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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Analysis of charge-transfer absorption and emission spectra on an absolute scale: Evaluation of free energies, matrix elements, and reorganization energies
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Analysis of charge-transfer absorption and emission spectra on an absolute scale: Evaluation of free energies, matrix elements, and reorganization energies

机译：绝对尺度上的电荷转移吸收和发射光谱分析：自由能，基质元素和重组能的评估

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摘要

The relationship between the absorption and emission spectra of the charge-transfer complexes formed between a series of methyl-substituted benzene donors with 1,2,4,5-tetracyanobenzene as acceptor in 1,2-dichloroethane was examined in detail. The association constants for charge-transfer complex formation and the emission quantum yields for these complexes were used to place the experimental absorption and emission spectra on absolute scales. The simultaneous analysis of these spectra is valid only when the Mulliken two-state model is justified. For several of the complexes included in this study the electron-transfer parameters, including the electronic coupling matrix elements, obtained from the analysis of the individual absorption and emission spectra are in close agreement. The simultaneous analysis of the combined absorption and emission spectra leads to a well-defined set of electron-transfer parameters for these complexes. In other complexes, where the two-state model does not apply because of the influence of localized excited states on the absorption spectrum, analysis of the absorption and emission spectra led to significantly different sets of electron-transfer parameters. It is demonstrated that the electronic coupling matrix elements are a very sensitive indicator of the influence of localized excited states on these spectra.
机译：详细研究了由1,2,4,5-四氰基苯作为受体的一系列甲基取代的苯供体在1,2-二氯乙烷中形成的电荷转移配合物的吸收和发射光谱之间的关系。电荷转移配合物形成的缔合常数和这些配合物的发射量子产率用于将实验吸收光谱和发射光谱置于绝对尺度上。仅当Mulliken两态模型合理时，对这些光谱的同时分析才有效。对于本研究中包括的几种配合物，通过分析单个吸收光谱和发射光谱获得的电子传递参数（包括电子耦合基质元素）非常一致。同时分析吸收光谱和发射光谱可以得出这些配合物的一组明确定义的电子转移参数。在其他配合物中，由于局部激发态对吸收光谱的影响而无法使用二态模型，对吸收光谱和发射光谱的分析导致了电子转移参数的显着不同。证明了电子耦合矩阵元件是局部激发态对这些光谱的影响的非常敏感的指示。

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