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Jan 08, 2019
Chemistry (Weinheim An Der Bergstrasse, Germany)
Luminescent seven-coordinated zirconium and hafnium complexes bearing three mono-anionic 2,2'-pyridylpyrrolide ligands and one chloride were synthesized. Solid state structures and the dynamic behaviour in solution were probed by X-ray crystallography and variable temperature 1H NMR experiments, respectively. Absorption spectroscopy and time-dependent density functional theory (TD-DFT) calculations supported a hybrid of ligand-to-metal charge transfer (LMCT)/ligand-to-ligand charge transfer (LLCT) for the visible light absorption band. The complexes (MePMPMe)3MCl (M = Zr, Hf, MePMPMe = 3,5-dimethyl-2-(2-pyridyl)pyrrolide) are emissive in solution at room temperature upon irradiation with visible light due to a combination of phosphorescence and fluorescence characterized by excited state lifetimes in the μs and low to sub-ns time-scale, respectively. Electrochemical experiments revealed that the zirconium complex possesses a reversible redox event under highly reducing condition (- 2.29 V vs Fc+/0).

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