Abstract
The solvation dynamics for deoxygenated and oxygenated Vaska’s complex, bis(triphenylphosphene) iridium(I) carbonyl chloride, (deoxy-VC and oxy-VC) were characterized using two-dimensional infrared (2D-IR) spectroscopy in d6-benzene, chloroform, and DMF. The iridium-bound carbonyl was used as a probe of the static and dynamic chemical environments in each solvent system. The linear IR spectra of the complexes were consistent with CO frequency modulation through d−π* backbonding interactions. The deoxy-VC center frequencies were insensitive to the solvent type, but those of oxy-VC were sensitive to the surrounding solvent, presumably due to the indirect influence of the dioxygen ligand on the carbonyl vibrational frequency. The vibrational lifetimes of the VC carbonyls were consistent with intramolecular relaxation through the metal d–π orbitals. 2D-IR spectra were analyzed using the inverse centerline slope (CLS) as a representative of the normalized frequency–frequency correlation function. Multiexponent...
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