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

Nastasi, Francesco; Santoro, Antonio; Serroni, Scolastica; Campagna, Sebastiano; Kaveevivitchai, Nattawut; Thummel, Randolph P.

doi:10.1039/c8pp00530c

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

Journal Article · Mon Feb 18 00:00:00 EST 2019 · Photochemical & Photobiological Sciences

DOI:https://doi.org/10.1039/c8pp00530c· OSTI ID:1609790

^[1]; Santoro, Antonio ^[2]; Serroni, Scolastica ^[2]; ^[2]; Kaveevivitchai, Nattawut ^[3]; Thummel, Randolph P. ^[3]

University of Messina (Italy); DOE/OSTI
University of Messina (Italy)
Univ. of Houston, TX (United States)

Early events in a water oxidation chromophore-catalyst species are studied; ultrafast energy transfer occurs from the chromThe 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 (metal-centered) level. Compound 2 also exhibits a fast process, with a time constant of 170 fs, which is attributed to intercomponent energy transfer from the MLCT state centered in the {(bpy)₂Ru(μ-dntpz)}²⁺ unit to the MLCT state involving the {(I)(ttb-terpy)Ru(μ-dntpz)}⁺ unit. Both the intercomponent energy transfer and the MLCT-to-MC activation process take place from non-equilibrated MLCT states. ophore to the catalytic unit.

View Accepted Manuscript (DOE)

Research Organization:: University of Houston, TX (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: FG02-07ER15888

OSTI ID:: 1609790

Alternate ID(s):: OSTI ID: 1495836

Journal Information:: Photochemical & Photobiological Sciences, Journal Name: Photochemical & Photobiological Sciences Journal Issue: 9 Vol. 18; ISSN 1474-905X; ISSN PPSHCB

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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