Abstract
Time-resolved IR spectroscopy and density functional theory calculations indicate that the 14-electron, triplet species, 3Fe(CO)3, generated from photolysis of Fe(CO)5, appears to exist uncoordinated to alkyl groups in alkane solvents. In alcohols of varying lengths, triplet 3Fe(CO)3 forms a hydroxyl-coordinated complex on the time scale of tens of picoseconds, implying that its solvation kinetics are diffusion-limited. Surprisingly, the hydroxyl-coordinated complex remains in a triplet state, in contrast to the activity of triplet 3Fe(CO)4, which must convert to a singlet state to coordinate to a solvent molecule. To our knowledge, this study represents the first investigation into the detailed metal–solvent interactions and rearrangement kinetics of a 14-electron complex on the ultrafast time scale.
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