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首页> 外文期刊>Chemistry: A European journal >Excitation-wavelength-dependent, ultrafast photoinduced electron transfer in bisferrocene/BF_2-chelated-azadipyrromethene/fullerene tetrads
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Excitation-wavelength-dependent, ultrafast photoinduced electron transfer in bisferrocene/BF_2-chelated-azadipyrromethene/fullerene tetrads

机译：双铁茂铁/ BF_2螯合的叠氮二茂铁/富勒烯四联体中依赖于激发波长的超快光诱导电子转移

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摘要

Donor-acceptor distance, orientation, and photoexcitation wavelength are key factors in governing the efficiency and mechanism of electron-transfer reactions both in natural and synthetic systems. Although distance and orientation effects have been successfully demonstrated in simple donor-acceptor dyads, revealing excitation-wavelength-dependent photochemical properties demands multimodular, photosynthetic-reaction-center model compounds. Here, we successfully demonstrate donor- acceptor excitation-wavelength-dependent, ultrafast charge separation and charge recombination in newly synthesized, novel tetrads featuring bisferrocene, BF_2-chelated azadipyrromethene, and fullerene entities. The tetrads synthesized using multistep synthetic procedure revealed characteristic optical, redox, and photo reactivities of the individual components and featured "closely" and "distantly" positioned donor-acceptor systems. The near-IR-emitting BF_2-chelated azadipyrromethene acted as a photosensitizing electron acceptor along with fullerene, while the ferrocene entities acted as electron donors. Both tetrads revealed excitation-wavelength-dependent, photoinduced, electron-transfer events as probed by femtosecond transient absorption spectroscopy. That is, formation of the Fc~+-ADP-C_(60).- charge-separated state upon C_(60) excitation, and Fc~+-ADP.~--C _(60) formation upon ADP excitation is demonstrated.
机译：供体-受体的距离，取向和光激发波长是控制天然和合成系统中电子转移反应的效率和机理的关键因素。尽管在简单的供体-受体二元组中已成功证明了距离和方向效应，但揭示激发波长依赖的光化学性质需要多模量，光合反应中心模型化合物。在这里，我们成功地证明了供体-受体激发波长相关的超快电荷分离和电荷复合，这些化合物是新合成的新颖双分子，其特征为双二茂铁，BF_2螯合的氮杂二吡咯甲烯和富勒烯实体。使用多步合成程序合成的四线联体显示了各个组分的特征性光学，氧化还原和光反应性，并具有“紧密”和“远距离”定位的供体-受体系统。发射近红外光的BF_2螯合的氮杂二吡咯甲烷与富勒烯一起用作光敏电子受体，而二茂铁实体则用作电子给体。如飞秒瞬态吸收光谱所探测到的，两个四分体都显示出与激发波长有关的光诱导电子转移事件。即，证明了在C_（60）激发时形成Fc〜+ -ADP-C_（60）-电荷分离状态，并且在ADP激发时形成了Fc〜+ -ADP-C_（60）-。 。

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