JungHyun Noh

Macroscopic Control of Helix Orientation in Films Dried from Cholesteric Liquid-Crystalline Cellulose Nanocrystal Suspensions

The intrinsic ability of cellulose nanocrystals (CNCs) to self-organize into films and bulk materials with helical order in a cholesteric liquid crystal is scientifically intriguing and potentially important for the production of renewable multifunctional materials with attractive optical properties. A major obstacle, however, has been the lack of control of helix direction, which results in a defect-rich, mosaic-like domain structure. Herein, a method for guiding the helix during film formation is introduced, which yields dramatically improved uniformity, as confirmed by using polarizing optical and scanning electron microscopy. By raising the CNC concentration in the initial suspension to the fully liquid crystalline range, a vertical helix orientation is promoted, as directed by the macroscopic phase boundaries. Further control of the helix orientation is achieved by subjecting the suspension to a circular shear flow during drying.

Tuneable multicoloured patterns from photonic cross-communication between cholesteric liquid crystal droplets

Monodisperse droplets of planar-aligned cholesteric (N*) liquid crystal exhibit an intriguing capacity for photonic cross-communication, giving rise to colourful patterns that depend sensitively on the N* pitch, droplet positions and illuminated area. The phenomenon results from a combination of omnidirectional selective reflection of N* droplets—which thus act as spherically symmetric self-assembled photonic crystals—and total internal reflection at the continuous phase surface. We outline how the unique optical properties can be employed in numerous applications.

Liquid crystals in micron-scale droplets, shells and fibers

The extraordinary responsiveness and large diversity of self-assembled structures of liquid crystals are well documented and they have been extensively used in devices like displays. For long, this application route strongly influenced academic research, which frequently focused on the performance of liquid crystals in display-like geometries, typically between flat, rigid substrates of glass or similar solids. Today a new trend is clearly visible, where liquid crystals confined within curved, often soft and flexible, interfaces are in focus. Innovation in microfluidic technology has opened for high-throughput production of liquid crystal droplets or shells with exquisite monodispersity, and modern characterization methods allow detailed analysis of complex director arrangements. The introduction of electrospinning in liquid crystal research has enabled encapsulation in optically transparent polymeric cylinders with very small radius, allowing studies of confinement effects that were not easily accessible before. It also opened the prospect of functionalizing textile fibers with liquid crystals in the core, triggering activities that target wearable devices with true textile form factor for seamless integration in clothing. Together, these developments have brought issues center stage that might previously have been considered esoteric, like the interaction of topological defects on spherical surfaces, saddle-splay curvature-induced spontaneous chiral symmetry breaking, or the non-trivial shape changes of curved liquid crystal elastomers with non-uniform director fields that undergo a phase transition to an isotropic state. The new research thrusts are motivated equally by the intriguing soft matter physics showcased by liquid crystals in these unconventional geometries, and by the many novel application opportunities that arise when we can reproducibly manufacture these systems on a commercial scale. This review attempts to summarize the current understanding of liquid crystals in spherical and cylindrical geometry, the state of the art of producing such samples, as well as the perspectives for innovative applications that have been put forward.

Tuning the defect configurations in nematic and smectic liquid crystalline shells

Thin liquid crystalline shells surrounding and surrounded by aqueous phases can be conveniently produced using a nested capillary microfluidic system, as was first demonstrated by Fernandez-Nieves et al. in 2007. By choosing particular combinations of stabilizers in the internal and external phases, different types of alignment, uniform or hybrid, can be ensured within the shell. Here, we investigate shells in the nematic and smectic phases under varying boundary conditions, focusing in particular on textural transformations during phase transitions, on the interaction between topological defects in the director field and inclusions in the liquid crystal (LC), and on the possibility to relocate defects within the shell by rotating the shell in the gravitational field. We demonstrate that inclusions in a shell can seed defects that cannot form in a pristine shell, adding a further means of tuning the defect configuration, and that shells in which the internal aqueous phase is not density matched with the LC will gently rearrange the internal structure upon a rotation that changes the influence of gravity. Because the defects can act as anchor points for added linker molecules, allowing self-assembly of adjacent shells, the various arrangements of defects developing in these shells and the possibility of tuning the result by modifying boundary conditions, LC phase, thickness and diameter of the shell or applying external forces make this new LC configuration very attractive.

Taming Liquid Crystal Self‐Assembly: The Multifaceted Response of Nematic and Smectic Shells to Polymerization

By photopolymerizing liquid crystal shells, their rich variety of self-assembled structures can be rendered permanent and the lifetime extended from days to months, without removing the characteristic responsiveness. If polymerization is carried out close to either boundary of the nematic phase, the process triggers the transition into the adjacent phase, to higher or to lower degree of order.

Transmission polarized optical microscopy of short-pitch cholesteric liquid crystal shells

We recently demonstrated that colloidal crystal arrangements of monodisperse droplets or shells of planar-aligned cholesteric liquid crystal exhibit intricate patterns of circularly polarized reflection spots of different colors. The spots appear as a result of photonic cross communication between droplets, hence the patterns reflect the macroscopic arrangement of droplets or shells. Apart from being an interesting optical phenomenon, it offers attractive application opportunities in photonics and beyond, due to the unique characteristics of the patterns. It turns out that the optical quality of shells is much enhanced compared to that of droplets, hence we focus our attention primarily on shells, of varying thickness. Here we analyze and explain the intriguing textures arising when studying planar-aligned short-pitch cholesteric shells in transmission polarizing optical microscopy. In this case, the texture reflects the properties of each individual shell, without any sign of cross communication, yet also this pattern holds some fascinating mysteries. These can only be elucidated by considering all the peculiar optical properties of cholesterics together, as well as the unusual situation given by the spherical shell geometry.

Dynamic and complex optical patterns from colloids of cholesteric liquid crystal droplets

Drops or shells of a planar-aligned short-pitch cholesteric liquid crystal exhibit unique optical properties due to the combination of Bragg reflection in the cholesteric helix and a radial orientation of the helix axis. If such a droplet is illuminated from above, light is reflected into a continuous set of cones, the opening angles of which depend on where on the droplet the light hits its surface. For the wavelength that fulfills the Bragg condition the reflection is dramatically enhanced, yielding the light cones colored. A photonic cross communication scheme arises for certain angles, reflecting light back to the observer from a different droplet than the one originally illuminated. This gives rise to an intricate pattern of colored and circularly polarized spots. A number of interesting applications may be developed based on this pattern, e.g. in identification and authentication devices. We have carried out a detailed spectrophotometric analysis of the patterns, localized to individual spot maxima. A quantitative comparison between the measured spectra and the reflection wavelength expected from a model for the pattern generation allows us to conclude that the droplets are in fact not spherical but slightly ellipsoidal.

Elucidating the fine details of cholesteric liquid crystal shell reflection patterns

ABSTRACT Clusters of planar-aligned short-pitch cholesteric liquid crystal spheres generate dynamic colourful patterns due to multiple selective reflections from the radially oriented cholesteric helices in neighbour shells at varying distances. These photonic communication patterns were widely investigated for the cases of both droplets and shells, demonstrating not only intriguing optical phenomena but also potential for applications as new optical elements for photonics, sensing or security pattern generation. However, the optics of these clusters is truly complex and until now only the strongest and most fundamental reflections have been analysed and explained. In this report, we elucidate the origin of a number of more subtle reflections and we explain the extension in space of various spots as well as their internal colour variations. GRAPHICAL ABSTRACT