Optothermally driven colloidal transport in a confined nematic liquid crystal.

We demonstrate transport of microparticles by rapid movement of a laser spot in a thin layer of a nematic liquid crystal. The transport is achieved by fluid flow, caused by two different mechanisms. The thermoviscous expansion effect induces colloidal transport in the direction opposite to the laser movement, whereas thermally induced local melting of the liquid crystal pulls the particles in the direction of the laser movement. We demonstrate control of colloidal transport by changing the speed of the laser trap movement and the laser power. We anticipate that complex optofluidic colloidal transport could be realized in the nematic liquid crystal using a channel-free optofluidic approach.

Dynamics of topological monopoles annihilation on a fibre in a thick and thin nematic layer.

We study topological defect annihilation on a glass fibre with homeotropic surface anchoring of nematic liquid crystal molecules. The fibre is set parallel to the nematic director of a planar cell with variable thickness and we create pairs of Saturn ring and Saturn anti-ring using the laser tweezers. In thick cells we observe in the whole region of defect separation a Coulomb-like pair attraction with no background force, [Formula: see text] with [Formula: see text]. In cells with thickness comparable to glass fibre diameter, we observe the Coulomb-like attraction only at small separations of the defect pair. For separations larger than the fibre diameter, the pair interaction force is independent of separation. This string-like force is attributed to the formation of defect lines, connecting both monopoles and are indeed visible only on extremely confined fibre, where the fibre diameter is practically equal to the nematic layer thickness. Numerical simulations confirm the formation of defect lines connecting both rings.

Annihilation dynamics of topological monopoles on a fiber in nematic liquid crystals.

We use the laser tweezers to create isolated pairs of topological point defects in a form of radial and hyperbolic hedgehogs, located close and attracted to a thin fiber with perpendicular surface orientation of nematic liquid crystal molecules in a thin planar nematic cell. We study the time evolution of the interaction between the two monopoles by monitoring their movement and reconstructing their trajectories and velocities. We find that there is a crossover in the pair interaction force between the radial and hyperbolic hedgehog. At small separation d, the elastic force between the opposite monopoles results in an increase of the attractive force with respect to the far field, and their relative velocity v scales as a v(d)∝d^{-2±0.2} power law. At large separations, the two oppositely charged monopoles can either attract or repel with constant interaction force. We explain this strange far-field behavior by the experimental inaccuracy in setting the fiber exactly perpendicular to the cell director.

Surface charge and interactions of 20-nm nanocolloids in a nematic liquid crystal.

We studied real-time motion of individual 20-nm silica nanoparticles in a thin layer of a nematic liquid crystal using a dark-field optical videomicroscopy. By tracking the positions of individual nanoparticles we observed that particle pair interactions are not only mediated by strong thermal fluctuations of the nematic liquid crystal, but also with a repulsive force of electric origin. We determined the total electric charge of silanated silica particles in the nematic liquid crystal 5CB by observing the electric-force-driven drift. Surprisingly, the surface electric charge density depends on colloidal size and is ∼4.5×10(-3)C/m(2) for 20-nm nanocolloids, and two orders of magnitude lower, i.e., ∼2.3×10(-5)C/m(2), for 1-µm colloids. We conclude that electrostatic repulsion between like-charged particles prevents the formation of permanent colloidal assemblies of nanometer size. We also observed strong attraction of 20-nm silica nanoparticles to confining polyimide surfaces and larger clusters, which gradually results in complete expulsion of nanoparticles from the nematic liquid crystal to the surfaces of the confining cell.

Topological defect transformation and structural transition of two-dimensional colloidal crystals across the nematic to smectic-A phase transition.

We observe that topological defects in nematic colloids are strongly influenced by the elasticity and onset of smectic layering across the nematic (N) to smectic-A (SmA) phase transition. When approaching the SmA phase from above, the nematic hyperbolic hedgehog defect that accompanies a spherical colloidal inclusion is transformed into a focal conic line in the SmA phase. This phase transformation has a strong influence on the pairwise colloidal interaction and is responsible for a structural transition of two-dimensional colloidal crystals. The pretransitional behavior of the point defect is supported by Landau-de Gennes Q-tensor modeling accounting for the increasing elastic anisotropy.

Topological binding and elastic interactions of microspheres and fibres in a nematic liquid crystal.

We present a detailed analysis of topological binding and elastic interactions between a long, and micrometer-diameter fiber, and a microsphere in a homogeneously aligned nematic liquid crystal. Both objects are surface treated to produce strong perpendicular anchoring of the nematic liquid crystal. We use the opto-thermal micro-quench of the laser tweezers to produce topological defects with prescribed topological charge, such as pairs of a Saturn ring and an anti-ring, hyperbolic and radial hedgehogs on a fiber, as well as zero-charge loops. We study the entanglement and topological charge interaction between the topological defects of the fiber and sphere and we observe a huge variety of different entanglement topologies and defect-mediated elastic bindings. We explain all observed phenomena with simple topological rule: like topological charges repel each other and opposite topological charges attract. These binding mechanisms not only demonstrate the fascinating topology of nematic colloids, but also open a novel route to the assembly of very complex topological networks of fibers, spheres and other objects for applications in liquid crystal photonics.

Light-induced rewiring and winding of Saturn ring defects in photosensitive chiral nematic colloids.

We study the winding and unwinding of Saturn ring defects around silica microspheres with homeotropic surface anchoring in a cholesteric liquid crystal with a variable pitch. We use mixtures of a nematic liquid crystal 5CB and various photoresponsive chiral dopants to vary the helical pitch and sense of the helical winding by illuminating the mixtures with UV or visible light. Upon illumination, we observe motion of the Grandjean-Cano disclination lines in wedge-like cells. When the line touches the colloidal particle, we observe topological reconstruction of the Grandjean-Cano line and the Saturn ring. The result of this topological reconstruction is either an increase or decrease of the degree of winding of the Saturn ring around the colloidal particle. This phenomenon is similar to topological rewiring of -1/2 disclination lines, observed recently in chiral nematic colloids.

Consolidation trend design based on Young's modulus of clarithromycin single crystals.

The key aim of this study was to determine single mechanical properties of clarithromycin polymorphic forms in order to select some of them as more suitable for the tableting process. For this purpose, AFM single-point nanoindentation was used. The Young's moduli of clarithromycin polymorphs were substantially different, which was consistent with the structural variations in their packing motifs. The presence of the adjacent layers, which can easily slide over each other due to the low energy barrier (the lowest Young's modulus was 0.25 GPa) resulted in better bulk compressibility (the highest Heckel coefficient) of clarithromycin Form I. We also addressed the importance of tip geometry screening because the stress during the force mode often results in tip apex fracture. Even the initial manufacture of the diamond-coated tips can result in defects such as double-apex tips.

Transport of particles by a thermally induced gradient of the order parameter in nematic liquid crystals.

We demonstrate manipulation and transport of microparticles and even fluorescent molecules by the thermally induced gradient of the order parameter in the nematic liquid crystal. We use IR light absorption of the tightly focused beam of laser tweezers to heat locally a thin layer of the nematic liquid crystal by several degrees. This creates a spatial gradient of temperature of the nematic liquid crystal over separations of several tens of micrometers. We show that a dipolar colloidal particle is attracted into the hot spot of the laser tweezers. The depth of the trapping potential scales linearly with particle radius, indicating that the trapping mechanism is due to elastic self-energy of the distorted nematic liquid crystal around the particle and softening of the elasticity with increased temperature of the liquid crystal. We also demonstrate that this thermal trapping mechanism is efficient down to the nanoscale, as fluorescent molecules are also transported into hotter regions of the liquid crystal. This effect is absent in the isotropic phase, which calls into question particle transport due to the Soret effect.

Chirality screening and metastable states in chiral nematic colloids.

We show that forces between two colloidal particles in a thin layer of a chiral nematic liquid crystal strongly depend on the chirality of the liquid crystal. The observed pair potentials are attractive, but are oscillatory functions of colloidal separation. The number and the position of local energy minima increase with increasing chirality. The pair interaction is the strongest for the pitch equal to the colloidal diameter and decreases with increasing chirality. We show that the chirality of the medium is responsible for this oscillatory nature and screening of the colloidal interaction in the far and near field. The measurements are in agreement with numerical calculations using Landau-de Gennes theory.

Laser-driven microflow-induced bistable orientation of a nematic liquid crystal in perfluoropolymer-treated unrubbed cells.

We demonstrate laser-driven microflow-induced orientational change (homeotropic to planar) in a dye-doped nematic liquid crystal. The homeotropic to planar director alignment is achieved in unrubbed cells in the thermal hysteresis range of a discontinuous anchoring reorientation transition due to the local heating by light absorption in dye-doped sample. Various bistable patterns were recorded in the cell by a programmable laser tweezers. The width of the patterns depend on the scanning speed of the tightly focussed laser beam and the minimum width obtained is approximately equal to 0.57µm which is about 35 times smaller than the earlier report in the rubbed cells. We show that the motion of the microbeam spot causes local flow as a result the liquid crystal director is aligned along that direction.

Assembly and control of 3D nematic dipolar colloidal crystals.

Topology has long been considered as an abstract mathematical discipline with little connection to material science. Here we demonstrate that control over spatial and temporal positioning of topological defects allows for the design and assembly of three-dimensional nematic colloidal crystals, giving some unexpected material properties, such as giant electrostriction and collective electro-rotation. Using laser tweezers, we have assembled three-dimensional colloidal crystals made up of 4 µm microspheres in a bulk nematic liquid crystal, implementing a step-by-step protocol, dictated by the orientation of point defects. The three-dimensional colloidal crystals have tetragonal symmetry with antiparallel topological dipoles and exhibit giant electrostriction, shrinking by 25-30% at 0.37 V µm(-1). An external electric field induces a reversible and controllable electro-rotation of the crystal as a whole, with the angle of rotation being ~30° at 0.14 V µm(-1), when using liquid crystal with negative dielectric anisotropy. This demonstrates a new class of electrically highly responsive soft materials.

Viscoelasticity of ambient-temperature nematic binary mixtures of bent-core and rodlike molecules.

We report measurements of the temperature variations of physical parameters in ambient-temperature nematic liquid crystal mixtures of bent-core (BC) and rodlike molecules (5CB): birefringence Δn; static dielectric constants ε(||) and ε(⊥); splay K(11) and bend K(33) elastic constants; rotational viscosity γ(1); and diffusion coefficients D(||) and D(⊥) of a microsphere. Both Δn and ε(||) decreases rapidly with increasing BC concentration, whereas ε(⊥) remains almost constant. At a shifted temperature (e.g., T-T(NI)=-10 °C), K(11) increases by ~50% and K(33) decreases by ~80% compared to pure 5CB when the BC concentration is increased to ~43 mol % in the mixture. Viscosities parallel and perpendicular to the director, η(||), η(⊥), which are nearly equal to the Miesowicz viscosities η(2) and η(3), respectively, were obtained by D(||) and D(⊥) using the Stokes-Einstein relation. Both the viscosities at room temperature increase by 60 and 50 times, respectively, whereas γ(1) increases by 180 times (at ~43 mol %) compared to the corresponding values of pure 5CB. The stiffening of K(11) and exorbitantly large enhancement in all the viscosities at a higher mol % of BC indicate that the viscoelastic properties are highly impacted by the presence of smectic clusters of BC molecules that results from the restricted free rotation of the molecules along the bow axis in the nematic phase. A possible attachment model of smectic type clusters of BC molecules surrounding the microparticle is presented.

Colloidal entanglement in highly twisted chiral nematic colloids: twisted loops, Hopf links, and trefoil knots.

The topology and geometry of closed defect loops is studied in chiral nematic colloids with variable chirality. The colloidal particles with perpendicular surface anchoring of liquid crystalline molecules are inserted in a twisted nematic cell with the thickness that is only slightly larger than the diameter of the colloidal particle. The total twist of the chiral nematic structure in cells with parallel boundary conditions is set to 0, π, 2π, and 3π, respectively. We use the laser tweezers to discern the number and the topology of the -1/2 defect loops entangling colloidal particles. For a single colloidal particle, we observe that a single defect loop is winding around the particle, with the winding pattern being more complex in cells with higher total twist. We observe that colloidal dimers and colloidal clusters are always entangled by one or several -1/2 defect loops. For colloidal pairs in π-twisted cells, we identify at least 17 different entangled structures, some of them exhibiting linked defect loops-Hopf link. Colloidal entanglement is even richer with a higher number of colloidal particles, where we observe not only linked, but also colloidal clusters knotted into the trefoil knot. The experiments are in good agreement with numerical modeling using Landau-de Gennes theory coupled with geometrical and topological considerations using the method of tetrahedral rotation.

Direct and inverted nematic dispersions for soft matter photonics.

General properties and recent developments in the field of nematic colloids and emulsions are discussed. The origin and nature of pair colloidal interactions in the nematic colloids are explained and an overview of the stable colloidal 2D crystalline structures and superstructures discovered so far is given. The nature and role of topological defects in the nematic colloids is discussed, with an emphasis on recently discovered entangled colloidal structures. Applications of inverted nematic emulsions and binding force mechanisms in nematic colloids for soft matter photonic devices are discussed.

Square colloidal lattices and pair interaction in a binary system of quadrupolar nematic colloids.

Spherical colloidal particles with normal and tangential surface director alignment in a nematic liquid crystal induce elastic quadrupoles of opposite signs that attract one another along and perpendicular to the director. We utilize this unique angular profile of the mixed quadrupolar interaction to build 2D crystals with square lattices by laser tweezers.

Light-driven oscillations of entangled nematic colloidal chains.

Laser tweezers have been used to drive the oscillations of a chain of entangled colloidal particles in the nematic liquid crystal 5CB. The amplitude and phase of light-driven oscillations have been determined for the motion of individual colloidal particles. The collective motion of 4.8µm silica particles is highly damped for a driving frequency above 0.5Hz. The results were compared to an effective bead-spring model, where the motion of elastically coupled particles is hindered by viscous damping and hydrodynamic coupling. Qualitative agreement between theory and experiment was obtained.

Design of 2D binary colloidal crystals in a nematic liquid crystal.

In this paper, we examine directed self-assembly in a 2D binary system of dipolar and quadrupolar colloidal particles with normal surface boundary conditions, dispersed in the nematic liquid crystal. Using the laser tweezers, we assembled a large variety of stable 2D colloidal crystal structures. In all analyzed structures, the particles, their surface treatment and the cell conditions were the same, which gives us the ability to systematically follow the evolution of colloidal assembly when many particles are present. We present an analogy between molecular self-assembly and organization of colloidal microspheres in liquid crystalline medium to extend the strategy for designing colloidal crystalline structures of different level of complexity.

Hierarchical self-assembly of nematic colloidal superstructures.

We show that colloidal superstructures could be assembled in mixtures of large and small colloidal particles dispersed in a nematic liquid crystal. Using elastic interaction of small colloidal particles with the disclination lines we succeed to demonstrate how one can decorate with small particles a topological matrix of defect rings and loops formed by an array of large colloidal particles. Our simulations show that this concept of colloidal self-assembly in nematics could be extended down to the nanoscale particles.

Interactions of quadrupolar nematic colloids.

We present experimental and theoretical study of colloidal interactions in quadrupolar nematic liquid crystal colloids, confined to a thin planar nematic cell. Using the laser tweezers, the particles have been positioned in the vicinity of other colloidal particles and their interactions have been determined using particle tracking video microscopy. Several types of interactions have been analyzed: (i) quadrupolar pair interaction, (ii) the interaction of an isolated quadrupole with a quadrupolar chain, and (iii) the interaction of an isolated quadrupolar colloidal particle with a two-dimensional (2D) quadrupolar crystallite. In all cases, the interactions are of the order of several 100k(B)T for 2 microm particles, which gives rise to relatively stable 2D colloidal crystals. The experimental results are compared to the predictions of Landau-de Gennes theory and we find a relatively good qualitative agreement.