Abstract
By using gas-phase ultraviolet photoelectron spectroscopy, vis/NIR spectroscopy, and electronic-structure calculations, we have investigated the electron-vibration and electronic interactions in a series of bisdimethylamino mixed-valence systems: N,N,N′,N′-tetramethyl-p-phenylenediamine, N,N,N′,N′-tetramethylbenzidine, and N,N,N′,N′-tetramethyltolane-4,4′-diamine. Experiment and theory concur to indicate that the electron-vibration coupling in these systems is dominated by interactions with symmetric modes. The results reveal that the strength of both electronic and electron-vibration couplings decreases as the molecular bridge lengthens. The parameters derived for the present compounds have been compared to those of diarylamino-based structural analogs. This comparison underlines that the replacement of the methyl terminal groups with p-anisyl groups has a significant effect on the electronic and electron-vibrational interactions.
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