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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photoinduced electron transfer in double-bridged porphyrin-fullerene triads
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Photoinduced electron transfer in double-bridged porphyrin-fullerene triads

机译：双桥卟啉-富勒烯三联体中的光诱导电子转移

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摘要

Electron and energy transfer reactions of porphyrin-porphyrin-fullerene triads (P2P1C) with controllable sandwich-like structures have been studied using spectroscopic and electrochemical methods. The stabile, stacked structure of the molecules was achieved applying a two-linker strategy developed previously for porphyrin-fullerene dyads. Different triad structures with altered linker positions, linker lengths, and center atoms of the porphyrin rings were studied. The final charge-separated (CS) state and the different transient states of the reactions have been identified and energies of the states estimated based on the experimental results. In particular,a complete CS state P2+P1C- was achieved in a zinc porphyrin-free-base porphyrin-fullerene triad (ZnP(2)t9P(1)C) in both polar (benzonitrile) and nonpolar (toluene) solvents. The lifetime of this state was longer living in the nonpolar solvent. An outstanding feature of the ZnP(2)t9P(1)C triad is the extremely fast formation of the final CS state, P2+P1C-. This state is formed after primary excitation of either zinc porphyrin or free-base porphyrin chromophores in less than 200 fs. Although the intermediate steps between the locally excited states and the final CS state were not time-resolved for this compound, the process is clearly multistep and the fastest ever observed for porphyrin-based compounds.
机译：用光谱和电化学方法研究了具有可控三明治状结构的卟啉-卟啉-富勒烯三联体（P2P1C）的电子和能量转移反应。使用先前为卟啉-富勒烯二聚体开发的双接头策略，可实现分子的稳定堆叠结构。研究了具有改变的接头位置，接头长度和卟啉环中心原子的三合一结构。已经确定了最终的电荷分离（CS）状态和反应的不同瞬态，并根据实验结果估算了这些态的能量。特别是，在极性（苯甲腈）和非极性（甲苯）溶剂中，无锌卟啉基卟啉-富勒烯三联体（ZnP（2）t9P（1）C）中均获得了完全的CS状态P2 + P1C-。在非极性溶剂中，该状态的寿命更长。 ZnP（2）t9P（1）C三联体的一个突出特点是最终CS态P2 + P1C-的快速形成。在小于200 fs的时间内激发锌卟啉或游离碱卟啉发色团后形成此状态。尽管对于该化合物而言，在局部激发态和最终CS态之间的中间步骤没有时间分辨，但该过程显然是多步骤的，并且对于基于卟啉的化合物而言是观察到最快的。

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