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Protein-Framed Multi-Porphyrin Micelles for a Hybrid Natural-Artificial Light-Harvesting Nanosystem

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      Lessons from nature about solar light harvesting.

      Solar fuel production often starts with the energy from light being absorbed by an assembly of molecules; this electronic excitation is subsequently transferred to a suitable acceptor. For example, in photosynthesis, antenna complexes capture sunlight and direct the energy to reaction centres that then carry out the associated chemistry. In this Review, we describe the principles learned from studies of various natural antenna complexes and suggest how to elucidate strategies for designing light-harvesting systems. We envisage that such systems will be used for solar fuel production, to direct and regulate excitation energy flow using molecular organizations that facilitate feedback and control, or to transfer excitons over long distances. Also described are the notable properties of light-harvesting chromophores, spatial-energetic landscapes, the roles of excitonic states and quantum coherence, as well as how antennas are regulated and photoprotected.
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        Light-harvesting conjugated microporous polymers: rapid and highly efficient flow of light energy with a porous polyphenylene framework as antenna.

        The molecular design of light-harvesting antennae requires not only the segregation of a large number of chromophore units in a confined nanospace but also the cooperation of these units in achieving highly efficient energy transduction. This article describes the synthesis and functions of a polyphenylene-based conjugated microporous polymer (PP-CMP). PP-CMP was recently designed and synthesized by Suzuki polycondensation reaction and used as an antenna for the noncovalent construction of a light-harvesting system. In contrast to linear polyphenylene, PP-CMP consists of conjugated three-dimensional polyphenylene scaffolds and holds inherent porous structure with uniform pore size (1.56 nm) and large surface area (1083 m(2) g(-1)). It emits blue photoluminescence, is capable of excitation energy migration over the framework, and enables rapid transportation of charge carrier with intrinsic mobility as high as 0.04 cm(2) V(-1) s(-1). The microporous structure of PP-CMP allows for the spatial confinement of energy-accepting coumarin 6 molecules in the pores and makes the high-throughput synthesis of light-harvesting systems with designable donor-acceptor compositions possible. Excitation of the PP-CMP skeleton leads to brilliant green emission from coumarin 6, with an intensity 21-fold as high as that upon direct excitation of coumarin 6 itself, while the fluorescence from PP-CMP itself is wholly quenched as a result of energy transfer from the light-harvesting PP-CMP framework to coumarin 6. The PP-CMP skeleton is highly cooperative, with an average of 176 phenylene units working together to channel the excitation energy to one coumarin 6 molecule, and features the energy-transfer process with quick, efficient, and vectorial character. These unique characteristics clearly originate from the conjugated porous structure and demonstrate the usefulness of CMPs in the exploration of pi-electronic functions, in addition to their gas adsorption properties thus far reported.
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          Light-harvesting metal-organic frameworks (MOFs): efficient strut-to-strut energy transfer in bodipy and porphyrin-based MOFs.

          A pillared-paddlewheel type metal-organic framework material featuring bodipy- and porphyrin-based struts, and capable of harvesting light across the entire visible spectrum, has been synthesized. Efficient-essentially quantitative-strut-to-strut energy transfer (antenna behavior) was observed for the well-organized donor-acceptor assembly consituting the ordered MOF structure.
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            Author and article information

            Affiliations
            [1 ]School of Chemistry and Chemical Engineering; State Key Laboratory of Metal Matrix Composites; Shanghai Jiao Tong University; 800 Dongchuan Road Shanghai 200240 China
            Journal
            Angewandte Chemie International Edition
            Angew. Chem. Int. Ed.
            Wiley
            14337851
            July 04 2016
            July 04 2016
            May 17 2016
            : 55
            : 28
            : 7952-7957
            10.1002/anie.201601516
            © 2016

            http://doi.wiley.com/10.1002/tdm_license_1.1

            http://onlinelibrary.wiley.com/termsAndConditions#vor

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