David Seč

Geometrical frustration of chiral ordering in cholesteric droplets

Frustration of chiral ordering is explored in cholesteric liquid crystal droplets with planar degenerate anchoring using numerical modeling. Droplets of variable pitches are studied, demonstrating the role of a gradually increasing cholesteric pitch and the corresponding equilibrium structures. All previously known structures are identified but with notable differences. The structures presented with director fields are complemented with a detailed description of the defect regions. The characteristic half-diameter +2 disclination from previous studies is found to be in fact a double-helix of two λ+1 disclination lines, whereas the full-diameter +1 disclination is composed of an alternating series of τ−1/2 and λ+1/2 disclination rings. Finally, two new meta-stable cholesteric structures -Lyre and Yeti- are found, which are characterised by complex compositions of cholesteric disclinations.

Topological zoo of free-standing knots in confined chiral nematic fluids

Knotted fields are an emerging research topic relevant to different areas of physics where topology plays a crucial role. Recent realization of knotted nematic disclinations stabilized by colloidal particles raised a challenge of free-standing knots. Here we demonstrate the creation of free-standing knotted and linked disclination loops in the cholesteric ordering fields, which are confined to spherical droplets with homeotropic surface anchoring. Our approach, using free energy minimization and topological theory, leads to the stabilization of knots via the interplay of the geometric frustration and intrinsic chirality. Selected configurations of the lowest complexity are characterized by knot or link types, disclination lengths and self-linking numbers. When cholesteric pitch becomes short on the confinement scale, the knotted structures change to practically unperturbed cholesteric structures with disclinations expelled close to the surface. The drops with knots could be controlled by optical beams and may be used for photonic elements.

Microparticles confined to a nematic liquid crystal shell

A seminal paper [D. R. Nelson, Nano Lett., 2002, 2, 1125.] has proposed that a nematic coating could be used to create a valency for spherical colloidal particles through the functionalization of nematic topological defects. Experimental realizations however question the complex behaviour of solid particles and defects embedded in such a nematic spherical shell. In order to address the related topological and geometrical issues, we have studied micrometer-sized silica beads trapped in nematic shells. We underline the mechanisms that strongly modify the texture of the simple (particle-free) shells when colloidal particles are embedded. Finally, we show how the coupling between capillarity and nematic elasticity offers new ways to control the valence and directionality of shells.

Sensing surface morphology of biofibers by decorating spider silk and cellulosic filaments with nematic microdroplets

Significance Biological microfibers are remarkable materials with diverse structural and mechanical properties, such as high wear-resistance, elasticity, and biodegradability. However, with current techniques, there are few robust ways to sense the surface properties of the fibers, which crucially affect the organization of the fibers and their interactions with the surrounding material. In this paper, we show that surfaces of diverse biofibers, including spider silks and cellulosic fibers, can be easily sensed by depositing droplets of a nematic fluid onto the fibers. The droplets reveal the surface properties of the fibers via their optical images, notably showing also the fiber chirality. Further, the droplets are used to study the entanglement of biofibers, as a route toward novel biological and bioinspired materials. Probing the surface morphology of microthin fibers such as naturally occurring biofibers is essential for understanding their structural properties, biological function, and mechanical performance. The state-of-the-art methods for studying the surfaces of biofibers are atomic force microscopy imaging and scanning electron microscopy, which well characterize surface geometry of the fibers but provide little information on the local interaction potential of the fibers with the surrounding material. In contrast, complex nematic fluids respond very well to external fields and change their optical properties upon such stimuli. Here we demonstrate that liquid crystal droplets deposited on microthin biofibers—including spider silk and cellulosic fibers—reveal characteristics of the fibers’ surface, performing as simple but sensitive surface sensors. By combining experiments and numerical modeling, different types of fibers are identified through the fiber-to-nematic droplet interactions, including perpendicular and axial or helicoidal planar molecular alignment. Spider silks align nematic molecules parallel to fibers or perpendicular to them, whereas cellulose aligns the molecules unidirectionally or helicoidally along the fibers, indicating notably different surface interactions. The nematic droplets as sensors thus directly reveal chirality of cellulosic fibers. Different fiber entanglements can be identified by depositing droplets exactly at the fiber crossings. More generally, the presented method can be used as a simple but powerful approach for probing the surface properties of small-size bioobjects, opening a route to their precise characterization.

Liquid crystal necklaces: cholesteric drops threaded by thin cellulose fibres

Liquid crystals in confined geometries exhibit numerous complex structures often including topological defects that are controlled by the nematic elasticity, chirality and surface anchoring. In this work, we study the structures of cholesteric droplets pierced by cellulose fibres with planar anchoring at droplet and fibre surfaces. By varying the temperature we demonstrate the role of twisting power and droplet diameter on the equilibrium structures. The observed structures are complemented by detailed numerical simulations of possible director fields decorated by defects. Three distinct structures, a bipolar and two ring configurations, are identified experimentally and numerically. Designing cholesteric liquid crystal microdroplets on thin long threads opens new routes to produce fibre waveguides decorated with complex microresonators.

Waltzing route toward double-helix formation in cholesteric shells

Significance Droplets of chiral liquid crystals, or cholesterics, typically exhibit an intriguing radial defect which results from frustrations in the molecular order. This configuration shows a fascinating analogy to the Dirac monopole, a hypothetical magnetic charge, and plays a crucial role in the droplet optical properties, recently exploited to produce microlasers. Despite its evident interest, the nature of this disclination remains uncertain. We experimentally show, by studying spherical cholesteric shells, that it is composed of two line defects that wrap around each other on a double-helix structure. By tuning the system chirality, we can make this configuration dissociate into two independent stacks of disclination rings. The transition between configurations is reversible and entails an unexpected defect waltz dynamics. Liquid crystals, when confined to a spherical shell, offer fascinating possibilities for producing artificial mesoscopic atoms, which could then self-assemble into materials structured at a nanoscale, such as photonic crystals or metamaterials. The spherical curvature of the shell imposes topological constraints in the molecular ordering of the liquid crystal, resulting in the formation of defects. Controlling the number of defects, that is, the shell valency, and their positions, is a key success factor for the realization of those materials. Liquid crystals with helical cholesteric order offer a promising, yet unexplored way of controlling the shell defect configuration. In this paper, we study cholesteric shells with monovalent and bivalent defect configurations. By bringing together experiments and numerical simulations, we show that the defects appearing in these two configurations have a complex inner structure, as recently reported for simulated droplets. Bivalent shells possess two highly structured defects, which are composed of a number of smaller defect rings that pile up through the shell. Monovalent shells have a single radial defect, which is composed of two nonsingular defect lines that wind around each other in a double-helix structure. The stability of the bivalent configuration against the monovalent one is controlled by c = h/p, where h is the shell thickness and p the cholesteric helical pitch. By playing with the shell geometry, we can trigger the transition between the two configurations. This transition involves a fascinating waltz dynamics, where the two defects come closer while turning around each other.

Sensing and tuning microfiber chirality with nematic chirogyral effect

Microfibers with their elongated shape and translation symmetry can act as important components in various soft materials, notably for their mechanics on the microscopic level. Here we demonstrate the mechanical response of a micro-object to imposed chirality, in this case, the tilt of disclination rings in an achiral nematic medium caused by the chiral surface anchoring on an immersed microfiber. This coupling between chirality and mechanical response, used to demonstrate sensing of chirality of electrospun cellulose microfibers, is revealed in the optical micrographs due to anisotropy in the elastic response of the host medium. We provide an analytical explanation of the chirogyral effect supported with numerical simulations and perform an experiment to test the effect of the cell confinement and fiber size. We controllably twist the microfibers and demonstrate the response of the nematic medium. More generally the demonstrated study provides means for experimental discrimination of surface properties and allows mechanical control over the shape of disclination rings.

Light-driven oscillations of entangled nematic colloidal chains

Abstract.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.