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A Combined Spectroscopic and Theoretical Study on a Ruthenium Complex Featuring a π‐Extended dppz Ligand for Light‐Driven Accumulation of Multiple Reducing Equivalents

The design of photoactive systems capable of storing and relaying multiple electrons is highly demanded in the field of artificial photosynthesis, where transformations of interest rely on multielectronic redox processes. The photophysical properties of the ruthenium photosensitizer [(bpy)(2)Ru(oxim...

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Detalles Bibliográficos
Autores principales: Müller, Carolin, Schwab, Alexander, Randell, Nicholas M., Kupfer, Stephan, Dietzek‐Ivanšić, Benjamin, Chavarot‐Kerlidou, Murielle
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9311760/
https://www.ncbi.nlm.nih.gov/pubmed/35261087
http://dx.doi.org/10.1002/chem.202103882
Descripción
Sumario:The design of photoactive systems capable of storing and relaying multiple electrons is highly demanded in the field of artificial photosynthesis, where transformations of interest rely on multielectronic redox processes. The photophysical properties of the ruthenium photosensitizer [(bpy)(2)Ru(oxim‐dppqp)](2+) (Ru), storing two electrons coupled to two protons on the π‐extended oxim‐dppqp ligand under light‐driven conditions, are investigated by means of excitation wavelength‐dependent resonance Raman and transient absorption spectroscopies, in combination with time‐dependent density functional theory; the results are discussed in comparison to the parent [(bpy)(2)Ru(dppz)](2+) and [(bpy)(2)Ru(oxo‐dppqp)](2+) complexes. In addition, this study provides in‐depth insights on the impact of protonation or of accumulation of multiple reducing equivalents on the reactive excited states.