Coarsening of Quasi Two-Dimensional Emulsions Formed by Islands in Free-Standing Smectic Films.

We study the coarsening behavior of assemblies of islands on smectic A freely suspended films in ISS microgravity experiments. The islands can be regarded as liquid inclusions in a two-dimensional fluid in analogy to liquid droplets of the discontinuous phase of an emulsion. The coarsening is effectuated by two processes, predominantly by island coalescence, but to some extend also by Ostwald ripening, whereby large islands grow at the expense of surrounding smaller ones. A peculiarity of this system is that the continuous and the discontinuous phases consist of the same material. We determine the dynamics, analyze the self-similar aging of the island size distribution and discuss characteristic exponents of the mean island growth.

Coalescence of biphasic droplets embedded in free standing smectic A films.

We investigate micrometer-sized flat droplets consisting of an isotropic core surrounded by a nematic rim in freely suspended smectic A liquid-crystal films. In contrast to purely isotropic droplets which are characterized by a sharp edge and no long-range interactions, the nematic fringe introduces a continuous film thickness change resulting in long-range mutual attraction of droplets. The coalescence scenario is divided in two phases. The first one consists in the fusion of the nematic regions. The second phase involves the dissolution of a thin nematic film between the two isotropic cores. The latter has many similarities with the rupture of thin liquid films between droplets coalescing in an immiscible viscous liquid.

The structure of disintegrating defect clusters in smectic C freely suspended films.

Disclinations or disclination clusters in smectic C freely suspended films with topological charges larger than one are unstable. They disintegrate, preferably in a spatially symmetric fashion, into single defects with individual charges of +1, which is the smallest positive topological charge allowed in polar vector fields. While the opposite process of defect annihilation is well-defined by the initial defect positions, disintegration starts from a singular state and the following scenario including the emerging regular defect patterns must be selected by specific mechanisms. We analyze experimental data and compare them with a simple model where the defect clusters adiabatically pass quasi-equilibrium solutions in one-constant approximation. It is found that the defects arrange in geometrical patterns that correspond very closely to superimposed singular defect solutions, without additional director distortions. The patterns expand by affine transformations where all distances between individual defects scale with the same time-dependent scaling factor proportional to the square-root of time.

Shape instabilities of islands in smectic films under lateral compression.

Smectic liquid crystals are fluids, and in most rheological situations they behave as such. Nevertheless, when thin freely floating films of smectic A or smectic C materials are compressed quickly in-plane, they resist such stress by buckling similar to solid membranes under lateral stress. We report experimental observations of wrinkling and bulging of finite domains within the films, so-called islands, and give a qualitative explanation of different observed patterns. Depending on the external stress and their dimensions, the islands can expel a specifically shaped bulge in their center, form radial wrinkles or develop target-like wrinkle structures. When the external stress is relaxed, these patterns disappear reversibly.

Smectic free-standing films under fast lateral compression.

Smectic freely-suspended films can wrinkle like solid sheets. This has been demonstrated earlier with shape-fluctuating smectic bubbles. Here, we exploit the collapse of smectic catenoid films with a central equatorial film to expose the latter to rapid lateral compression. Wrinkle formation is observed in the planar film and the thickness dependence of the undulation wavelength is measured. In addition to the central film, its border undergoes an undulation instability as well.

Force chains in crystalline and frustrated packing visualized by stress-birefringent spheres.

Force networks play an important role in the stability of configurations when granular material is packed into a container. These networks can redirect part of the weight of grains inside a container to the side walls. We employ monodisperse stress-birefringent spheres to visualize the contact forces in a quasi-2D and a nearly-2D configuration of these spheres in a thin cuboid cell. The packing structures are particularly simple: a hexagonal lattice in the ground state when the cell width is equal to the sphere diameter, and a frustrated, slightly distorted lattice in thicker cells. The force redistribution is substantially changed by this geometrical modification. In both cases, we observe an 'inverse' Janssen effect with the pressure decreasing from the top to the bottom of the container when the material is loaded with a weight on top of the vessel.

Silo discharge of mixtures of soft and rigid grains.

We study the outflow dynamics and clogging phenomena of mixtures of soft, elastic low-friction spherical grains and hard frictional spheres of similar size in a quasi-two-dimensional (2D) silo with narrow orifice at the bottom. Previous work has demonstrated the crucial influence of elasticity and friction on silo discharge. We show that the addition of small amounts, even as low as 5%, of hard grains to an ensemble of soft, low-friction grains already has significant consequences. The mixtures allow a direct comparison of the probabilities of the different types of particles to clog the orifice. We analyze these probabilities for the hard, frictional and the soft, slippery grains on the basis of their participation in the blocking arches, and compare outflow velocities and durations of non-permanent clogs for different compositions of the mixtures. Experimental results are compared with numerical simulations. The latter strongly suggest a significant influence of the inter-species particle friction.

Self similarity of liquid droplet coalescence in a quasi-2D free-standing liquid-crystal film.

Coalescence of droplets is an ubiquitous phenomenon in chemical, physical and biological systems. The process of merging of liquid objects has been studied during the past years experimentally and theoretically in different geometries. We introduce a unique system that allows a quasi two-dimensional description of the coalescence process: Micrometer-sized flat droplets in freely suspended smectic liquid-crystal films. We find that the bridge connecting the droplets grows linearly in time during the initial stage of coalescence, both with respect to its height and lateral width. We also verify self-similar dynamics of the bridge during the first stage of coalescence. We compare our results with a model based on the thin sheet equations. Our experiments confirm that the most important geometrical parameter influencing the coalescence rate is the contact angle of the droplets.

Intermittent flow and transient congestions of soft spheres passing narrow orifices.

Soft, low-friction particles in silos show peculiar features during their discharge. The outflow velocity and the clogging probability both depend upon the momentary silo fill height, in sharp contrast to silos filled with hard particles. The reason is the fill-height dependence of the pressure at the orifice. We study the statistics of silo discharge of soft hydrogel spheres. The outflow is found to become increasingly fluctuating and even intermittent with decreasing orifice size, and with decreasing fill height. In orifices narrower than two particle diameters, outflow can stop completely, but in contrast to clogs formed by rigid particles, these congestions may dissolve spontaneously. We analyze such non-permanent congestions and attribute them to slow reorganization processes in the container, caused by viscoelasticity of the material.

Dynamic wrinkling of freely floating smectic films.

We demonstrate spontaneous wrinkling as a transient dynamical pattern in thin freely floating smectic liquid-crystalline films. The peculiarity of such films is that, while behaving liquid-like with respect to flow in the film plane, they cannot quickly expand their thickness because that requires stacking of additional smectic layers. At short time scales, they therefore behave like quasi-incompressible membranes, very different from soap films. Smectic films can develop a transient undulation instability or form bulges in response to lateral compression. Optical experiments with freely floating bubbles on parabolic flights and in ground lab experiments are reported. The characteristic wavelengths of the wrinkles are in the submillimeter range. We demonstrate the dynamic nature of the pattern formation mechanism and develop a basic model that explains the physical mechanism for the wavelength selection and wrinkle orientation.

The role of structural anisotropy in the magnetooptical response of an organoferrogel with mobile magnetic nanoparticles.

We investigate the structure and the magnetooptical response of isotropic and anisotropic fibrillous organoferrogels with mobile magnetic nanoparticles (MNPs). We demonstrate that the presence of the gel network restricts the magnetooptical response of the ferrogel. Even though the ferrogel exhibits no magnetic hysteresis, an optical hysteresis has been found. This suggests that the magnetooptical response is primarily determined by the dynamics of self-assembly of the MNPs into shape-anisotropic agglomerates. Furthermore, we show that the optical anisotropy of the system can be fine-tuned by varying the concentration of the gelator and the MNPs, respectively. The optical response in structurally anisotropic gels becomes orientation-dependent, revealing an intricate interplay between the gel mesh and the MNPs.

Frequency-dependent conversion of the torque of a rotating magnetic field on a ferrofluid confined in a spherical cavity.

The dynamics of magnetic nanoparticles in rotating magnetic fields is studied both experimentally and theoretically. The experimental investigation is focused on the conversion of the magnetic forces to a mechanical torque acting on a ferrofluid confined in a spherical cavity in a rotating magnetic field. Polydispersity usually present in diluted ferrofluids is shown to play a crucial role in the torque conversion. Important features observed experimentally are reproduced theoretically in studies on the dynamics of particles with uniaxial magnetic anisotropy in the presence of thermal noise. The phase lag between the rotating magnetic field and the induced rotating magnetization, as well as the corresponding torque which is transferred to the carrier fluid because of the mutual coupling between both, is analyzed as a function of the particle size. It is shown that for large particles the magnetic moment is locked to the anisotropy axis. On lowering the particle radius, Néel relaxation becomes increasingly important. Illustrative numerical calculations demonstrating this behavior are performed for magnetic parameters typical for iron oxide.

Structure and dynamics of a two-dimensional colloid of liquid droplets.

Droplet arrays in thin, freely suspended liquid-crystalline smectic A films can form two-dimensional (2D) colloids. The droplets interact repulsively, arranging locally in a more or less hexagonal arrangement with only short-range spatial and orientational correlations and local lattice cell parameters that depend on droplet size. In contrast to quasi-2D colloids described earlier, there is no 3D bulk liquid subphase that affects the hydrodynamics. Although the films are surrounded by air, the droplet dynamics are genuinely 2D, the mobility of each droplet in its six-neighbor cage being determined by the ratio of cage and droplet sizes, rather than by the droplet size as in quasi-2D colloids. These experimental observations are described well by Saffman's model of a diffusing particle in a finite 2D membrane. The experiments were performed in microgravity, on the International Space Station.

Free Cooling of a Granular Gas of Rodlike Particles in Microgravity.

Granular gases as dilute ensembles of particles in random motion are at the basis of elementary structure-forming processes in the Universe, involved in many industrial and natural phenomena, and also excellent models to study fundamental statistical dynamics. The essential difference to molecular gases is the energy dissipation in particle collisions. Its most striking manifestation is the so-called granular cooling, the gradual loss of mechanical energy E(t) in the absence of external excitation. We report an experimental study of homogeneous cooling of three-dimensional granular gases in microgravity. The asymptotic scaling E(t)∝t^{-2} obtained by Haff's minimal model [J. Fluid Mech. 134, 401 (1983)JFLSA70022-112010.1017/S0022112083003419] proves to be robust, despite the violation of several of its central assumptions. The shape anisotropy of the grains influences the characteristic time of energy loss quantitatively but not qualitatively. We compare kinetic energies in the individual degrees of freedom and find a slight predominance of translational motions. In addition, we observe a preferred rod alignment in the flight direction, as known from active matter or animal flocks.

Frustrated packing in a granular system under geometrical confinement.

Optimal packings of uniform spheres are solved problems in two and three dimensions. The main difference between them is that the two-dimensional ground state can be easily achieved by simple dynamical processes while in three dimensions, this is impossible due to the difference in the local and global optimal packings. In this paper we show experimentally and numerically that in 2 + ε dimensions, realized by a container which is in one dimension slightly wider than the spheres, the particles organize themselves in a triangular lattice, while touching either the front or rear side of the container. If these positions are denoted by up and down the packing problem can be mapped to a 1/2 spin system. At first it looks frustrated with spin-glass like configurations, but the system has a well defined ground state built up from isosceles triangles. When the system is agitated, it evolves very slowly towards the potential energy minimum through metastable states. We show that the dynamics is local and is driven by the optimization of the volumes of 7-particle configurations and by the vertical interaction between touching spheres.

Optically driven translational and rotational motions of microrod particles in a nematic liquid crystal.

A small amount of azo-dendrimer molecules dissolved in a liquid crystal enables translational and rotational motions of microrods in a liquid crystal matrix under unpolarized UV light irradiation. This motion is initiated by a light-induced trans-to-cis conformational change of the dendrimer adsorbed at the rod surface and the associated director reorientation. The bending direction of the cis conformers is not random but is selectively chosen due to the curved local director field in the vicinity of the dendrimer-coated surface. Different types of director distortions occur around the rods, depending on their orientations with respect to the nematic director field. This leads to different types of motions driven by the torques exerted on the particles by the director reorientations.

Smectic C to smectic A transition induced mechanically by the rupture of freely suspended liquid crystal films.

The tilt angle of smectic C phases can be controlled by external forces of very different nature. In particular near a smectic A-smectic C transition, it is susceptible to temperature changes. It can be influenced with electric fields (electroclinic effect), and even mechanically by intra-layer stresses in elastomers. We show that capillary forces that act during the rupture of a free-standing smectic C film can trigger a smectic C to smectic A transition, which rapidly reduces the surface area of the films, concurrently increasing the film thickness. The effect occurs on the sub-millisecond scale, practically independent of film thickness and temperature. We propose that this mechanical effect could even trigger a ferroelectric to paraelectric transition in chiral phases.

Doping of nematic cyanobiphenyl liquid crystals with mesogen-hybridized magnetic nanoparticles.

Magnetic nanoparticles (MNPs) functionalized with (pro-)mesogenic ligands are implemented into a nematic liquid crystal (LC) and studied regarding both colloidal stability and magneto-optical behavior. In this study, the particle surface is specifically engineered to tune the MNP interactions with the LC host. For this purpose, four types of (pro-)mesogenic ligands (ML) are synthesized, which are composed of three structural parts, i.e., a rigid, LC motif (i.e., cyanobiphenyl) and a functional group for nanoparticle binding, both linked via a flexible spacer of different alkyl chain lengths. Electrostatically stabilized CoFe2O4 and γ-Fe2O3 nanoparticles with narrow size distribution and sizes below 3 nm are obtained via co-precipitation and subsequently functionalized to yield MNP@ML nanoparticles. Studies on the behaviour of the MNP@ML nanoparticles in the commercial LC host (i.e., 4-pentyl-4'-cyanobiphenyl (5CB)) in the bulk and in thin films in LC test cells, reveal the initial formation of some heterogeneities after transition from the isotropic to the nematic phase. Homogenous MNP@ML-5CB hybrids with long-term, colloidal stability, however, are obtained after magnetic separation of initially formed particle aggregates. In particular, MLs with carboxy groups and high structural flexibility (i.e., long linker lengths) are shown to be well suited to form stable MNP colloids, allowing for high MNP doping levels. As compared to undoped 5CB, the CoFe2O4@MLx-5CB hybrids show an increased sensitivity to the magnetic field, affecting the Fréedericksz transition. The strongest effect, however, is observed in magnetic and electric fields. The coupling of the ultrasmall, spherical MNPs with the LC director in the magnetic field suggests the formation of LC-induced, anisometric MNP clusters.

Photomanipulation of the anchoring strength using a spontaneously adsorbed layer of azo dendrimers.

We systematically studied the photoinduced anchoring transition in a nematic liquid crystal containing azo dendrimers. Because the azo dendrimers in the trans-isomer state were spontaneously adsorbed at substrate surfaces, which was confirmed by optical second-harmonic generation (SHG), a homeotropic orientation was established at the first stage. Ultraviolet (UV) light irradiation triggered a transition into a planar state which was accompanied by a suppression of the SH generation. The monotonic decrease of the effective scalar order parameter with increasing UV light intensity was determined by polarized attenuated total reflection infrared (ATR-IR) spectroscopy. The variation of anchoring strength and extrapolation length was evaluated by observing the Fréedericksz transition as a function of UV light intensity at a certain visible (VIS) light intensity. Such a photoinduced variation can be interpreted as a variation of the anchoring strength depending on the trans/cis ratio at the surfaces based on a modified Rapini-Papoular model. Thus, this system provides the opportunity for a controlled change in the anchoring strength.

Colloidal Suspensions of Rodlike Nanocrystals and Magnetic Spheres under an External Magnetic Stimulus: Experiment and Molecular Dynamics Simulation.

Using experiments and molecular dynamics simulations, we explore magnetic field-induced phase transformations in suspensions of nonmagnetic rodlike and magnetic sphere-shaped particles. We experimentally demonstrate that an external uniform magnetic field causes the formation of small, stable clusters of magnetic particles that, in turn, induce and control the orientational order of the nonmagnetic subphase. Optical birefringence was studied as a function of the magnetic field and the volume fractions of each particle type. Steric transfer of the orientational order was investigated by molecular dynamics (MD) simulations; the results are in qualitative agreement with the experimental observations. By reproducing the general experimental trends, the MD simulation offers a cohesive bottom-up interpretation of the physical behavior of such systems, and it can also be regarded as a guide for further experimental research.