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Eric R. Weeks

Publications and source records attributed to Eric R. Weeks.

At least 55 records · Page 3Linked to original sources

Affine and non-affine motions in sheared polydisperse jammed emulsions

We study dense and highly polydisperse emulsions at droplet volume fractions ϕ>= 0.65. We apply oscillatory shear and observe droplet motion using confocal microscopy. The presence of droplets with sizes several times the mean size dramatically changes the motion of smaller droplets. Both affine and nonaffine droplet motions are observed, with the more nonaffine motion exhibited by the smaller droplets which are pushed around by the larger droplets. Droplet motions are correlated over length scales from one to four times the mean droplet diameter, with larger length scales corresponding to higher strain amplitudes (up to strains of about 6%).

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Soap films as two-dimensional fluids: Diffusion and flow fields

We observe tracer particles diffusing in soap films to measure the two-dimensional (2D) viscous properties of the films. We make soap films with a variety of water-glycerol mixtures and of differing thicknesses. The single-particle diffusivity relates closely to parameters of the film (such as thickness $h$) for thin films, but the relation breaks down for thicker films. Notably, the diffusivity is faster than expected for thicker films, with the transition at $h/d = 5.2 \pm 0.9$ using the tracer particle diameter $d$. This indicates a transition from purely 2D diffusion to diffusion that is more three-dimensional. Additionally, we measure larger length scale flow fields from correlated particle motions and find good agreement with what is expected from theory of 2D fluids for all our films, thin and thick. We measure the effective 2D viscosity of a soap film using single-particle diffusivity measurements in thin films, and using the two-particle correlation measurements in all films.

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Dynamic facilitation observed near the colloidal glass transition

We present experimental confirmation of dynamic facilitation in monodisperse and bidisperse colloidal suspensions near the glass transition volume fraction. Correlations in particle dynamics are seen to exist not only in space (clusters and strings) but also as bubbles in space-time. Quantitatively, highly mobile particles are more likely (than immobile particles) to have nearest neighbors that were highly mobile in immediately preceding times. The interpretation is that a particle's mobility enables or facilitates the subsequent motion of its neighbors. Facilitation is most pronounced at the relaxation time that corresponds with cage-breaking, when dynamic heterogeneity is also maximized.

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Boundary mobility controls glassiness of confined colloidal liquids

We use colloidal suspensions encapsulated in emulsion droplets to model confined glass-forming liquids with tunable boundary mobility. We show dynamics in these idealized systems are governed by physical interactions with the boundary. Gradients in dynamics are present for more mobile boundaries, whereas for less mobile boundaries gradients are almost entirely suppressed. Motions in a system are not isotropic, but have a strong directional dependence with respect to the boundary. These findings bring into question the ability of conventional quantities to adequately describe confined glasses.

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Influence of Particle Size Distribution on Random Close Packing

The densest amorphous packing of rigid particles is known as random close packing. It has long been appreciated that higher densities are achieved by using collections of particles with a variety of sizes. The variety of sizes is often quantified by the polydispersity of the particle size distribution: the standard deviation of the radius divided by the mean radius. Several prior studies quantified the increase of the packing density as a function of polydispersity. Of course, a particle size distribution is also characterized by its skewness, kurtosis, and higher moments, but the influence of these parameters has not been carefully quantified before. In this work, we numerically generate many packings with different particle radii distributions, varying polydispersity and skewness independently of one another. We find two significant results. First, the skewness can have a significant effect on the packing density and in some cases can have a larger effect than polydispersity. Second, the packing fraction is relatively insensitive to the value of the kurtosis. We present a simple empirical formula for the value of the random close packing density as a function of polydispersity and skewness.

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Experimental measurements of stress redistribution in flowing emulsions

We study how local rearrangements alter droplet stresses within flowing dense quasi-two-dimensional emulsions at area fractions $ϕ\geq 0.88$. Using microscopy, we measure droplet positions while simultaneously using their deformed shape to measure droplet stresses. We find that rearrangements alter nearby stresses in a quadrupolar pattern: stresses on neighboring droplets tend to either decrease or increase depending on location. The stress redistribution is more anisotropic with increasing $ϕ$. The spatial character of the stress redistribution influences where subsequent rearrangements occur. Our results provide direct quantitative support for rheological theories of dense amorphous materials that connect local rearrangements to changes in nearby stress.

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Local elastic response measured near the colloidal glass transition

We examine the response of a dense colloidal suspension to a local force applied by a small magnetic bead. For small forces, we find a linear relationship between the force and the displacement, suggesting the medium is elastic, even though our colloidal samples macroscopically behave as fluids. We interpret this as a measure of the strength of colloidal caging, reflecting the proximity of the samples' volume fractions to the colloidal glass transition. The strain field of the colloidal particles surrounding the magnetic probe appears similar to that of an isotropic homogeneous elastic medium. When the applied force is removed, the strain relaxes as a stretched exponential in time. We introduce a model that suggests this behavior is due to the diffusive relaxation of strain in the colloidal sample.

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Experimental study of forces between quasi-two-dimensional emulsion droplets near jamming

We experimentally study the jamming of quasi-two-dimensional emulsions. Our experiments consist of oil-in-water emulsion droplets confined between two parallel plates. From the droplet outlines, we can determine the forces between every droplet pair to within 8% over a wide range of area fractions $ϕ$. We study three bidisperse samples that jam at area fractions $ϕ_c \approx 0.86$. Our data show that for $ϕ> ϕ_c$, the contact numbers and pressure have power-law dependence on $ϕ-ϕ_c$ in agreement with the critical scaling found in numerical simulations. Furthermore, we see a link between the interparticle force law and the exponent for the pressure scaling, supporting prior computational observations. We also observe linear-like force chains (chains of large inter-droplet forces) that extend over 10 particle lengths, and examine the origin of their linearity. We find that the relative orientation of large force segments are random and that the tendency for force chains to be linear is not due to correlations in the direction of neighboring large forces, but instead occurs because the directions are biased towards being linear to balance the forces on each droplet.

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Slow dynamics in cylindrically confined colloidal suspensions

We study bidisperse colloidal suspensions confined within glass microcapillary tubes to model the glass transition in confined cylindrical geometries. We use high speed three-dimensional confocal microscopy to observe particle motions for a wide range of volume fractions and tube radii. Holding volume fraction constant, we find that particles move slower in thinner tubes. The tube walls induce a gradient in particle mobility: particles move substantially slower near the walls. This suggests that the confinement-induced glassiness may be due to an interfacial effect.

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Topological rearrangements and stress fluctuations in quasi-two-dimensional hopper flow of emulsions

We experimentally study the shear flow of oil-in-water emulsion droplets in a thin sample chamber with a hopper shape. In this thin chamber, the droplets are quasi-2D in shape. The sample is at an area fraction above jamming and forced to flow with a constant flux rate. Stresses applied to a droplet from its neighbors deform the droplet outline, and this deformation is quantified to provide an ad hoc measure of the stress. As the sample flows through the hopper we see large fluctuations of the stress, similar in character to what has been seen in other flows of complex fluids. Periods of time with large decreases in stress are correlated with bursts of elementary rearrangement events ("T1 events" where four droplets rearrange). More specifically, we see a local relationship between these observations: a T1 event decreases the inter-droplet forces up to 3 droplet diameters away from the event. This directly connects microscopic structural changes to macroscopic fluctuations, and confirms theoretical pictures of local rearrangements influencing nearby regions. These local rearrangements are an important means of reducing and redistributing stresses within a flowing material.

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In Search of Colloidal Hard Spheres

We recently reviewed the experimental determination of the volume fraction, $ϕ$, of hard-sphere colloids, and concluded that the absolute value of $ϕ$ was unlikely to be known to better than $\pm 3$-6%. Here, in a second part to that review, we survey effects due to softness in the interparticle potential, which necessitates the use of an {\em effective} volume fraction. We review current experimental systems, and conclude that the one that most closely approximates hard spheres remains polymethylmethacrylate spheres sterically stabilised by polyhydroxystearic acid `hairs'. For these particles their effective hard sphere diameter is around 1-10% larger than the core diameter, depending on the particle size. We argue that for larger colloids suitable for confocal microscopy, the effect of electrostatic charge cannot be neglected, so that mapping to hard spheres must be treated with caution.

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Measuring every particle's size from three-dimensional imaging experiments

Often experimentalists study colloidal suspensions that are nominally monodisperse. In reality these samples have a polydispersity of 4-10%. At the level of an individual particle, the consequences of this polydispersity are unknown as it is difficult to measure an individual particle size from microscopy. We propose a general method to estimate individual particle radii within a moderately concentrated colloidal suspension observed with confocal microscopy. We confirm the validity of our method by numerical simulations of four major systems: random close packing, colloidal gels, nominally monodisperse dense samples, and nominally binary dense samples. We then apply our method to experimental data, and demonstrate the utility of this method with results from four case studies. In the first, we demonstrate that we can recover the full particle size distribution {\it in situ}. In the second, we show that accounting for particle size leads to more accurate structural information in a random close packed sample. In the third, we show that crystal nucleation occurs in locally monodisperse regions. In the fourth, we show that particle mobility in a dense sample is correlated to the local volume fraction.

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Influence of Confinement on Dynamical Heterogeneities in Dense Colloidal Samples

We study a dense colloidal suspension confined between two quasiparallel glass plates as a model system for a supercooled liquid in confined geometries. We directly observe the three-dimensional Brownian motion of the colloidal particles using laser scanning confocal microscopy. The particles form dense layers along the walls, but crystallization is avoided as we use a mixture of two particle sizes. A normally liquid-like sample, when confined, exhibits slower diffusive motion. Particle rearrangements are spatially heterogeneous, and the shapes of the rearranging regions are strongly influenced by the layering. These rearranging regions become more planar upon confinement. The wall-induced layers and changing character of the spatially heterogeneous dynamics appear strongly connected to the confinement induced glassiness.

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A Free Energy Landscape for Cage Breaking of Three Hard Disks

We investigate cage breaking in dense hard disk systems using a model of three Brownian disks confined within a circular corral. This system has a six-dimensional configuration space, but can be equivalently thought to explore a symmetric one-dimensional free energy landscape containing two energy minima separated by an energy barrier. The exact free energy landscape can be calculated as a function of system size. Results of simulations show the average time between cage breaking events follows an Arrhenius scaling when the energy barrier is large. We also discuss some of the consequences of using a one-dimensional representation to understand dynamics in a multi-dimensional space, such as diffusion acquiring spatial dependence and discontinuities in spatial derivatives of free energy.

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The Physics of the Colloidal Glass Transition

As one increases the concentration of a colloidal suspension, the system exhibits a dramatic increase in viscosity. Structurally, the system resembles a liquid, yet motions within the suspension are slow enough that it can be considered essentially frozen. This kinetic arrest is the colloidal glass transition. For several decades, colloids have served as a valuable model system for understanding the glass transition in molecular systems. The spatial and temporal scales involved allow these systems to be studied by a wide variety of experimental techniques. The focus of this review is the current state of understanding of the colloidal glass transition. A brief introduction is given to important experimental techniques used to study the glass transition in colloids. We describe features of colloidal systems near and in glassy states, including tremendous increases in viscosity and relaxation times, dynamical heterogeneity, and ageing, among others. We also compare and contrast the glass transition in colloids to that in molecular liquids. Other glassy systems are briefly discussed, as well as recently developed synthesis techniques that will keep these systems rich with interesting physics for years to come.

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Tracking Rotational Diffusion of Colloidal Clusters

We describe a novel method of tracking the rotational motion of clusters of colloidal particles. Our method utilizes rigid body transfor- mations to determine the rotations of a cluster and extends conventional proven particle tracking techniques in a simple way, thus facilitating the study of rotational dynamics in systems containing or composed of colloidal clusters. We test our method by measuring dynamical properties of simulated Brownian clusters under conditions relevant to microscopy experiments. We then use the technique to track and describe the motions of a real colloidal cluster imaged with confocal microscopy.

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Incompressibility of polydisperse random close packed colloidal particles

We use confocal microscopy to study a random close packed sample of colloidal particles. We introduce an algorithm to estimate the size of each particle. Taking into account their sizes, we compute the compressibility of the sample as a function of wave vector $q$, and find that this compressibility vanishes linearly as $q \rightarrow 0$. The particle sizes must be considered to calculate the compressibility properly. These results also suggest that the experimental packing is hyperuniform.

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On measuring colloidal volume fractions

Hard-sphere colloids are popular as models for testing fundamental theories in condensed matter and statistical physics, from crystal nucleation to the glass transition. A single parameter, the volume fraction (phi), characterizes an ideal, monodisperse hard-sphere suspension. In comparing experiments with theories and simulation, researchers to date have paid little attention to likely uncertainties in experimentally-quoted phi values. We critically review the experimental measurement of phi in hard-sphere colloids, and show that while statistical uncertainties in comparing relative values of phi can be as low as 0.0001, systematic errors of 3-6% are probably unavoidable. The consequences of this are illustrated by way of a case study comparing literature data sets on hard-sphere viscosity and diffusion.

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