Optical trapping of interfaces at ultra-low interfacial tension.

We achieve active control of interfacial phenomena by optically trapping the interface using the gradient forces of a strongly focussed laser beam parallel to the interface. We illustrate our technique in a phase separated colloid-polymer mixture by distorting the interface in a very controlled way. The static structure of the manipulated interface as well as its dynamic relaxation behaviour are analysed. Both the statics and dynamics can be related to the capillary wave height-height correlation functions using the fluctuation dissipation theorem up to surprisingly large deformations of the interface. To underline the novelty and potential of our approach we also show multiple interface distortions and the controlled snap-off of liquid droplets.

Magnetic-field-induced nematic-nematic phase separation and droplet formation in colloidal goethite.

We demonstrate the suitability of polarization microscopy to study the recently discovered (parallel) nematic-(perpendicular) nematic phase separation. This novel type of phase transition is induced by applying an external magnetic field to a nematic liquid crystal of boardlike colloidal goethite and is due to an interplay between the intrinsic magnetic properties of goethite and the collective effect of liquid crystal formation. It is shown that the intense ochre colour of goethite does not preclude the use of polarization microscopy and interference colours, and that dichroism can give valuable qualitative information on the nature of the phases, their anchoring and their sedimentation and order parameter profiles. We also apply these techniques to study 'nematic-nematic tactoids': nematic droplets sedimenting within a nematic medium with mutually perpendicular orientations.

Magnetic field effects on tactoids of plate-like colloids.

We investigate the effect of a magnetic field on the shape and director field of nematic droplets in dispersions of sterically stabilized and charge-stabilized colloidal gibbsite platelets with a negative diamagnetic anisotropy. Depending on the magnetic field strength and tactoid size, we observe with polarized light microscopy several interesting structures, with different shapes and director fields both with and without defects. In particular, our findings provide the first experimental evidence for the existence of the split-core defect structure predicted ten years ago by Mkaddem and Gartland [Phys. Rev. E 62, 6694 (2000)]. The split-core structure is a metastable director-field configuration that can be stabilized by a sufficiently strong externally applied magnetic field but only if the diamagnetic anisotropy of the particles is negative. To account for our observations, we present a calculation of the stability regions of different shapes and director-field structures as a function of tactoid size, anchoring conditions, surface tension, elastic constants, and magnetic field strength. By fitting the experimental data to the theoretically predicted structures, we are able to extract values for the splay elastic constant, interfacial tension, and anchoring strength. Remarkably, we find significant differences between the two systems studied: for sterically stabilized gibbsite in bromotoluene the anchoring strength is one order of magnitude larger than that of aqueous gibbsite, with the latter exhibiting weak and the former strong anchoring of the director field to the interface. The splay elastic constants that we obtain are in agreement with earlier experiments, simulations, and theory, while the interfacial tension and anchoring strength are considerably larger than what was found in earlier experiments.

Tactoids of plate-like particles: size, shape, and director field.

We studied, by means of polarized light microscopy, the shape and director field of nematic tactoids as a function of their size in dispersions of colloidal gibbsite platelets in polar and apolar solvents. Because of the homeotropic anchoring of the platelets to the interface, we found large tactoids to be spherical with a radial director field, whereas small tactoids turn out to have an oblate shape and a homogeneous director field, in accordance with theoretical predictions. The transition from a radial to a homogeneous director field seems to proceed via two different routes depending in our case on the solvent. In one route, the what presumably is a hedgehog point defect in the center of the tactoid transforms into a ring defect with a radius that presumably goes to infinity with decreasing drop size. In the other route, the hedgehog defect is displaced from the center to the edge of the tactoid, where it becomes virtual again going to infinity with decreasing drop size. Furthermore, quantitative analysis of the tactoid properties provides us with useful information on the ratio of the splay elastic constant and the anchoring strength and the ratio of the anchoring strength and the surface tension.

Liquid crystal phase transitions in systems of colloidal platelets with bimodal shape distribution.

We have studied a system of polydisperse, charged colloidal gibbsite platelets with a bimodal distribution in the particle aspect ratio. We observe a density inversion of the coexisting isotropic and nematic phases as well as a three-phase equilibrium involving a lower density nematic phase, an isotropic phase of intermediate density, and a higher density columnar phase. To relate these phenomena to the bimodality of the shape distribution, we have calculated the liquid crystal phase behavior of binary mixtures of thick and thin hard platelets for various thickness ratios. The predictions are based on the Onsager-Parsons theory for the isotropic-nematic (I-N) transition combined with a modified Lennard-Jones-Devonshire cell theory for the columnar (C) state. For sufficiently large thickness ratios, the phase diagram features an I-N density inversion and triphasic I-N-C equilibrium, in agreement with experiment. The density inversion can be attributed to a marked shape fractionation among the coexisting phases with the thick species accumulating in the isotropic phase. At high concentrations, the theory predicts a coexistence between two columnar phases with distinctly different concentrations. In experiment, however, the demixing transition is pre-empted by a transition to a kinetically arrested, glassy state with structural features resembling a columnar phase.

Devitrification of the glassy state in suspensions of charged platelets.

Colloidal suspensions of charged gibbsite platelets at salt concentrations of 10(-2) M and below and with a sufficiently high particle concentration form a kinetically arrested, glassy state. We study the evolution of the glassy state in suspensions of three different gibbsite systems. Despite differences in size and polydispersity, we observe small, iridescent grains of the hexagonal columnar phase, for all these systems after periods of months to years. The connections between this devitrification phenomenon and the structure of the glassy state are discussed.

Orientation dependent Stokes drag in a colloidal liquid crystal.

Stokes drag on the (sub)micrometre scale plays a key role in phenomena ranging from Brownian motion to the rheology of particulate suspensions. We report the first measurement of the direction dependent Stokes drag in a nematic liquid crystal of colloidal rods, where the viscous forces are of equal importance to the elastic forces. By tracking a sedimenting sphere with combined fluorescence confocal microscopy and polarization microscopy we find that the Stokes drag for motion along the director is two times larger than for motion perpendicular to the director. This brings the unique viscoelastic properties of a colloidal liquid crystal into focus.