A combined spectroscopic and theoretical study on a ruthenium complex featuring a $\pi$-extended dppz ligand for light-driven accumulation of multiple reducing equivalents - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Chemistry - A European Journal Année : 2022

A combined spectroscopic and theoretical study on a ruthenium complex featuring a $\pi$-extended dppz ligand for light-driven accumulation of multiple reducing equivalents

Résumé

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 pi-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.
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Dates et versions

hal-03617666 , version 1 (30-08-2022)

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Carolin Müeller, Alexander Schwab, Nicholas M. Randell, Stephan Kupfer, Benjamin Dietzek-Ivansic, et al.. A combined spectroscopic and theoretical study on a ruthenium complex featuring a $\pi$-extended dppz ligand for light-driven accumulation of multiple reducing equivalents. Chemistry - A European Journal, 2022, 28 (18), pp.e202103882. ⟨10.1002/chem.202103882⟩. ⟨hal-03617666⟩
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