Kazem V. Edmond

Colloidal glass transition observed in confinement

We study a colloidal suspension confined between two quasiparallel 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.

Decoupling of rotational and translational diffusion in supercooled colloidal fluids

We use confocal microscopy to directly observe 3D translational and rotational diffusion of tetrahedral clusters, which serve as tracers in colloidal supercooled fluids. We find that as the colloidal glass transition is approached, translational and rotational diffusion decouple from each other: Rotational diffusion remains inversely proportional to the growing viscosity whereas translational diffusion does not, decreasing by a much lesser extent. We quantify the rotational motion with two distinct methods, finding agreement between these methods, in contrast with recent simulation results. The decoupling coincides with the emergence of non-Gaussian displacement distributions for translation whereas rotational displacement distributions remain Gaussian. Ultimately, our work demonstrates that as the glass transition is approached, the sample can no longer be approximated as a continuum fluid when considering diffusion.

Brownian motion and the hydrodynamic friction tensor for colloidal particles of complex shape

We synthesize colloidal particles with various anisotropic shapes and track their orientationally resolved Brownian trajectories using confocal microscopy. An analysis of appropriate short-time correlation functions provides direct access to the hydrodynamic friction tensor of the particles revealing nontrivial couplings between the translational and rotational degrees of freedom. The results are consistent with calculations of the hydrodynamic friction tensor in the low-Reynolds-number regime for the experimentally determined particle shapes.

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 transformations 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.

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 liquidlike 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.

Boundary Mobility Controls Glassiness in 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.

Local influence of boundary conditions on a confined supercooled colloidal liquid

Abstract. 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.

Tracking the Brownian diffusion of a colloidal tetrahedral cluster

Related Articles Diffusion in periodic two-dimensional channels formed by overlapping circles: Comparison of analytical and numerical results J. Chem. Phys. 135, 224101 (2011) Asymmetric stochastic localization in geometry controlled kinetics J. Chem. Phys. 135, 194111 (2011) Simulation of conformational preconditioning strategies for electrophoretic stretching of DNA in a microcontraction Biomicrofluidics 5, 044106 (2011) The stochastisation hypothesis and the spacing of planetary systems J. Math. Phys. 52, 113502 (2011) Enhanced diffusion in conic channels by means of geometric stochastic resonance J. Chem. Phys. 135, 174102 (2011)

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.