arXiv subjects

Eric R. Weeks

Publications and source records attributed to Eric R. Weeks.

At least 73 records · Page 4Linked to original sources

arXiv2011

Experimental verification of democratic particle motions by direct imaging of glassy colloidal systems

We analyze data from confocal microscopy experiments of a colloidal suspension to validate predictions of rapid sporadic events responsible for structural relaxation in a glassy sample. The trajectories of several thousand colloidal particles are analyzed, confirming the existence of rapid sporadic events responsible for the structural relaxation of significant regions of the sample, and complementing prior observations of dynamical heterogeneity. The emergence of relatively compact clusters of mobility allows the dynamics to transition between the large periods of local confinement within its potential energy surface, in good agreement with the picture envisioned long ago by Adam and Gibbs and Goldstein.

cond-mat.soft↗

arXiv2010

Glassy dynamics and dynamical heterogeneity in colloids

Concentrated colloidal suspensions are a well-tested model system which has a glass transition. Colloids are suspensions of small solid particles in a liquid, and exhibit glassy behavior when the particle concentration is high; the particles are roughly analogous to individual molecules in a traditional glass. Because the particle size can be large (100 nm - 1000 nm), these samples can be studied with a variety of optical techniques including microscopy and dynamic light scattering. Here we review the phenomena associated with the colloidal glass transition, and in particular discuss observations of spatial and temporally heterogeneous dynamics within colloidal samples near the glass transition. Although this Chapter focuses primarily on results from hard-sphere-like colloidal particles, we also discuss other colloidal systems with attractive or soft repulsive interactions.

cond-mat.soft↗

arXiv2010

The glass transition of two-dimensional binary soft disk mixtures with large size ratios

We simulate binary soft disk systems in two dimensions, and investigate how the dynamics slow as the area fraction is increased toward the glass transition. The "fragility" quantifies how sensitively the relaxation time scale depends on the area fraction, and the fragility strongly depends on the composition of the mixture. We confirm prior results for mixtures of particles with similar sizes, where the ability to form small crystalline regions correlates with fragility. However, for mixtures with particle size ratios above 1.4, we find that the fragility is not correlated with structural ordering, but rather with the spatial distribution of large particles. The large particles have slower motion than the small particles, and act as confining "walls" which slow the motion of nearby small particles. The rearrangement of these confining structures governs the lifetime of dynamical heterogeneity, that is, how long local regions exhibit anomalously fast or slow behavior. The strength of the confinement effect is correlated with the fragility and also influences the aging behavior of glassy systems.

cond-mat.soft↗

arXiv2010

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 $d_S/d_L=1/1.3$ and particle number ratio $N_S/N_L=1.56$, 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 $\sim 4$ small particle diameters. We also study temporal fluctuations using the dynamic susceptibility $χ_4$, 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 $ϕ_g \approx 0.58$, with characteristic signs of aging observed for all samples with $ϕ>ϕ_g$.

cond-mat.soft↗

arXiv2010

Local influence of boundary conditions on a confined supercooled colloidal liquid

We study confined colloidal suspensions as a model system which approximates the behavior of confined small molecule glass-formers. Dense colloidal suspensions become glassier when confined between parallel glass plates. We use confocal microscopy to study the motion of confined colloidal particles. In particular, we examine the influence particles stuck to the glass plates have on nearby free particles. Confinement appears to be the primary influence slowing free particle motion, and proximity to stuck particles causes a secondary reduction in the mobility of free particles. Overall, particle mobility is fairly constant across the width of the sample chamber, but a strong asymmetry in boundary conditions results in a slight gradient of particle mobility.

cond-mat.soft↗

arXiv2009

Microscopic Structural Relaxation in a Sheared Supercooled Colloidal Liquid

The rheology of dense amorphous materials under large shear strain is not fully understood, partly due to the difficulty of directly viewing the microscopic details of such materials. We use a colloidal suspension to simulate amorphous materials, and study the shear-induced structural relaxation with fast confocal microscopy. We quantify the plastic rearrangements of the particles in several ways. Each of these measures of plasticity reveals spatially heterogeneous dynamics, with localized regions where many particles are strongly rearranging by these measures. We examine the shapes of these regions and find them to be essentially isotropic, with no alignment in any particular direction. Furthermore, individual particles are equally likely to move in any direction, other than the overall bias imposed by the strain.

cond-mat.soft↗

arXiv2009

Characterization of chaotic motion in a rotating drum

Numerous studies have demonstrated the potential for simple fluid plus particle systems to produce complicated dynamical behavior. In this work, we study a horizontal rotating drum filled with pure glycerol and three large, heavy spheres. The rotation of the drum causes the spheres to cascade and tumble and thus interact with each other. We find several different behaviors of the spheres depending on the drum rotation rate. Simpler states include the spheres remaining well separated, or states where two or all three of the spheres come together and cascade together. We also see two more complex states, where two or three of the spheres move chaotically. We characterize these chaotic states and find that in many respects they are quite unpredictable. This experiment serves as a simple model system to demonstrate chaotic behavior in fluid dynamical systems.

physics.flu-dyn↗

arXiv2009

The equilibrium intrinsic crystal-liquid interface of colloids

We use confocal microscopy to study an equilibrated crystal-liquid interface in a colloidal suspension. Capillary waves roughen the surface, but locally the intrinsic interface is sharply defined. We use local measurements of the structure and dynamics to characterize the intrinsic interface, and different measurements find slightly different widths of this interface. In terms of the particle diameter $d$, this width is either $1.5d$ (based on structural information) or $2.4d$ (based on dynamics), both not much larger than the particle size. This work is the first direct experimental visualization of an equilibrated crystal-liquid interface.

cond-mat.soft↗

arXiv2009

Flow fields in soap films: relating surface viscosity and film thickness

We follow the diffusive motion of colloidal particles in soap films with varying $h/d$, where $h$ is the thickness of the film and $d$ the diameter of the particles. The hydrodynamics of these films are determined by looking at the correlated motion of pairs of particles as a function of separation $R$. The Trapeznikov approximation [A. A. Trapeznikov, \emph{PICSA} (1957)] is used to model soap films as an effective interface in contact with bulk air phases, that behaves as a 2D fluid. The flow fields determined from correlated particle motions show excellent agreement with what is expected for the theory of 2D fluids for all our films where $0.6 \leq h/d \leq 14.3$, with the surface viscosity matching that predicted by Trapeznikov. However, for thicker films with $h/d > 7 \pm 3$, single particle motion is faster than expected. Additionally, while the flow fields still match those expected for 2D fluids, the parameters of these flow fields change markedly for thick films. Our results indicate a transition from 2D to 3D fluid-like behavior occurs at this value of $h/d$.

cond-mat.soft↗

arXiv2009

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. When these systems are confined their structural properties 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 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.

cond-mat.soft↗

arXiv2008

2D to 3D transition in soap films demonstrated by microrheology

We follow the diffusive motion of colloidal particles of diameter $d$ in soap films of varying thickness $h$ with fluorescence microscopy. Diffusion constants are obtained both from one- and two-particle microrheological measurements of particle motion in these films. These diffusion constants are related to the surface viscosity of the interfaces comprising the soap films, by means of the Trapeznikov approximation [A. A. Trapeznikov, \emph{PICSA} (1957)] and Saffman's equation for diffusion in a 2D fluid. Unphysical values of the surface viscosity are found for thick soap films ($h/d > 7$), indicating a transition from 2D to 3D behavior.

cond-mat.soft↗

arXiv2008

Dynamics and structure of an aging binary colloidal glass

We study aging in a colloidal suspension consisting of micron-sized particles in a liquid. This system is made glassy by increasing the particle concentration. We observe samples composed of particles of two sizes, with a size ratio of 1:2.1 and a volume fraction ratio 1:6, using fast laser scanning confocal microscopy. This technique yields real-time, three-dimensional movies deep inside the colloidal glass. Specifically, we look at how the size, motion and structural organization of the particles relate to the overall aging of the glass. Particles move in spatially heterogeneous cooperative groups. These mobile regions tend to be richer in small particles, and these small particles facilitate the motion of nearby particles of both sizes.

cond-mat.soft↗

arXiv2008

Quantitative imaging of colloidal flows

We present recent advances in the instrumentation and analysis methods for quantitative imaging of concentrated colloidal suspensions under flow. After a brief review of colloidal imaging, we describe various flow geometries for two and and three-dimensional (3D) imaging, including a `confocal rheoscope'. This latter combination of a confocal microscope and a rheometer permits simultaneous characterization of rheological response and 3D microstructural imaging. The main part of the paper discusses in detail how to identify and track particles from confocal images taken during flow. After analyzing the performance of the most commonly used colloid tracking algorithm by Crocker and Grier extended to flowing systems, we propose two new algorithms for reliable particle tracking in non-uniform flows to the level of accuracy already available for quiescent systems. We illustrate the methods by applying it to data collected from colloidal flows in three different geometries (channel flow, parallel plate shear and cone-plate rheometry).

cond-mat.soft↗

arXiv2008

From particles to spins: Eulerian formulation of supercooled liquids and glasses

The dynamics of supercooled liquid and glassy systems are usually studied within the Lagrangian representation, in which the positions and velocities of distinguishable interacting particles are followed. Within this representation, however, it is difficult to define measures of spatial heterogeneities in the dynamics, as particles move in and out of any one given region within long enough times. It is also non-transparent how to make connections between the structural glass and the spin glass problems within the Lagrangian formulation. We propose an Eulerian formulation of supercooled liquids and glasses that allows for a simple connection between particle and spin systems, and that permits the study of dynamical heterogeneities within a fixed frame of reference similar to the one used for spin glasses. We apply this framework to the study of the dynamics of colloidal particle suspensions for packing fractions corresponding to the supercooled and glassy regimes, which are probed via confocal microscopy.

cond-mat.dis-nn↗

arXiv2007

Three-dimensional imaging of colloidal glasses under steady shear

Using fast confocal microscopy we image the three-dimensional dynamics of particles in a yielded hard-sphere colloidal glass under steady shear. The structural relaxation, observed in regions with uniform shear, is nearly isotropic but is distinctly different from that of quiescent metastable colloidal fluids. The inverse relaxation time $τ_α^{-1}$ and diffusion constant $D$, as functions of the {\it local} shear rate $\dotγ$, show marked shear thinning with $τ_α^{-1} \propto D \propto \dotγ^{0.8}$ over more than two decades in $\dotγ$. In contrast, the {\it global} rheology of the system displays Herschel-Bulkley behavior. We discuss the possible role of large scale shear localization and other mechanisms in generating this difference.

cond-mat.soft↗

arXiv2007

Colloidal glass transition observed in confinement

We study a colloidal suspension confined between two quasi-parallel walls as a model system for glass transitions in confined geometries. The suspension is a mixture of two particle sizes to prevent wall-induced crystallization. We use confocal microscopy to directly observe the motion of colloidal particles. This motion is slower in confinement, thus producing glassy behavior in a sample which is a liquid in an unconfined geometry. For higher volume fraction samples (closer to the glass transition), the onset of confinement effects occurs at larger length scales.

cond-mat.soft↗

arXiv2006

Two-Particle Microrheology of quasi-2D Viscous Systems

We study the correlated motions of colloidal particles in a quasi-2D system (Human Serum Albumin (HSA) protein molecules at an air-water interface) for different surface viscosities $η_{s}$. We observe a transition in the behavior of the correlated motion, from 2-D interface dominated at high $η_{s}$ to bulk fluid-dependent at low $η_{s}$. The correlated motions can be scaled onto a master curve which captures the features of this transition. This master curve also characterizes the spatial dependence of the flow field of a viscous interface in response to a force. From the flow field and the correlated particle motions, we calculate a two-particle MSD (mean square displacement) for direct comparison with rheological measurements.

cond-mat.soft↗

arXiv2006

Short and long range correlated motion observed in colloidal glasses and liquids

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.

cond-mat.dis-nn↗