Circularly Polarized Laser with Chiral Nematic Cellulose Nanocrystal Cavity.
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ABSTRACT:
SUBMITTER: Qu D
PROVIDER: S-EPMC8266174 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Circularly polarized light (CPL) detection and polarization state recognition are required for a wide range of applications. Conventional polarization detection with optical components causes difficulties for miniaturization and integration. An effective design strategy is proposed for direct CPL detection with chiral material. Here, we realized direct CPL detection based on the combination of chiral photonic cellulose nanocrystal (CNC) and ultraviolet-sensitive ZnO photoconductive material. The CNC layer deposited by evaporation-induced self-assembly established the left-handed chiral nematic structure with a photonic bandgap (PBG) to recognize left-handed CPL (LCPL) and right-handed CPL (RCPL) at specific wavelengths. The PBG of CNC layer has been modulated by the adjustment of chiral nematic pitch to match the semiconductor bandgap of ZnO film in ultraviolet region. The photocurrents under RCPL and LCPL are 2.23 × 10-6 A and 1.77 × 10-6 A respectively and the anisotropy factor Δgpc of 0.23 is acquired for the CPL detection based on the chiral photonic CNC. This design provides a new approach to the detection of CPL polarization state with competitive performance.
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Project description:Cellulosic liquid crystalline solutions and suspensions form chiral nematic phases that show a rich variety of optical textures in the liquid crystalline state. These ordered structures may be preserved in solid films prepared by evaporation of solvent or suspending medium. Film formation from aqueous suspensions of cellulose nanocrystals (CNC) was investigated by polarized light microscopy, optical profilometry and atomic force microscopy (AFM). An attempt is made to interpret qualitatively the observed textures in terms of the orientation of the cellulose nanocrystals in the suspensions and films, and the changes in orientation caused by the evaporative process. Mass transfer within the evaporating droplet resulted in the formation of raised rings whose magnitude depended on the degree of pinning of the receding contact line. AFM of dry films at short length scales showed a radial orientation of the CNC at the free surface of the film, along with a radial height variation with a period of approximately P/2, ascribed to the anisotropic shrinkage of the chiral nematic structure.
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Project description:The direct generation of efficient, tunable, and switchable circularly polarized laser emission (CPLE) would have far-reaching implications in photonics and material sciences. In this paper, we describe the first chiral simple organic molecules (SOMs) capable of simultaneously sustaining significant chemical robustness, high fluorescence quantum yields, and circularly polarized luminescence (CPL) ellipticity levels (|glum|) comparable to those of similar CPL-SOMs. All these parameters altogether enable efficient laser emission and CPLE with ellipticity levels 2 orders of magnitude stronger than the intrinsic CPL ones.
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Project description:Materials capable of circularly polarized luminescence (CPL) have attracted considerable attention for their promising potential applications. Bacterial cellulose (BC) was characterized as having a stable right-handed twist, which makes it a potential chiral host to endow luminophores with CPL. Then, the CPL-active BC composite film was constructed by simply impregnating bacterial cellulose pellicles with dilute aqueous solutions of luminophores (rhodamine B, carbon dots, polymer dots) and drying under ambient conditions. Simple encapsulation of luminophores renders BC with circularly polarized luminescence with a dissymmetry factor of up to 0.03. The multiple chiral centers of bacterial cellulose provide a primary asymmetric environment that can be further modulated by supramolecular chemistry, which is responsible for its circular polarization ability. We further demonstrate that commercial grade paper may endow luminophores with CPL activity, which reifies the universality of the method.
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Project description:Polymer electroluminescence devices producing circularly polarized luminescence (CP PLEDs) have valuable photonic applications. The fabrication of a CP PLED requires a polymer host that provides the appropriate chiral environment around the emitting dopant. However, chemical strategies for the design of chiral polymer hosts remain underdeveloped. We have developed new polymer hosts for CP PLED applications. These polymers were prepared through a free-radical polymerization of 3-vinylcarbazole with a chiral N-alkyl unit. This chiral unit forces the carbazole repeat units to form mutually helical half-sandwich conformers with preferred (P)-helical sense along the polymer main chain. Electronic circular dichroism measurements demonstrate the occurrence of chirality transfer from chiral monomers to achiral monomers during chain growth. The (P)-helical-sense-enriched polymer interacts diastereoselectively with an enantiomeric pair of new phosphorescent (R)- and (S)-dopants. The magnitude of the Kuhn dissymmetry factor (g abs) for the (P)-helically-enriched polymer film doped with the (R)-dopant was found to be one order of magnitude higher than that of the film doped with the (S)-dopant. Photoluminescence dissymmetry factors (g PL) of the order of 10-3 were recorded for the doped films, but the magnitude of diastereomeric enhancement decreased to that of g abs. The chiral polymer host permits faster energy transfer to the phosphorescent dopants than the achiral polymer host. Our photophysical and morphological investigations indicate that the acceleration in the chiral polymer host is due to its longer Förster radius and improved compatibility with the dopants. Finally, multilayer CP PLEDs were fabricated and evaluated. Devices based on the chiral polymer host with the (R)- and (S)-dopants exhibit electroluminescence dissymmetry factors (g EL) of 1.09 × 10-4 and -1.02 × 10-4 at a wavelength of 540 nm, respectively. Although challenges remain in the development of polymer hosts for CP PLEDs, our research demonstrates that chiroptical performances can be amplified by using chiral polymer hosts.
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Project description:Circularly polarized light (CPL) detection is required in various fields such as drug screening, security surveillance and quantum optics. Conventionally, CPL photodetector needs the installation of optical elements, imposing difficulties for integrated and flexible devices. The established CPL detectors without optical elements rely on chiral organic semiconductor and metal metamaterials, but they suffer from extremely low responsivity. Organic-inorganic hybrid materials combine CPL-sensitive absorption induced by chiral organics and efficient charge transport of inorganic frameworks, providing an option for direct CPL detection. Here we report the CPL detector using chiral organic-inorganic hybrid perovskites, and obtain a device with responsivity of 797 mA W-1, detectivity of 7.1 × 1011 Jones, 3-dB frequency of 150 Hz and one-month stability, a competitive combined feature for circularly polarized light detection. Thanks to the solution processing, we further demonstrate flexible devices on polyethylene terephthalate substrate with comparable performance.
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Project description:The chiral nematic nanostructure formed from cellulose nanocrystal (CNC) self-assembly has shown great potential as a matrix for generating circularly polarized luminescent (CPL) light with a high dissymmetry factor. Exploring the relationship between the device composition and structure and the light dissymmetry factor is crucial to a common strategy for a strongly dissymmetric CPL light. In this study, we have compared the single-layered and double-layered CNC-based CPL devices with different luminophores, such as rhodamine 6G (R6G), methylene blue (MB), crystal violet (CV), and silicon quantum dots (Si QDs). We demonstrated that forming a double-layered structure of CNCs nanocomposites is a simple but effective pathway for enhancing the CPL dissymmetry factor for CNC-based CPL materials containing different luminophores. The |glum| values of double-layered CNC devices (dye@CNC5||CNC5) versus that of single-layered devices (dye@CNC5) are 3.25 times for Si QDs, 3.7 times for R6G, 3.1 times for MB, and 2.78 times for CV series. The different enhancement degrees of these CNC layers with a similar thickness may be due to the different pitch numbers in the chiral nematic liquid crystal layers whose photonic band gap (PBG) has been modified to match the emission wavelengths of dyes. Furthermore, the assembled CNC nanostructure has great tolerance to the addition of nanoparticles. Gold nanorods coated with the SiO2 layer (Au NR@SiO2) were added for enhancing the dissymmetry factor of MB in CNC composites (named MAS devices). When the strong longitudinal plasmonic band of the Au NR@SiO2 matched the emission wavelength of MB and the PBG of assembled CNC structures simultaneously, the increase in the glum factor and quantum yield of MAS composites was obtained. The good compatibility of the assembled CNC nanostructures makes it a universal platform for developing strong CPL light sources with a high dissymmetry factor.
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