There is considerable interest in the development of chromophores derived from earth-abundant complexes that yield separable electron–hole pairs for bimolecular chemistry upon irradiation with visible light. However, most complexes of Fe(II) feature lowest energy excited states that are Ligand Field or Metal-Centered in character. Accordingly, these excited states are short lived and are not suitable for separation of electron and hole or bimolecular chemistry. We recently published computational and spectroscopic results on [Fe(tpy)(CN)<sub>3</sub>]<sup>–</sup>, which featured the spectroscopic signatures of an MLCT (Metal-to-Ligand Charge-Transfer) state. We have derivatized the tpy ligand to lower the π* orbital of the accepting ligand to extend the excited state lifetime. In this talk, we will share results from femtosecond to microsecond transient absorption spectroscopy, electrochemical studies, quenching experiments, and DFT calculations. We will use these results to create an electronic structural model demonstrating a long-lived MLCT of Fe(II).

Creation of a long-lived Fe(II) MLCT state for solar driven reactions

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