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- W2032536157 abstract "Transient 1:1 precursor complexes for intermolecular self-exchange between various organic electron donors (D) and their paramagnetic cation radicals (D+*), as well as between different electron acceptors (A) paired with their anion radicals (A-*), are spectrally (UV-NIR) observed and structurally (X-ray) identified as the cofacial (pi-stacked) associates [D, D+*] and [A-*, A], respectively. Mulliken-Hush (two-state) analysis of their diagnostic intervalence bands affords the electronic coupling elements (HDA), which together with the Marcus reorganization energies (lambda) from the NIR spectral data are confirmed by molecular-orbital computations. The HDA values are found to be a sensitive function of the bulky substituents surrounding the redox centers. As a result, the steric modulation of the donor/acceptor separation (rDA) leads to distinctive electron-transfer rates between sterically hindered donors/acceptors and their more open (unsubstituted) parents. The latter is discussed in the context of a continuous series of outer- and inner-sphere mechanisms for organic electron-transfer processes in a manner originally formulated by Taube and co-workers for inorganic (coordination) donor/acceptor dyads-with conciliatory attention paid to traditional organic versus inorganic concepts." @default.
- W2032536157 created "2016-06-24" @default.
- W2032536157 creator A5030343286 @default.
- W2032536157 creator A5091859622 @default.
- W2032536157 date "2007-03-01" @default.
- W2032536157 modified "2023-09-23" @default.
- W2032536157 title "Continuum of Outer- and Inner-Sphere Mechanisms for Organic Electron Transfer. Steric Modulation of the Precursor Complex in Paramagnetic (Ion-Radical) Self-Exchanges" @default.
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- W2032536157 doi "https://doi.org/10.1021/ja069149m" @default.
- W2032536157 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/17338527" @default.
- W2032536157 hasPublicationYear "2007" @default.
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