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Time-resolved resonance Raman (TR3) spectra of the emissive and photochemically active metal-to-ligand charge-transfer (MLCT) electronic states of Ru(bpy)32+, Os(bpy)32+, and related complexes are reported. These spectra are compared to those of complexes containing neutril bipyridine and bipyridine radical anion. In the Ru(bpy)32+ complex it is conclusively demonstrated that the realistic formulation of the MLCT state is [RuIII(bpy)2(bpy-?)]2+. This conclusion is reached by four lines of evidence: (i) large frequency shifts in bpy modes in the MLCT state, which approximate those observed upon one-electron chemical reduction of bpy to bpy-?; (ii) the TR3 spectrum observed upon saturation of the MLCT state, which exhibits peaks due to both neutral and radical-like bipyridine; (iii) precise frequencies of “unshifted” bpy modes in the MLCT state, which resemble RuIII(bpy)33+; and (iv) the frequency shifts observed in MLCT states of bis(bipyridine)ruthenium(II) complexes, which are essentially the same as those of the tris chelate. In Os(bpy)32+, criteria ii-iv above have not been successfully tested, but the magnitudes of the large excited state frequency shifts strongly suggest the formulation [OsIII(bpy)2(bpy-?)]2+ for the MLCT state of this complex.
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Reference：
Highly efficient and robust molecular ruthenium catalysts for water oxidation,
Catalysts | Special Issue : Ruthenium Catalysts – MDPI