首页> 外文期刊>Chemistry: A European journal >Strongly Coupled Oxasmaragdyrin-BF_2 Chelated Dipyrrin Dyads: Syntheses, X-ray Structure, Ground- and Excited-State Charge- Transfer Interactions
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Strongly Coupled Oxasmaragdyrin-BF_2 Chelated Dipyrrin Dyads: Syntheses, X-ray Structure, Ground- and Excited-State Charge- Transfer Interactions

机译:强耦合的Oxasmaragdyrin-BF_2螯合的双吡啶二元:合成,X射线结构,地面和兴奋状态电荷相互作用

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摘要

Oxasmaragdyrin (osm), a 22-π electron aromatic macrocycle containing four pyrroles and a furan ring connected by three methine bridges and two direct bonds is shown to be an excellent electron donor-sensitizer exhibiting adequate spectral and redox properties. Further, this novel heterocyclic macromolecule has been utilized in building donor-acceptor systems involving BF_2-chelated dipyrromethenes (BODIPYs). The osm-BODIPY dyads were fully characterized by optical, electrochemical, computational, and X-ray diffraction studies. Due to close proximity and electronic structure of the donor and acceptor entities, strong intramolecular charge-transfer interactions in these dyads was witnessed and was supported by computational studies. Solvent-polarity-dependent rapid charge separation and charge recombination in these dyads is witnessed from photochemical studies involving time-resolved emission and femtosecond transient absorption studies. The present studies bring out the importance of oxasmaragdyrin as an electron donor in light-energy-harvesting artificial photosynthesis model systems.
机译:Oxasmaragdyrin(OSM),含有四个胃蛋白的22-π电子芳族宏环和由三个甲基桥连接的呋喃环和两个直接键合,是一种优异的电子供体敏化剂,其具有足够的光谱和氧化还原性能。此外,这种新的杂环大分子已被用于建立涉及BF_2-Chelated Dizyromethenes(Bodipys)的供体 - 受体系统。 OSM-Bodipy Dyads通过光学,电化学,计算和X射线衍射研究完全表征。由于施主和受体实体的近距离和电子结构,目睹了这些二元的强的分子内电荷转移相互作用,并通过计算研究支持。这些二元的溶剂极性依赖性快速分离和电荷重组得到了涉及时间分辨排放和飞秒瞬态吸收研究的光化学研究。本研究提出了在光能收集人造光合作用模型系统中作为电子供体的氧镁杀死的重要性。

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