Piecewise Phototuning of Self‐Organized Helical Superstructures

Cholesteric liquid crystals (CLCs) exhibit selective reflection that can be tuned owing to the dynamic control of inherent self‐organized helical superstructures. Although phototunable reflection is reported, these systems hitherto suffer from a limitation in that the tuning range is restricted to one narrow period and the optically addressed images have to sacrifice one color in the visible spectrum to serve as the background, resulting from the insufficient variation in helical twisting power of existing photoresponsive chiral switches that are all bistable. Here, delicate patterns of three primary red, green, and blue (RGB) colors with a black background are presented, which is realized based on piecewise reflection tuning of the CLC induced by a newly designed photoresponsive tristable chiral switch. Three stable configurations of the chiral switch endow the CLC with two continuous and adjacent tuning periods of the reflection, covering not only entire visible spectrum, but also one more wide period within near‐infrared region. Therefore, the concept of piecewise tuning in CLC system demonstrates a new strategy for phototunable RGB and black reflective display.     

Digitalizing Self‐Assembled Chiral Superstructures for Optical Vortex Processing

Cholesteric liquid crystal (CLC) chiral superstructures exhibit unique features; that is, polychromatic and spin‐determined phase modulation. Here, a concept for digitalized chiral superstructures is proposed, which further enables the arbitrary manipulation of reflective geometric phase and may significantly upgrade existing optical apparatus. By encoding a specifically designed binary pattern, an innovative CLC optical vortex (OV) processor is demonstrated. Up to 25 different OVs are extracted with equal efficiency over a wavelength range of 116 nm. The multiplexed OVs can be detected simultaneously without mode crosstalk or distortion, permitting a polychromatic, large‐capacity, and in situ method for parallel OV processing. Such complex but easily fabricated self‐assembled chiral superstructures exhibit versatile functionalities, and provide a satisfactory platform for OV manipulation and other cutting‐edge territories. This work is a vital step towards extending the fundamental understanding and fantastic applications of ordered soft matter.     

Dynamic Control of Light Direction Enabled by Stimuli‐Responsive Liquid Crystal Gratings

The ability to control light direction with tailored precision via facile means is long‐desired in science and industry. With the advances in optics, a periodic structure called diffraction grating gains prominence and renders a more flexible control over light propagation when compared to prisms. Today, diffraction gratings are common components in wavelength division multiplexing devices, monochromators, lasers, spectrometers, media storage, beam steering, and many other applications. Next‐generation optical devices, however, demand nonmechanical, full and remote control, besides generating higher than 1D diffraction patterns with as few optical elements as possible. Liquid crystals (LCs) are great candidates for light control since they can form various patterns under different stimuli, including periodic structures capable of behaving as diffraction gratings. The characteristics of such gratings depend on several physical properties of the LCs such as film thickness, periodicity, and molecular orientation, all resulting from the internal constraints of the sample, and all of these are easily controllable. In this review, the authors summarize the research and development on stimuli‐controllable diffraction gratings and beam steering using LCs as the active optical materials. Dynamic gratings fabricated by applying external field forces or surface treatments and made of chiral and nonchiral LCs with and without polymer networks are described. LC gratings capable of switching under external stimuli such as light, electric and magnetic fields, heat, and chemical composition are discussed. The focus is on the materials, designs, applications, and future prospects of diffraction gratings using LC materials as active layers.     

Light‐Patterned Crystallographic Direction of a Self‐Organized 3D Soft Photonic Crystal

Uniform and patterned orientation of a crystallographic direction of ordered materials is of fundamental significance and of great interest for electronic and photonic applications. However, such orientation control is generally complicated and challenging with regard to inorganic and organic crystalline materials due to the occurrence of uncontrollable dislocations or defects. Achieving uniform lattice orientation in frustrated liquid‐crystalline phases, like cubic blue phases, is a formidable task. Taming and tailoring the ordering of such soft, cubic lattices along predetermined or desired directions, and even imparting a prescribed pattern on lattice orientation, are more challenging, due to the entropy‐domination attribute of soft matter. Herein, we disclose a facile way to realize designed micropatterning of a crystallographic direction of a soft, cubic liquid‐crystal superstructure, exhibiting an alternate uniform and random orientation of the lattice crystallographic direction enabled by a photoalignment technique. Because of the rewritable trait of the photoalignment film, the pattern can be erased and rewritten on‐demand by light. Such an oriented soft lattice sensitively responds to various external stimuli such as temperature, electric field, and light irradiation. Furthermore, advanced reflective photonic applications are achieved based on the patterned crystallographic orientation of the cubic blue phase, soft lattice.     

Light‐Driven Reversible Transformation between Self‐Organized Simple Cubic Lattice and Helical Superstructure Enabled by a Molecular Switch Functionalized Nanocage

Self‐organized stimuli‐responsive smart materials with adjustable attributes are highly desirable for a plethora of device applications. Simple cubic lattice is quite uncommon in soft condensed matter due to its lower packing factor. Achieving a stable simple cubic soft lattice and endowing such a lattice with dynamic reconstruction capability solely by a facile light irradiation are of paramount significance for both fundamental studies and engineering explorations. Herein, an elegant stable self‐organized simple cubic soft lattice, i.e., blue phase II, in a chiral liquid crystal (LC) system is disclosed, which is stable down to room temperature and exhibits both reversible lattice deformation and transformation to a helical superstructure, i.e., cholesteric LC, by light stimulation. Such an amazing trait is attained by doping a judiciously designed achiral photoresponsive molecular switch functionalized polyhedral oligomeric silsesquioxane nanocage into a chiral LC host. An unprecedented reversible collapse and reconstruction of such a high symmetric simple cubic blue phase II driven by light has been achieved. Furthermore, a well‐defined conglomerate micropattern composed of simple cubic soft lattice and helical superstructure, which is challenging to fabricate in organic and inorganic crystalline materials, is produced using photomasking technology. Moreover, the promising photonic application based on such a micropattern is demonstrated.     

Visible‐Light‐Induced Self‐Organized Helical Superstructure in Orientationally Ordered Fluids

Light‐induced phenomena occurring in nature and in synthetic materials are fascinating and have been exploited for technological applications. Here visible‐light‐induced formation of a helical superstructure is reported, i.e., a cholesteric liquid crystal phase, in orientationally ordered fluids, i.e., nematic liquid crystals, enabled by a visible‐light‐driven chiral molecular switch. The cyclic‐azobenzene‐based chiral molecular switch exhibits reversible photoisomerization in response to visible light of different wavelengths due to the band separation of n–π* transitions of its trans‐ and cis‐isomers. Green light (530 nm) drives the trans‐to‐cis photoisomerization whereas the cis‐to‐trans isomerization process of the chiral molecular switch can be caused by blue light (440 nm). It is observed that the helical twisting power of this chiral molecular switch increases upon irradiation with green light, which enables reversible induction of helical superstructure in nematic liquid crystals containing a very small quantity of the molecular switch. The occurrence of the light‐induced helical superstructure enables the formation of diffraction gratings in cholesteric films.     

Dynamic Orthogonal Switching of a Thermoresponsive Self‐Organized Helical Superstructure

Controllable manipulation of self‐organized dynamic superstructures of functional molecular materials by external stimuli is an enabling enterprise. Herein, we have developed a thermally driven, self‐organized helical superstructure, i.e., thermoresponsive cholesteric liquid crystal (CLC), by integrating a judiciously chosen thermoresponsive chiral molecular switch into an achiral liquid crystalline medium. The CLC in lying state, in both planar and twisted nematic cells, exhibits reversible in‐plane orthogonal switching of its helical axis in response to the combined effect of temperature and electric field. Consequently, the direction of the cholesteric grating has been observed to undergo 90° switching in a single cell, enabling non‐mechanical beam steering along two orthogonal directions. The ability to reversibly switch the cholesteric gartings along perpendicular directions by appropriately adjusting temperature and electric field strength could facilitate their applications in 2D beam steering, spectrum scanning, optoelectronics and beyond.     

Stimuli‐Directed Colorimetric Interconversion of Helical Polymers Accompanied by a Tunable Self‐Assembly Process

Interconversion between extended and bent structures at the pendant groups of a chiral polyene framework [poly(phenylacetylene) with (R)‐(2‐methoxy‐2‐phenylacetyl)glycine residues linked to 4‐vinylanilines] allows the reversible colorimetric transformation from stretched to compressed helical cis‐transoid polyenic structures through manipulation of the flexible spacer. This transformation generates either organogels (stretched helical form) or nanoparticles (compressed helical form) under the control of polar/low polar stimuli respectively and opens the way to the development of new sensors and stimuli‐sensitive materials based on these concepts.     

Light‐Driven Chiral Molecular Switches or Motors in Liquid Crystals

The ability to tune molecular self‐organization with an external stimulus is a main driving force in the bottom‐up nanofabrication of molecular devices. Light‐driven chiral molecular switches or motors in liquid crystals that are capable of self‐organizing into optically tunable helical superstructures undoubtedly represent a striking example, owing to their unique property of selective light reflection and which may lead to applications in the future. In this review, we focus on different classes of light‐driven chiral molecular switches or motors in liquid crystal media for the induction and manipulation of photoresponsive cholesteric liquid crystal systems and their consequent applications. Moreover, the change of helical twisting powers of chiral dopants and their capability of helix inversion in the induced cholesteric phases are highlighted and discussed in the light of their molecular geometric changes.     

Visualization and Quantitative Detection of Friction Force by Self‐Organized Organic Layered Composites

Visualization and quantitative detection of external stimuli are significant challenges in materials science. Quantitative detection of friction force, a mechanical stress, is not easily achieved using conventional stimuli‐responsive materials. Here, the quantitative detection of friction force is reported, such as the strength and accumulated ammount, from the visible color of organic layered composites consisting of polydiacetylene (PDA) and organic amines without an excitation light source. The composites of the layered diacetylene monomer crystal and interlayer organic amine are synthesized through self‐organization from the precursor solution. After topochemical polymerization, the layered composites based on PDA show tunable temperature‐responsive and mechanoresponsive color‐change properties depending on the types of interlayer amines. The layered composites are homogeneously coated on a filter paper. The change in color of the paper is quantitatively used to visualize the strength and accumulated amount of the applied friction force. Furthermore, writing pressure is measured by friction force using the paper device.