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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >[6,6]-Closed versus [6-5]-Open Isomers of Imino- and Methanofullerenes: A Comparison with Pristine C_(60) and (C_(59)N)~·
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[6,6]-Closed versus [6-5]-Open Isomers of Imino- and Methanofullerenes: A Comparison with Pristine C_(60) and (C_(59)N)~·

机译：氨基-和甲基富勒烯的[6,6]-封闭和[6-5]-开放异构体：与原始C_（60）和（C_（59）N）〜·的比较

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摘要

Two sets of [6-6]-closed and [6-5]-open isomers, namely, those of a methano- and iminofullerene series, are probed in light of their excited state and electron acceptor properties. Steady-state emission, fluorescence, and phosphorescence indicate that the excited-state energy levels of the [6-5]-open (2) and [6-6]-closed (1) iminofullerene isomers follow a seemingly surprising, reverse trend relative to the [6-5]-open (4) and [6-6]-closed (3) methanofullerene isomers. Specifically, the [6-5]-open iminofullerene (2) reveals almost identical characteristics to that of the [6-6]-closed methanofullerene (3). On the other hand the [6-6]-closed iminofullerene (1) is observed to resemble the [6-5]-open methanofullerene (4). Transient absorption spectra, i.e., singlet-singlet, triplet-triplet, and π-radical anion absorption are in accord with the emission studies. These effects have been rationalized in terms of an efficient engagement between the nitrogen electron pair and the fullerene π-system. The [6-5]-open methanofullerene (4) is, therefore, considered to be a true isoelectronic analogue of pristine C_(60) (60 π-electrons). Although the [6-6]-closed iminofullerene (1), constitutes a quasi 60 π-electron system, it appears to bear only a weak resemblance with the former two. In contrast, the [6-6]-closed isomer (3) is characterized by a 58 π-electron system, and the [6-5]-open isomer (2) is characterized by a 62 π-electron system. In terms of optimizing the electron acceptor properties and photostability, the most promising monofunctionalized fullerene derivative for the design of multicomponent donor acceptor arrays is unequivocally the [6-6]-closed iminofullerene (1).
机译：根据它们的激发态和电子受体性质，研究了两组[6-6]-封闭和[6-5]-开放的异构体，即亚甲基富勒烯和亚氨基富勒烯系列的异构体。稳态发射，荧光和磷光表明，[6-5]-开放（2）和[6-6]-封闭（1）亚氨基富勒烯异构体的激发态能级遵循看似令人惊讶的相反趋势相对-[6-5]-开式（4）和[6-6]-开式（3）的甲基富勒烯异构体。具体地，[6-5]-开放的亚氨基富勒烯（2）显示出与[6-6]-封闭的亚甲基富勒烯（3）几乎相同的特征。另一方面，观察到[6-6]-封闭的亚氨基富勒烯（1）类似于[6-5]-开放的亚甲基富勒烯（4）。瞬态吸收光谱，即单重态，三重态和三重态阴离子吸收与发射研究一致。就氮电子对与富勒烯π系统之间的有效结合而言，已合理化了这些效应。因此，认为[6-5]-开的甲基富勒烯（4）是原始C_（60）（60π电子）的真实等电子类似物。尽管[6-6]封闭的亚氨基富勒烯（1）构成了一个近似的60π电子系统，但似乎只与前两者具有微弱的相似性。相反，[6-6]-封闭异构体（3）的特征在于58π电子体系，[6-5]-开放异构体（2）的特征在于62π电子体系。在优化电子受体性能和光稳定性方面，用于设计多组分供体受体阵列的最有前途的单官能化富勒烯衍生物无疑是[6-6]-封闭的亚氨基富勒烯（1）。

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