Biomedical subjects

Roel P A Dullens

Publications and source records attributed to Roel P A Dullens.

10 recordsLinked to original sources

PubMed2006

Dynamic broadening of the crystal-fluid interface of colloidal hard spheres.

We investigate the structure and dynamics of the crystal-fluid interface of colloidal hard spheres in real space by confocal microscopy. Tuning the buoyancy of the particles allows us to study the interface close to and away from equilibrium. We find that the interface broadens from 8-9 particle diameters close to equilibrium to 15 particle diameters away from equilibrium. Furthermore, the interfacial velocity, i.e., the velocity by which the interface moves upwards, increases significantly. The increasing gravitational drive leads to supersaturation of the fluid above the crystal surface. This dramatically affects crystal nucleation and growth, resulting in the observed dynamic broadening of the crystal-fluid interface.

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PubMed2006

In situ imaging of field-induced hexagonal columns in magnetite ferrofluids.

Field-induced structures in a ferrofluid with well-defined magnetite nanoparticles with a permanent magnetic dipole moment are analyzed on a single-particle level by in situ cryogenic transmission electron microscopy (2D). The field-induced columnar phase locally exhibits hexagonal symmetry and confirms the structures observed in simulations for ferromagnetic dipolar fluids in 2D. The columns are distorted by lens-shaped voids, due to the weak interchain attraction relative to field-directed dipole-dipole attraction. Both dipolar coupling and the dipole concentration determine the dimensions and the spatial arrangement of the columns. Their regular spacing manifests long-range end-pole repulsions that eventually dominate the fluctuation-induced attractions between dipole chains that initiate the columnar transition.

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PubMed2006

Devitrification of colloidal glasses in real space.

Confocal scanning laser microscopy has been used to quantitatively analyze the structure and dynamics of concentrated suspensions of spherical colloids in which the magnitude of the short-range attractive potential is increased by adding nonadsorbing polymers. These systems undergo a reentrant glass transition upon increasing polymer concentration. We find that melting of the glass is accompanied by significant changes in the displacement distribution and its moments. However, no significant variations have been detected in the shapes of the displacement distributions. Moreover, structural correlation functions and the magnitude of local density fluctuations do not vary significantly between the glass states and the fluid. Considering our experimental setup, these observations imply that local density fluctuations cannot be larger than a few percent of the average density.

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PubMed2006

Quantitative real-space analysis of self-assembled structures of magnetic dipolar colloids.

We present the first real-space analysis on a single-particle level of the dipolar chains and branched clusters self-assembling in magnetic fluids in zero field. Spatial correlations and chain-length distributions directly obtained from tracked particle positions in vitrified films of synthetic magnetic (Fe3O4) dispersions provide a quantitative test for simulations and theory of dipolar fluids. A pertinent example is the cluster-size distribution that can be analyzed with a one-dimensional aggregation model to yield a dipolar attraction energy that agrees well with the dipole moment found from independent magnetization measurements.

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PubMed2006

Shape-induced frustration of hexagonal order in polyhedral colloids.

The effect of a nonspherical particle shape and shape polydispersity on the structure of densely packed hard colloidal particles was studied in real space by confocal microscopy. We show that the first layer at the wall of concentrated size-monodisperse but shape-polydisperse polyhedral colloids exhibits significant deviations from a hexagonal lattice. These deviations are identified as bond-orientational fluctuations which lead to percolating "mismatch lines." While the shape-induced geometrical frustration of the hexagonal symmetry suppresses translational order, bond-orientational order is clearly retained, indicating a hexaticlike structure of the polyhedral colloids.

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PubMed2006

Direct measurement of the free energy by optical microscopy.

We report the direct measurement of thermodynamic properties of colloidal hard spheres by optical microscopy. By using confocal microscopy, we obtain three-dimensional snapshots of a colloidal hard-sphere suspension over a wide range of densities. From these snapshots, the available volume to insert an additional sphere and the surface area of that volume are determined, which are directly related to the thermodynamics of the system. This procedure enables us to measure in a direct and noninterfering way, in principle, all thermodynamic properties, here demonstrated for the pressure, the chemical potential, and the free-energy density of a colloidal hard-sphere suspension. The "visual" determination of thermodynamic quantities opens up the possibility to experimentally study the relation between thermodynamics and geometry in real space beyond the hard-sphere potential.

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PubMed2005

Colloidal hard-sphere crystal growth frustrated by large spherical impurities.

Impurities affect the nucleation, growth, and structure of crystals. Here we report the effect of large, spherical, polymethylmethacrylate impurities on the crystal growth of monodisperse, hard, polymethylmethacrylate colloids in a density- and optically matching apolar solvent mixture. Crystal growth, initiated at the bottom of the sample, was studied by imaging sequences of two-dimensional xy slices in the plane of the impurity's center with a laser scanning confocal microscope. Impurities form the center of grain boundaries, and a single fluid particle layer around the impurity persists in all cases. The growth rate sensitively depends on the impurity's size. Crystal growth is inhibited to a greater extent near smaller impurities, pointing to local crystal frustration induced by the curvature of the impurity.

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PubMed2005

Topological lifetimes of polydisperse colloidal hard spheres at a wall.

Confocal scanning laser microscopy was used to study the behavior of dense suspensions of model colloidal hard spheres at a single wall. Due to the slight polydispersity, our system shows a reentrant melting transition at high densities involving a hexatic structure [Phys. Rev. Lett 92, 195702 (2004)]]. The reentrant melting transition is accompanied by an increase in the mean-squared displacement. The correlation between structure and dynamics was quantitatively analyzed on a single-particle level. In particular, the topological lifetime, being the average time that a particle spends having the same coordination number, is determined for all coordination numbers and as a function of volume fraction. The defective (non-sixfold-coordinated) particles exhibit shorter lifetimes than sixfold-coordinated particles, indicating that the mobility of the system is larger at or close to defective particles. The lifetime itself is a strong function of volume fraction. In particular, the global behavior of the mean-squared displacement is proportional to the hopping frequency (the inverse of the lifetime), showing that particles changing their coordination number contribute most to the local mobility.

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PubMed2004

Reentrant surface melting of colloidal hard spheres.

Concentrated suspensions of model colloidal hard spheres at a wall were studied in real space by means of time-resolved fluorescence confocal scanning microscopy. Both structure and dynamics of these systems differ dramatically from their bulk analogs (i.e., far away from a wall). In particular, systems that are a glass in the bulk show significant hexagonal order at a wall. Upon increasing the volume fraction of the colloids, a reentrant melting transition involving a hexatic structure is observed. The last observation points to two-dimensional behavior of matter at walls.

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PubMed2002

Layer-by-layer growth of binary colloidal crystals.

We report the growth of binary colloidal crystals with control over the crystal orientation through a simple layer-by-layer process. Well-ordered single binary colloidal crystals with a stoichiometry of large (L) and small (S) particles of LS2 and LS were generated. In addition, we observed the formation of an LS3 superstructure. The structures formed as a result of the templating effect of the first layer and the forces exerted by the surface tension of the drying liquid. By using spheres of different composition, one component can be selectively removed, as is demonstrated in the growth of a hexagonal non-close-packed colloidal crystal.

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