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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Anomalously Selective Quenching of S_2Fluorescence from Upper Excited State of Zinc5-(1'-Pyrenyl)-10,15,20-triphenylporphyrin Derivatives through Intramolecular ChargeTransfer State
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Anomalously Selective Quenching of S_2Fluorescence from Upper Excited State of Zinc5-(1'-Pyrenyl)-10,15,20-triphenylporphyrin Derivatives through Intramolecular ChargeTransfer State

机译：通过分子内电荷转移态从Zinc5-（1'-yr烯基）-10,15,20-三苯基卟啉衍生物的上激发态对S_2荧光的异常选择性猝灭

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摘要

Zinc 5-(1'-pyrenyl)-l0,15,20-tris(p-methoxyphenyl)porphyrin (ZnP-Py) and zinc 5-(1'-pyreny1)-10,15,20-tris(pentafluorophenyl)porphyrin (ZnFP-Py), in which a pyrenyl group is directly connected at the meso-positions of their corresponding porphyrins, were synthesized and investigated on the photophysical properties.While the S_1 fluorescence of the porphyrin moieties was not quenched by the pyrenyl group at all, theS_2fluorescence was remarkably quenched. The anomalously selective quenching of the S_2fluorescence wasdependent on the solvent polarity, and the quenching was enhanced in the polar solvent. The S_2fluorescencequenching is considered to take place through an intramolecular charge transfer state. Interestingly, the chargetransfer state relaxes to the S_1, state through the rapid charge recombination with high quantum yield. Thecharge transfer rate of ZnFP-Py, which was calculated from the S_2fluorescence quenching, was larger thanthat of ZnP-Py, possibly due to the differences in the free-energy changes of the electron transfer and theelectron densities at their meso-positions. This study has suggested that ultrafast electron transfer from theupper excited state and charge recombination to S_1 can occur in a directly connected electron donor—acceptorsystem.
机译：锌5-（1'-苯基）-1,0,15,20-三（对甲氧基苯基）卟啉（ZnP-Py）和锌5-（1'-苯基）-1,10,15,20-三（五氟苯基）卟啉（ZnFP-Py）合成了一个在其相应卟啉的介孔位置上直接连接有pyr基的化合物（ZnFP-Py），并对其光物理性质进行了研究。尽管卟啉部分的S_1荧光并未完全被enyl基淬灭，S_2荧光被显着淬灭。 S_2荧光的异常选择性猝灭取决于溶剂的极性，而极性溶剂的猝灭作用增强。 S_2荧光猝灭被认为是通过分子内电荷转移状态发生的。有趣的是，通过快速的电荷重组和高量子产率，电荷转移状态松弛到S_1状态。由S_2荧光猝灭计算得出的ZnFP-Py的电荷转移速率大于ZnP-Py的电荷转移速率，这可能是由于电子转移的自由能变化和介电常数处电子密度的差异所致。这项研究表明，在直接连接的电子供体-受体系统中，可以发生从上激发态到电荷再结合到S_1的超快电子转移。

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