Early photophysical events of a ruthenium(ii) molecular dyad capable of performing photochemical water oxidation and of its model compounds

Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology
Francesco NastasiRandolph P Thummel

Abstract

The early photophysical events occurring in the dinuclear metal complex [(ttb-terpy)(I)Ru(μ-dntpz)Ru(bpy)2]3+ (2; ttb-terpy = 4,4',4''-tri-tert-butyl-terpy; bpy = 2,2'-bipyridine; dntpz = 2,5-di-(1,8-dinaphthyrid-2-yl)pyrazine) - a species containing the chromophoric {(bpy)2Ru(μ-dntpz)}2+ subunit and the catalytic {(I)(ttb-terpy)Ru(μ-dntpz)}+ unit, already reported to be able to perform photocatalytic water oxidation - have been studied by ultrafast pump-probe spectroscopy in acetonitrile solution. The model species [Ru(bpy)2(dntpz)]2+ (1), [(bpy)2Ru(μ-dntpz)Ru(bpy)2]4+ (3), and [(ttb-terpy)(I)Ru((μ-dntpz)Ru[(ttb-terpy)(I)]2+ (4) have also been studied. For completeness, the absorption spectra, redox behavior of 1-4 and the spectroelectrochemistry of the dinuclear species 2-4 have been investigated. The usual 3MLCT (metal-to-ligand charge transfer) decay, characterized by relatively long lifetimes on the ns timescale, takes place in 1 and 3, whose lowest-energy level involves a {(bpy)2Ru(dntpz)}2+ unit, whereas for 2 and 4, whose lowest-energy excited state involves a 3MLCT centered on the {(I)(ttb-terpy)Ru(μ-dntpz)}+ subunit, the excited-state lifetimes are on the ps timescale, possibly involving population of a low-lying 3MC ...Continue Reading

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Citations

Jan 13, 2021·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Giovanni BellaMassimiliano Cordaro

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Methods Mentioned

BETA
X-ray

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