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Three symmetric Mo2 dimers [Mo2(DAniF)3](μ-E2CCE2)[Mo2(DAniF)3] (DAniF = N,N′-di(p-anisyl)formamidinate) with oxalate (E = O) or the thiolated derivatives (E = O or S) as bridging ligands have been synthesized, and the optical properties of the mixed-valence (MV) derivatives obtained by one-electron oxidation studied within the framework of the vibronic two-state model. These Mo2–Mo2 systems are effective models for testing electron transfer theories, with the δ electrons of the Mo2 fragments that are responsible for the redox and optical properties of the MV complex being well isolated from other metal d and ligand π-type orbitals. This in turn gives rise to unique, well-resolved metal to ligand (MLCT) and intervalence charge transfer (IVCT) absorption bands that permit accurate analyses based on band shape. In the series [Mo2(DAniF)3](μ-E2CCE2)[Mo2(DAniF)3], the extent of electron delocalization between the Mo2 cores increases with increasing number of sulfur atoms, E, in the bridge. Higher-energy IVCT ...

the journal of physical chemistry c

Optical Behaviors and Electronic Properties of Mo<sub>2</sub>–Mo<sub>2</sub> Mixed-Valence Complexes within or beyond the Class III Regime: Testing the Limits of the Two-State Model

Optical Behaviors and Electronic Properties of Mo2–Mo2 Mixed-Valence Complexes within or beyond the Class III Regime: Testing the Limits of the Two-State Model

Optical Behaviors and Electronic Properties of Mo₂–Mo₂ Mixed-Valence Complexes within or beyond the Class III Regime: Testing the Limits of the Two-State Model