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- W1523797505 abstract "Initial steps in the photodissociation of nitrosyl ferrous and ferric heme complexes have been investigated by calculation of the ground and excited states and electronic spectra as a function of iron-ligand bond lengthening. The method used is an all valence semi empirical INDO-SCF-CI procedure with transition metal parameterization and the ability to calculate configuration interaction for closed shell systems and, more recently, radical species. The results of these studies allow identification of a common photodissociating state involving dπ → d*z2 excitations for both systems, the same state found in previous studies of carbonyl and oxy ferrous heme complexes. This result is consistent with the observation of nearly equal initial photodissociation product for all four systems at a picosecond time scale. The low quantum yield at long time (~ 400 µs) observed for the ferrous nitrosyl complex is attributed to the population of charge transfer states with a minimum which allow trapping of the NO radical near the iron. Such states can be involved in both rapid geminate recombination or energy decay to the liganded state. The high quantum yield of the ferric nitrosyl complex is attributed to eventual photodissociation of ferric heme and NO radical on a triplet surface which does not allow population of the low energy charge transfer states also found to be present for these system. By contrast, the high quantum yield of the isoelectronic ferrous carbonyl heme complex is associated with the absence of such charge transfer states." @default.
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- W1523797505 date "1986-10-15" @default.
- W1523797505 modified "2023-10-18" @default.
- W1523797505 title "Porphyrins" @default.
- W1523797505 doi "https://doi.org/10.1021/bk-1986-0321" @default.
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