final equilibrium state of each sample. BCAT-5-Compete will utilize samples 6 - 8 in the BCAT-5 hardware to study the competition between phase separation and crystallization, which is important in the manufacture of plastics and other materials.

Binary Colloidal Alloy Test - 3 and 4: Critical Point (BCAT-3-4-CP) will determine phase separation rates and add needed points to the phase diagram of a model critical fluid system. Crewmembers photograph samples of polymer and colloidal particles (tiny nanoscale spheres suspended in liquid) that model liquid/gas phase changes. Results will help scientists develop fundamental physics concepts previously cloaked by the effects of gravity.

The Physics of Colloids in Space (PCS) experiment was accommodated within International Space Station (ISS) EXpedite the PRocessing of Experiments to Space Station (EXPRESS) Rack 2 and was remotely operated from early June 2001 until February 2002 from NASA Glenn Research Center's Telescience Support Center (TSC) in Cleveland, Ohio, and from the remote site at Harvard University in Cambridge, Massachusetts. PCS was launched on 4/19/2001 on Space Shuttle STS-100. The experiment was activated on 5/31/2001. The entire experimental setup performed remarkably well, and accomplished 2400 hours of science operations on-orbit. The sophisticated instrumentation in PCS is capable of dynamic and static light scattering from 11 to 169 degrees, Bragg scattering over the range from 10 to 60 degrees, dynamic and static light scattering at low angles from 0.3 to 6.0 degrees, and color imaging. The long duration microgravity environment on the ISS facilitated extended studies on the growth and coarsening characteristics of binary crystals. The de-mixing of the colloid-polymer critical-point sample was also studied as it phase-separated into two phases. Further, aging studies on a col-pol gel, gelation rate studies in extremely low concentration fractal gels over several days, and studies on a glass sample, all provided valuable information. Several exciting and unique aspects of these results are discussed here.

We have pursued the use of biological crosslinking molecules of several types to make colloidal materials at relatively low volume fraction of colloidal particles. The objective is to make binary alloys of colloidal particles, made of two different colloidal particles coated with complementary biological lock-and-key binding molecules, which assemble due to the biological specificity. The long-term goal is to use low affinity lock-and-key biological interactions, so that the can anneal to form crystalline states. We have used a variety of different surface chemistries in order to make colloidal materials. Our first system involved using selectin-carbohydrate (sialyl-Lewis) interactions; this chemistry is derived from immune system. This chemical interaction is of relatively low affinity, with timescales for dissociation of several seconds. Furthermore, the adhesion mediated by these molecules can be reversed by the chelation of calcium atoms; thus assembled structures can be disassembled reversibly. Our second system employed avidin-biotin chemistry. This well-studied system is of high affinity, and is generally irreversible on a laboratory time-scale. Thus, we would expect selectin-carbohydrate interactions at high molecular density and avidin-biotin interactions to give kinetically-trapped structures; however, at low densities, we would expect significant differences in the structure and dynamics of the two materials, owing to their very different release rates. We have also begun to use a third chemistry - DNA hybridization. By attaching single stranded DNA oligonucleotide chains to beads, we can drive the assembly of colloidal materials by hybridization of complementary DNA chains. It is well known that DNA adenosine-thymine (A-T) and guanine-cytosine (G-C) bases hybridize pairwise with a Gibbs free energy change of 1.7 kcal/mol per base; thus, the energy of the assembly can be modulated by altering the number of complementary bases in the DNA chains. Using these different crosslinking molecules, we have assembled colloidal materials from different-sized colloidal particles, A and B. In the first sets of experiment, we used high densities of adhesion molecules, and 0.96 micron (A) and 5.5 micron (B) diameter particles. The high density of adhesion molecules means that the structures are kinetically trapped in nonequilibrium configurations. The structure of the suspension can be varied by changing the number ratio of the two types of colloidal particles, NA and NB, where A is the smaller particle. With carbohydrate-selectin or avidin-biotin interactions, large NA/NB leads to the formation of colloidal micelles, with the large center B particle surrounded by many smaller A particles. As the ratio NA/NB decreases, the structures become more extended, approaching the formation of macro-Rouse polymers - extended linear chains where A beads are connected with intervening small B linkers.

The Physics of Colloids in Space is an experiment which flew in the ISS. Data on several different samples of colloidal particles were obtained. They provided unexpected information about the behavior of the samples in microgravity. The data are currently being analyzed. The most recent findings will be discussed in this talk.

Particle Image Velocimetry (PIV) is used to study the slow settling motions of spheres in suspensions ranging from dilute to highly concentrated, 0.05 less than phi less than 0.50. During sedimentation, velocity fluctuations are found to be organized into regions of characteristic size L approximately 11 a phi(exp-1/3) and buoyant mass DELTA m given by the rms density fluctuations in a region of size L(sup 3) assuming random statistics with excluded volume effects. A simple model accurately predicts the magnitudes of the velocity fluctuations DELTA V. Finally, we find a new universal relation for particle diffusion during sedimentation that can be written in a Stokes-Einstein type form as D approximately (DELTA mg L)/(6 pi eta L), where the effective temperature DELTA mg L is the gravitational potential energy of density fluctuations.

We have studied colloidal aggregation in a model colloid plus polymer system with short-range attractive interactions. By varying the colloid concentration and the strength of the attraction, we explored regions where the equilibrium phase is expected to consist of colloidal crystallites in coexistance with colloidal gas (i.e. monomers). This occurs for moderate values of the potential depth, U approximately equal to 2-5 kT. Crystallization was not always observed. Rather, over an extended sub-region two new metastable phases appear, one fluid-like and one solid-like. These were examined in detail with light scattering and microscopy techniques. Both phases consist of a near uniform distribution of small irregular shaped clusters of colloidal particles. The dynamical and structural characteristics of the ergodic-nonergodic transition between the two phases share much in common with the colloidal hard sphere glass transition.