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Acc Chem Res

Title:		Molecular and Supramolecular Designs of Organic/Polymeric Micro-photoemitters for Advanced Optical and Laser Applications
Author(s):		Yamamoto Y; Yamagishi H; Huang JS; Lorke A;
Address:		"Department of Materials Science, Faculty of Pure and Applied Sciences, and Tsukuba Research Center for Energy Materials Science (TREMS), University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573, Japan. Leibniz Institute of Photonic Technology, Albert-Einstein Str. 9, 07745 Jena, Germany. Institute of Physical Chemistry and Abbe Center of Photonics, Friedrich-Schiller-Universitat Jena, Helmholtzweg 4, D-07743 Jena, Germany. Research Center for Applied Sciences, Academia Sinica, 128 Sec. 2, Academia Road, Nankang District, Taipei 11529, Taiwan. Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan. Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, Lotharstrabetae 1, Duisburg D-47048, Germany"
Journal Title:		Acc Chem Res
Year:		2023
Volume:		20230523
Issue:		12
Page Number:		1469 - 1481
DOI:		10.1021/acs.accounts.3c00084
ISSN/ISBN:		1520-4898 (Electronic) 0001-4842 (Linking)
Abstract:		"ConspectusFor optical and electronic applications of supramolecular assemblies, control of the hierarchical structure from nano- to micro- and millimeter scale is crucial. Supramolecular chemistry controls intermolecular interactions to build up molecular components with sizes ranging from several to several hundreds of nanometers using bottom-up self-assembly process. However, extending the supramolecular approach up to a scale of several tens of micrometers to construct objects with precisely controlled size, morphology, and orientation is challenging. Especially for microphotonics applications such as optical resonators and lasers, integrated optical devices, and sensors, a precise design of a micrometer-scale object is required. In this Account, we review the recent progress on precise control of microstructures from pi-conjugated organic molecules and polymers, which work as micro-photoemitters and are suitable for optical applications.After the introduction on the importance of the control of the hierarchical structures from molecular assembly, we review supramolecular methodology for assembling molecules and supramolecules to form microstructures such as spheres and polygons with precisely controlled morphology and molecular orientations. The resultant microstructures act as anisotropic emitters of circularly polarized luminescence. We report that synchronous crystallization of pi-conjugated chiral cyclophanes forms concave hexagonal pyramidal microcrystals with homogeneous size, morphology, and orientation, which clearly paves the way for the precise control of skeletal crystallization under kinetic control. Furthermore, we show microcavity functions of the self-assembled micro-objects. The self-assembled pi-conjugated polymer microspheres work as whispering gallery mode (WGM) optical resonators, where the photoluminescence exhibits sharp and periodic emission lines. The spherical resonators with molecular functions act as long-distance photon energy transporters, convertors, and full-color microlasers. Fabrication of microarrays with photoswitchable WGM microresonators by the surface self-assembly technique realizes optical memory with physically unclonable functions of WGM fingerprints. All-optical logic operations are demonstrated by arranging the WGM microresonators on synthetic and natural optical fibers, where the photoswitchable WGM microresonators act as a gate for light propagation via a cavity-mediated energy transfer cascade. Meanwhile, the sharp WGM emission line is appropriate for utilization as optical sensors for monitoring the mode shift and mode splitting. The resonant peaks sensitively respond to humidity change, absorption of volatile organic compounds, microairflow, and polymer decomposition by utilizing structurally flexible polymers, microporous polymers, nonvolatile liquid droplets, and natural biopolymers as media of the resonators. We further construct microcrystals from pi-conjugated molecules with rods and rhombic plates, which act as WGM laser resonators with light-harvesting function. Our developments, precise design and control of organic/polymeric microstructures, form a bridge between nanometer-scale supramolecular chemistry and bulk materials and pave the way toward flexible micro-optics applications"
Keywords:
Notes:		"PubMed-not-MEDLINEYamamoto, Yohei Yamagishi, Hiroshi Huang, Jer-Shing Lorke, Axel eng 2023/05/23 Acc Chem Res. 2023 Jun 20; 56(12):1469-1481. doi: 10.1021/acs.accounts.3c00084. Epub 2023 May 23"