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- W2801197748 endingPage "7186" @default.
- W2801197748 startingPage "7176" @default.
- W2801197748 abstract "The electrochemical and spectroscopic properties of eight bis(tridentate) cyclometalated RuII compounds covalently linked by a phenyl- or xylyl-thiophene bridge to a pendant triphenylamine (TPA) were characterized in fluid solution and immobilized on metal oxide surfaces. Upon surface immobilization, the TPA+/0 reduction potentials of the phenyl-bridged compounds exhibited large changes, ±100 mV, relative to solution-based values, yet those observed for the xylyl-bridged compounds were relatively unchanged. The highest occupied molecular orbital of the surface-immobilized compounds was associated with either TPA or RuII, enabling the study of the electron transfer in opposite directions. Electron transfer in the mixed-valent states of the compounds was found to proceed by different optical pathways for RuII → TPA+ relative to TPA → RuIII. Mulliken-Hush analysis of intervalence charge transfer bands for the phenyl-bridged compounds revealed that the electronic coupling matrix element, HDA, was ∼950 cm-1 for RuII → TPA+, while HDA for TPA → RuIII appeared to be 2500 cm-1. In contrast, the xylyl-bridged compounds were weakly coupled. A superexchange analysis, where unoccupied bridge orbitals were taken directly into account, led to a very different conclusion: HDA did not depend on the charge-transfer direction or path. The results imply that the electron-transfer direction can alter optical charge transfer pathways without influencing the electronic coupling." @default.
- W2801197748 created "2018-05-17" @default.
- W2801197748 creator A5006832213 @default.
- W2801197748 creator A5025530595 @default.
- W2801197748 creator A5028005131 @default.
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- W2801197748 creator A5050580371 @default.
- W2801197748 creator A5073119387 @default.
- W2801197748 creator A5078264149 @default.
- W2801197748 date "2018-05-07" @default.
- W2801197748 modified "2023-09-29" @default.
- W2801197748 title "Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways" @default.
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- W2801197748 doi "https://doi.org/10.1021/jacs.8b02715" @default.
- W2801197748 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/29733590" @default.