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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 Porphyrin- and Fullerene/Porphyrin-Based Rotaxanes as Studied by Time-Resolved EPR Spectroscopy
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Photoinduced Electron Transfer in Porphyrin- and Fullerene/Porphyrin-Based Rotaxanes as Studied by Time-Resolved EPR Spectroscopy

机译：时间分辨EPR光谱研究基于卟啉和富勒烯/卟啉的轮烷中的光诱导电子转移

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摘要

Photoinduced intramolecular electron-transfer (ET) and energy-transfer (EnT) processes in two rotaxanes, one containing both zinc porphyrin and C60 fullerene moieties incorporated around the Cu(I) bisphenanthroline core [(ZnP)2-Cu(I)(phen)2-C60] and a second complex lacking the fullerene [(ZnP)2-Cu(I)(phen)2], were studied by time-resolved electron paramagnetic resonance (TREPR) spectroscopy at 9.5 GHz (X-band) combined with a selective photoexcitation of the rotaxane moieties. The experiments were carried out in isotropic toluene and ethanol and in anisotropic nematic liquid-crystal (E-7) media over a wide range of temperatures corresponding to the different states of the solvents. The TREPR results are compared with those obtained previously by optical methods in dichloromethane at room temperature. It is demonstrated that the efficiencies and pathways of the light-driven ET and EnT processes in both rotaxanes strongly depend on the properties of their microenvironment, resulting in the formation of distinct charge-separated states under different experimental conditions. The complementary results revealed by the optical and TREPR techniques are attributed to the relatively high conformational mobility of the mechanically interlocked rotaxane systems. Because of the solute-solvent interactions, the rotaxanes are able to change conformation in different microenvironments, which affects the parameters of the photoinduced processes occurring in these systems.
机译：两种轮烷中的光诱导分子内电子转移（ET）和能量转移（EnT）过程，其中一种包含卟啉锌和C60富勒烯部分，并结合在Cu（I）双菲咯啉核[（ZnP）2-Cu（I）（phen）周围）2-C60]和缺少富勒烯的第二种复合物[（ZnP）2-Cu（I）（phen）2]，通过时间分辨电子顺磁共振（TREPR）光谱在9.5 GHz（X波段）组合下进行了研究对轮烷部分进行选择性光激发。实验是在各向同性甲苯和乙醇中以及在各向异性向列液晶（E-7）介质中，在与溶剂的不同状态相对应的较宽温度范围内进行的。将TREPR结果与先前通过光学方法在室温于二氯甲烷中获得的结果进行比较。结果表明，两种轮烷中光驱动的ET和EnT过程的效率和途径强烈取决于其微环境的性质，导致在不同的实验条件下形成不同的电荷分离态。光学和TREPR技术揭示的互补结果归因于机械互锁轮烷体系的相对较高的构象迁移率。由于溶质与溶剂的相互作用，轮烷能够在不同的微环境中改变构象，从而影响这些系统中发生的光诱导过程的参数。

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