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    Three-dimensional control of the helical axis of a chiral nematic liquid crystal by light. Zheng Zhi-gang,Li Yannian,Bisoyi Hari Krishna,Wang Ling,Bunning Timothy J,Li Quan Nature Chiral nematic liquid crystals--otherwise referred to as cholesteric liquid crystals (CLCs)--are self-organized helical superstructures that find practical application in, for example, thermography, reflective displays, tuneable colour filters and mirrorless lasing. Dynamic, remote and three-dimensional control over the helical axis of CLCs is desirable, but challenging. For example, the orientation of the helical axis relative to the substrate can be changed from perpendicular to parallel by applying an alternating-current electric field, by changing the anchoring conditions of the substrate, or by altering the topography of the substrate's surface; separately, in-plane rotation of the helical axis parallel to the substrate can be driven by a direct-current field. Here we report three-dimensional manipulation of the helical axis of a CLC, together with inversion of its handedness, achieved solely with a light stimulus. We use this technique to carry out light-activated, wide-area, reversible two-dimensional beam steering--previously accomplished using complex integrated systems and optical phased arrays. During the three-dimensional manipulation by light, the helical axis undergoes, in sequence, a reversible transition from perpendicular to parallel, followed by in-plane rotation on the substrate surface. Such reversible manipulation depends on experimental parameters such as cell thickness, surface anchoring condition, and pitch length. Because there is no thermal relaxation, the system can be driven either forwards or backwards from any light-activated intermediate state. We also describe reversible photocontrol between a two-dimensional diffraction state, a one-dimensional diffraction state and a diffraction 'off' state in a bilayer cell. 10.1038/nature17141
    Self-Regulation of Infrared Using a Liquid Crystal Mixture Doped with Push-Pull Azobenzene for Energy-Saving Smart Windows. Oh Seung-Won,Nam Seung-Min,Kim Sang-Hyeok,Yoon Tae-Hoon,Kim Wook Sung ACS applied materials & interfaces A self-regulating liquid crystal (LC) smart window whose reflectance changes with ambient conditions is demonstrated. Thermally or optically induced switching between the transparent state and a near-infrared (NIR) reflective state can be used for energy-saving windows. Reflection of NIR can reduce the energy used for cooling, while remaining transparent to visible light. By changing the initial alignment of LCs, the window can be switched between hazy-opaque and IR-reflective states to be used for privacy windows. 10.1021/acsami.0c19015
    Optically Rewritable Transparent Liquid Crystal Displays Enabled by Light-Driven Chiral Fluorescent Molecular Switches. Li Juntao,Bisoyi Hari Krishna,Tian Jiajun,Guo Jinbao,Li Quan Advanced materials (Deerfield Beach, Fla.) Functional soft materials exhibiting distinct functionalities in response to a specific stimulus are highly desirable towards the fabrication of advanced devices with superior dynamic performances. Herein, two novel light-driven chiral fluorescent molecular switches have been designed and synthesized that are able to exhibit unprecedented reversible Z/E photoisomerization behavior along with tunable fluorescence intensity in both isotropic and anisotropic media. Cholesteric liquid crystals fabricated using these new fluorescent molecular switches as chiral dopants exhibit reversible reflection color tuning spanning the visible and infrared region of the spectrum. Transparent display devices have been fabricated using both low chirality and high chirality cholesteric films that operate either exclusively in fluorescent mode or in both fluorescent and reflection mode, respectively. The dual mode display device employing short pitch cholesteric film is able to function on demand under all ambient light conditions including daylight and darkness with fast response and high resolution. Moreover, the proof-of-concept for a "remote-writing board" using cholesteric films containing one of the light-driven chiral fluorescent molecular switches with ease of fabrication and operation is disclosed herein. Such optically rewritable transparent display devices enabled by light-driven chiral fluorescent molecular switches pave a new way for developing novel display technology under different lighting conditions. 10.1002/adma.201807751
    Mechanochromic, Shape-Programmable and Self-Healable Cholesteric Liquid Crystal Elastomers Enabled by Dynamic Covalent Boronic Ester Bonds. Ma Jiazhe,Yang Yanzhao,Valenzuela Cristian,Zhang Xuan,Wang Ling,Feng Wei Angewandte Chemie (International ed. in English) Endowing a cholesteric liquid crystal elastomer (CLCE) exhibiting a helicoidal nanostructure with dynamically tailorable functionalities is of paramount significance for its emerging applications in diverse fields such as adaptive optics and soft robotics. Here, a mechanochromic, shape-programmable and self-healable CLCE is judiciously designed and synthesized through integrating dynamic covalent boronic ester bonds into the main-chain CLCE polymer network. The circularly polarized reflection of CLCEs can be reversibly and dynamically tuned across the entire visible spectrum by mechanical stretching. Thanks to the introduction of dynamic boronic ester bonds, the CLCEs were found to show robust reprogrammable and self-healing capabilities. The research disclosed herein can provide new insights into the development of 4D (color and 3D shape) programmable photonic actuators towards bioinspired camouflage, adaptive optical systems, and next-generation intelligent machines. 10.1002/anie.202116219
    Cellulose Nanocrystal Aqueous Colloidal Suspensions: Evidence of Density Inversion at the Isotropic-Liquid Crystal Phase Transition. Advanced materials (Deerfield Beach, Fla.) The colloidal suspensions of aqueous cellulose nanocrystals (CNCs) are known to form liquid crystalline (LC) systems above certain critical concentrations. From an isotropic phase, tactoid formation, growth, and sedimentation have been determined as the genesis of a high-density cholesteric phase, which, after drying, originates solid iridescent films. Herein, the coexistence of a liquid crystal upper phase and an isotropic bottom phase in CNC aqueous suspensions at the isotropic-nematic phase separation is reported. Furthermore, isotropic spindle-like domains are observed in the low-density LC phase and high-density LC phases are also prepared. The CNCs isolated from the low- and high-density LC phases are found to have similar average lengths, diameters, and surface charges. The existence of an LC low-density phase is explained by the presence of air dissolved in the water present within the CNCs. The air dissolves out when the water solidifies into ice and remains within the CNCs. The self-adjustment of the cellulose chain conformation enables the entrapment of air within the CNCs and CNC buoyancy in aqueous suspensions. 10.1002/adma.202108227
    Photonic Multishells Composed of Cholesteric Liquid Crystals Designed by Controlled Phase Separation in Emulsion Drops. Park Sihun,Lee Sang Seok,Kim Shin-Hyun Advanced materials (Deerfield Beach, Fla.) Cholesteric liquid crystals (CLCs), also known as chiral nematic LCs, show a photonic stopband, which is promising for various optical applications. In particular, CLCs confined in microcompartments are useful for sensing, lasing, and optical barcoding at the microscale. The integration of distinct CLCs into single microstructures can provide advanced functionality. In this work, CLC multishells with multiple stopbands are created by liquid-liquid phase separation (LLPS) in a simple yet highly controlled manner. A homogeneous ternary mixture of LC, hydrophilic liquid, and co-solvent is microfluidically emulsified to form uniform oil-in-water drops, which undergo LLPS to form onion-like drops composed of alternating CLC-rich and CLC-depleted layers. The multiplicity is controlled from one to five by adjusting the initial composition of the ternary mixture, which dictates the number of consecutive steps of LLPS. Interestingly, the concentration of the chiral dopant becomes reduced from the outermost to the innermost CLC drop due to uneven partitioning during LLPS, which results in multiple stopbands. Therefore, the photonic multishells show multiple structural colors. In addition, dye-doped multishells provide band-edge lasing at two different wavelengths. This new class of photonic multishells will provide new opportunities for advanced optical applications. 10.1002/adma.202002166
    Liquid Crystals: Versatile Self-Organized Smart Soft Materials. Bisoyi Hari Krishna,Li Quan Chemical reviews Smart soft materials are envisioned to be the building blocks of the next generation of advanced devices and digitally augmented technologies. In this context, liquid crystals (LCs) owing to their responsive and adaptive attributes could serve as promising smart soft materials. LCs played a critical role in revolutionizing the information display industry in the 20th century. However, in the turn of the 21st century, numerous beyond-display applications of LCs have been demonstrated, which elegantly exploit their controllable stimuli-responsive and adaptive characteristics. For these applications, new LC materials have been rationally designed and developed. In this Review, we present the recent developments in light driven chiral LCs, i.e., cholesteric and blue phases, LC based smart windows that control the entrance of heat and light from outdoor to the interior of buildings and built environments depending on the weather conditions, LC elastomers for bioinspired, biological, and actuator applications, LC based biosensors for detection of proteins, nucleic acids, and viruses, LC based porous membranes for the separation of ions, molecules, and microbes, living LCs, and LCs under macro- and nanoscopic confinement. The Review concludes with a summary and perspectives on the challenges and opportunities for LCs as smart soft materials. This Review is anticipated to stimulate eclectic ideas toward the implementation of the nature's delicate phase of matter in future generations of smart and augmented devices and beyond. 10.1021/acs.chemrev.1c00761
    Cholesteric liquid crystals with a broad light reflection band. Mitov Michel Advanced materials (Deerfield Beach, Fla.) The cholesteric-liquid-crystalline structure, which concerns the organization of chromatin, collagen, chitin, or cellulose, is omnipresent in living matter. In technology, it is found in temperature and pressure sensors, supertwisted nematic liquid crystal displays, optical filters, reflective devices, or cosmetics. A cholesteric liquid crystal reflects light because of its helical structure. The reflection is selective - the bandwidth is limited to a few tens of nanometers and the reflectance is equal to at most 50% for unpolarized incident light, which is a consequence of the polarization-selectivity rule. These limits must be exceeded for innovative applications like polarizer-free reflective displays, broadband polarizers, optical data storage media, polarization-independent devices, stealth technologies, or smart switchable reflective windows to control solar light and heat. Novel cholesteric-liquid-crystalline architectures with the related fabrication procedures must therefore be developed. This article reviews solutions found in living matter and laboratories to broaden the bandwidth around a central reflection wavelength, do without the polarization-selectivity rule and go beyond the reflectance limit. 10.1002/adma.201202913
    Thermochromic Cholesteric Liquid Crystal Microcapsules with Cellulose Nanocrystals and a Melamine Resin Hybrid Shell. Yang Tingjiao,Yuan Dong,Liu Wei,Zhang Zhe,Wang Kaiyu,You Yuxin,Ye Huapeng,de Haan Laurens T,Zhang Zhen,Zhou Guofu ACS applied materials & interfaces Thermochromic coatings that can change their color in response to variations in ambient temperature have various potential applications. Cholesteric liquid crystals (CLCs) are promising thermochromic materials due to their selective light reflection and wide regulation range. However, it remains a challenge to fabricate thermochromic coatings that combine good responsivity, mechanical strength, fabrication feasibility, and flexibility. In this study, CLC microcapsules containing cellulose nanocrystals (CNCs) and a melamine-formaldehyde (MF) resin hybrid shell were fabricated via in situ polymerization using CNC-stabilized Pickering emulsions as templates. The CNCs were employed as both Pickering emulsifiers and alignment agents of CLCs to prepare CLC Pickering emulsions. The CLC microcapsules were mixed with curable binders to obtain coating slurries, and thermochromic coatings were prepared by painting the slurries on substrates and drying. The thermochromic coatings could adjust their color in the visible wavelength range in a temperature range of 12 to 42 °C. Moreover, the obtained thermochromic coatings displayed a relatively high reflectance of up to 30-40% and can even be applied to flexible substrates. The CLC microcapsules with CNCs and an MF hybrid shell are promising in the field of smart decorative paints, anti-counterfeit labels, and artificial skins. 10.1021/acsami.1c23101
    Redox-Responsive Chiral Dopant for Quick Electrochemical Color Modulation of Cholesteric Liquid Crystal. Tokunaga Shoichi,Itoh Yoshimitsu,Tanaka Hiroyuki,Araoka Fumito,Aida Takuzo Journal of the American Chemical Society Here, we report the first redox-active chiral dopant D, which electrically alters its helical twisting power (HTP) for a cholesteric liquid crystalline (LC) medium and quickly changes the reflection color. D is composed of an axially chiral binaphthyl unit in conjunction with a redox-active ferrocene unit. A cholesteric LC phase of 4'-pentyloxy-4-cyanobiphenyl, doped with D (3.0 mol %), developed a blue reflection color. When nitrosyl tetrafluoroborate, a one-electron oxidant, was added to this cholesteric LC phase, D was oxidized to decrease its original HTP value by 13%, so that a green reflection color was developed. In the presence of a supporting electrolyte, the reflection color was electrochemically modulated using a sandwich-type glass cell with indium tin oxide electrodes. In quick response to the applied voltage of +1.5 V, the reflection color changed from blue to green within 0.4 s. When 0 V was applied, the reflection color returned to its original blue color. The D-doped cholesteric LC is characterized by its fastest electrochemical response and lowest operating voltage among those reported for electrically driven cholesteric LC devices. 10.1021/jacs.8b06323
    Broadband Reflection in Polymer-Stabilized Cholesteric Liquid Crystals via Thiol-Acrylate Chemistry. Hu Wei,Chen Mei,Wang Qian,Zhang Lanying,Yuan Xiaotao,Chen Feiwu,Yang Huai Angewandte Chemie (International ed. in English) Thiols are prone to react with a multitude of various functional groups in high yields, which has been widely used for surface- and particle-patterning, bioorganic synthesis, polymer modification, imprint nanolithography, the fabrication of optical components, hydrogel synthesis, and the curing of hard protective coatings. In this work, a chiral thiol with a high helical twisting power was synthesized through a novel synthetic route with high selectivity, yield, and cost-effectiveness. It was then used to fabricate a liquid-crystal composite film with ultra-wide broadband reflection via thiol click chemistry. Cholesteric liquid-crystal materials with broadband reflection have many potential applications for broadband polarizers, polarizer-free displays, organic optical data storage media, smart switchable reflective windows, and continuous waveband laser protection. 10.1002/anie.201902681
    Bioinspired, Cholesteric Liquid-Crystal Reflectors with Time-Controlled Coexisting Chiral and Achiral Structures. Boyon Cécilia,Soldan Vanessa,Mitov Michel ACS applied materials & interfaces The twisted structures of the chitin-based cuticle of beetles confer specific optical characteristics on them. Intrigued by the observation of Bragg gratings with a depth-dependent periodicity in the cuticle of beetles, we determine the experimental conditions leading to their transcription into cholesteric liquid-crystal oligomers. We correlate the optical properties of reflectors thus produced with their internal morphology, as observed by transmission electron microscopy. With the use of a single parameter, thermal annealing time, the reflection color is made time-tunable. Different spectral bands and reflection colors from golden yellow to NIR are available, and the irreversibility of the final color is reached at the end. On the basis of the design concept and these properties, these hybrid chiral-achiral materials inspire the fabrication of smart reflective labels. When encapsulated in the package of a product to be kept under cold conditions, the label records the history of the product conservation. Two kinds of information based on color changes are recorded as follows: qualitative information reporting that the product was kept outside of the specified storage temperature and quantitative information giving an indication of the time elapsed since the temperature exceeded the storage temperature of the product. 10.1021/acsami.1c08218
    Dynamic Circularly Polarized Luminescence with Tunable Handedness and Intensity Enabled by Achiral Dichroic Dyes in Cholesteric Liquid Crystal Medium. Advanced materials (Deerfield Beach, Fla.) Cholesteric liquid crystals (CLCs) are chiral supramolecular systems that self-assemble into a highly regular helical arrangement in a liquid crystal (LC) medium. Such an arrangement is highly beneficial for the chiral enlargement effect on circularly polarized luminescence (CPL) signals. Dichroic dyes with rod-like molecular structures can exhibit fluorescence anisotropy along both the long and short molecular axes owing to their transition dipole moment (TDM) vectors. In this work, a pair of donor-accepter (D-A) achiral dichroic dyes is prepared, namely, 3,4-ethylenedioxythiophene derivative (P1, whose TDM vector is parallel to the long axis of the molecule, i.e., F  > F ) and anthraquinone derivative (N1, whose TDM vector is perpendicular to the long axis of the molecule, i.e., F  < F ). CLCs can be fabricated by doping P1 or N1 together with chiral 1,1'-binaphthyl-derived inducers into SLC1717 medium. Dynamic CPL with tunable handedness and intensity is achieved by changing the N1:P1 mass ratio, and the luminescence dissymmetry factor (g ) value reaches |0.71|. This work describes the first observation of dynamic CPL with tunable handedness and intensity enabled by TDM regulation of achiral dichroic dyes in a CLC medium. 10.1002/adma.202202309
    Nanoscale Organization of a Platinum(II) Acetylide Cholesteric Liquid Crystal Molecular Glass for Photonics Applications. Cooper Thomas M,Haley Joy E,Stewart David J,Long Stephanie,Krein Douglas M,Burke Aaron R,Arias Eduardo,Moggio Ivana,Turlakov Gleb,Ziolo Ronald F,Biler Michal,Linares Mathieu,Norman Patrick Advanced functional materials The fabrication, molecular structure, and spectroscopy of a stable cholesteric liquid crystal platinum acetylide glass obtained from -Pt(PEt)(C≡C-CH-C≡N)(C≡C-CH-COO-Cholesterol), are described and designated as PE1-CN-Chol. Polarized optical microscopy, differential scanning calorimetry, and wide-angle X-ray scattering experiments show room temperature glassy/crystalline texture with crystal formation upon heating to 165 °C. Further heating results in conversion to cholesteric phase. Cooling to room temperature leads to the formation of a cholesteric liquid crystal glass. Scanning tunneling microscopy of a PE1-CN-Chol monolayer reveals self-assembly at the solid-liquid interface with an array of two molecules arranged in pairs, oriented head-to-head through the CN groups, giving rise to a lamella arrangement. The lamella structure obtained from molecular dynamics calculations shows a clear phase separation between the conjugated platinum acetylide and the hydrophobic cholesterol moiety with the lamellae separation distance being 4.0 nm. Ultrafast transient absorption and flash photolysis spectra of the glass show intersystem crossing to the triplet state occurring within 100 ps following excitation. The triplet decay time of the film compared to aerated and deoxygenated solutions is consistent with oxygen quenching at the film surface but not within the film. The high chromophore concentration, high glass thermal stability, and long triplet lifetime in air show that these materials have potential as nonlinear absorbing materials. 10.1002/adfm.201910562
    3D-Printed Biomimetic Systems with Synergetic Color and Shape Responses Based on Oblate Cholesteric Liquid Crystal Droplets. Yang Chenjing,Wu Baiheng,Ruan Jian,Zhao Peng,Chen Li,Chen Dong,Ye Fangfu Advanced materials (Deerfield Beach, Fla.) Living organisms in nature have amazing control over their color, shape, and morphology in response to environmental stimuli for camouflage, communication, or reproduction. Inspired by the camouflage of the octopus via the elongation or contraction of its pigment cells, oblate cholesteric liquid crystal droplets are dispersed in a polymer matrix, serving as the role of pigment cells and showing structural color due to selective Bragg reflection by their periodic helical structure. The color of 3D-printed biomimetic systems can be tuned by changing the helical pitch via the chiral dopant concentration or temperature. When the oblate liquid crystal droplets are heated up to isotropic, the opaque and colored biomimetic systems become transparent and colorless. Meanwhile, the isotropic liquid crystal droplets tend to become spherical, causing volume contraction along the film plane and volume dilation in the perpendicular direction. The internal strain combined with the gradient distribution of the oblate isotropic liquid crystal droplets result in corresponding shape transformations. The camouflage of a biomimetic octopus and the blossom of a biomimetic flower, both of which show synergetic color and shape responses, are demonstrated to inspire the design of functional materials and intelligent devices. 10.1002/adma.202006361
    Remotely Controlling Drug Release by Light-Responsive Cholesteric Liquid Crystal Microcapsules Triggered by Molecular Motors. Huang Rui,Lan Ruochen,Shen Chen,Zhang Zhongping,Wang Zichen,Bao Jinying,Wang Zizheng,Zhang Lanying,Hu Wei,Yu Zhan,Zhu Siquan,Wang Lei,Yang Huai ACS applied materials & interfaces Stimuli-responsive smart nanocarriers are an emerging class of materials applicable in fields including drug delivery and tissue engineering. Instead of constructing responsive polymer shells to control the release and delivery of drugs, in this work, we put forward a novel strategy to endow the internal drugs with light responsivity. The microcapsule consisted of molecular motor (MM)-doped cholesteric liquid crystals (CLCs) and drugs. The drug in gelatin-gum arabic microcapsules can protect the carried drugs for a long time with a low release speed totally resulting from drug diffusion. Under UV light, the MM isomerizes and the chirality changes, inducing the alteration of the superstructure of the CLCs. In this process, the cooperative molecular disturbance accelerates the diffusion of the drugs from the microcapsule core to the outside. As a result, thanks to the cooperative effect of liquid crystalline mesogens, molecular-scale geometric changes of motors could be amplified to the microscale disturbance of the self-organized superstructure of the CLCs, resulting in the acceleration of the drug release. This method is hoped to provide opportunities in the design and fabrication of novel functional drug delivery systems. 10.1021/acsami.1c16367
    Dual-Cross-linked Liquid Crystal Hydrogels with Controllable Viscoelasticity for Regulating Cell Behaviors. ACS applied materials & interfaces The liquid crystal properties and viscoelasticity of the natural bone extracellular matrix (ECM) play a decisive role in guiding cell behavior, conducting cell signals, and regulating mineralization. Here, we develop a facile approach for preparing a novel polysaccharide hydrogel with liquid crystal properties and viscoelasticity similar to those of natural bone ECM. First, a series of chitin whisker/chitosan (CHW/CS) hydrogels were prepared by chemical cross-linking with genipin, in which CHW can self-assemble to form cholesteric liquid crystals under ultrasonic treatment and CS chains can enter into the gaps between the helical layers of the CHW cholesteric liquid crystal phase to endow morphological stability and good mechanical properties. Subsequently, the obtained chemically cross-linked liquid crystal hydrogels were immersed into the desired concentration of the NaCl solution to form physical cross-linking. Due to the Hofmeister effect, the as-prepared dual-cross-linked liquid crystal hydrogels showed an enhanced modulus, viscoelasticity similar to that of natural ECM with relatively fast stress relaxation behavior, and fold surface morphology. Compared to both CHW/CS hydrogels without liquid crystal properties and CHW/CS liquid crystal hydrogels without further physical cross-linking, the dual-cross-linked CHW/CS liquid crystal hydrogels are more favorable for the adhesion, proliferation, and osteogenic differentiation of bone marrow mesenchymal stem cells. This approach could inspire the design of hydrogels mimicking the liquid crystal properties and viscoelasticity of natural bone ECM for bone repair. 10.1021/acsami.2c02689
    Dispersing swimming microalgae in self-assembled nanocellulose suspension: Unveiling living colloid dynamics in cholesteric liquid crystals. Journal of colloid and interface science Active matter comprises individual energy-consuming components that convert locally stored energy into mechanical motion. Among these, liquid crystal dispersed self-propelled colloids have displayed fascinating dynamic effects and nonequilibrium behaviors. In this work, we introduce a new type of active soft matter based on swimming microalgae and lyotropic nanocellulose liquid crystal. Cellulose is a kind of biocompatible polysaccharide that nontoxic to living biological colloids. In contrast to microalgae locomotion in isotropic and low viscosity media, we demonstrate that the propulsion force of swimming microalgae can overcome the stabilizing elastic force in cholesteric nanocellulose liquid crystal, with the displacement dynamics (gait, direction, frequency, and speed) be altered by the surrounding medium. Simultaneously, the active stress and shear flow exerted by swimming microalgae can introduce local perturbation in surrounding liquid crystal orientation order. The latter effect yields hydrodynamic fluctuations in bulk phase as well as layer undulations, helicoidal axis splay deformation and director bending in the cholesteric assembly, which finally followed by a recovery according to the inherent viscoelasticity of liquid crystal matrix. Our results point to an unorthodox design concept to generate a new type of hybrid soft matter that combines nontoxic cholesteric liquid crystal and active particles, which are expected to open opportunities in biosensing and biomechanical applications. 10.1016/j.jcis.2022.05.012