Kenneth W. Desmond

Random Close Packing of Disks and Spheres in Confined Geometries

Studies of random close packing of spheres have advanced our knowledge about the structure of systems such as liquids, glasses, emulsions, granular media, and amorphous solids. In confined geometries, the structural properties of random-packed systems will change. To understand these changes, we study random close packing in finite-sized confined systems, in both two and three dimensions. Each packing consists of a 50-50 binary mixture with particle size ratio of 1.4. The presence of confining walls significantly lowers the overall maximum area fraction (or volume fraction in three dimensions). A simple model is presented, which quantifies the reduction in packing due to wall-induced structure. This wall-induced structure decays rapidly away from the wall, with characteristic length scales comparable to the small particle diameter.

Spatial and temporal dynamical heterogeneities approaching the binary colloidal glass transition

We study concentrated binary colloidal suspensions, a model system which has a glass transition as the volume fraction ϕ of particles is increased. We use confocal microscopy to directly observe particle motion within dense samples with ϕ ranging from 0.4 to 0.7. Our binary mixtures have a particle diameter ratio dS/dL = 1/1.3 and particle number ratio NS/NL = 1.56, which are chosen to inhibit crystallization and enable long-time observations. Near the glass transition we find that particle dynamics are heterogeneous in both space and time. The most mobile particles occur in spatially localized groups. The length scales characterizing these mobile regions grow slightly as the glass transition is approached, with the largest length scales seen being ∼ 4 small particle diameters. We also study temporal fluctuations using the dynamic susceptibility χ4, and find that the fluctuations grow as the glass transition is approached. Analysis of both spatial and temporal dynamical heterogeneity show that the smaller species play an important role in facilitating particle rearrangements. The glass transition in our sample occurs at ϕg ≈ 0.58, with characteristic signs of aging observed for all samples with ϕ > ϕg.

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 over a wide range of area fractions ϕ. We study three bidisperse samples that jam at area fractions ϕc ≈ 0.86. Our data show that for ϕ > ϕc, the contact numbers and pressure have power-law dependence on ϕ − ϕc 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.

Measurement 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≥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.

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. For spheres, 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. 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 sphere packings with different particle radii distributions, varying polydispersity and skewness independently of one another. We find that the packing density can increase significantly with increasing skewness and in some cases skewness can have a larger effect than polydispersity. However, the packing fraction is relatively insensitive to the higher moment 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.

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.