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The Excited‐State Creutz–Taube Ion

German E. Pieslinger, Ivana Ramírez‐Wierzbicki, Alejandro Cadranel

2022Angewandte Chemie International Edition22 citationsDOIOpen Access PDF

Abstract

Abstract The excited‐state version of the Creutz–Taube ion was prepared via visible light excitation of [(NH 3 ) 5 Ru II ( μ ‐pz)Ru II (NH 3 ) 5 ] 4+ . The resulting excited state is a mixed valence {Ru III–δ ( μ ‐pz⋅ − )Ru II+δ } transient species, which was characterized using femtosecond transient absorption spectroscopy with vis‐NIR detection. Very intense photoinduced intervalence charge transfers were observed at 7500 cm −1 , revealing an excited‐state electronic coupling element H DA =3750 cm −1 . DFT calculations confirm a strongly delocalized excited state. A notable consequence of strong electron delocalization is the nanosecond excited state lifetime, which was exploited in a proof‐of‐concept intermolecular electron transfer. The excited‐state Creutz–Taube ion is established as a reference, and demonstrates that electron delocalization in the excited state can be leveraged for artificial photosynthesis or other photocatalytic schemes based on electron transfer chemistry.

Topics & Concepts

Excited stateDelocalized electronIonUltrafast laser spectroscopyAtomic physicsNanosecondChemistryElectron transferSpectroscopyValence (chemistry)PhotochemistryPhysicsLaserQuantum mechanicsOpticsOrganic chemistryPhotochemistry and Electron Transfer StudiesMetal-Catalyzed Oxygenation MechanismsPorphyrin and Phthalocyanine Chemistry
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