NDLI: Excited State Tuning of Bis(tridentate) Ruthenium(II) Polypyridine Chromophores by Push–Pull Effects and Bite Angle Optimization: A Comprehensive Experimental and Theoretical Study

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Excited State Tuning of Bis(tridentate) Ruthenium(II) Polypyridine Chromophores by Push–Pull Effects and Bite Angle Optimization: A Comprehensive Experimental and Theoretical Study

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Breivogel, Aaron Förster, Christoph Laquai, Frédéric Meister, Michael Heinze, Katja
Description	Author Affiliation: Breivogel A ( Institute of Inorganic Chemistry and Analytical Chemistry, Johannes Gutenberg-University of Mainz, Duesbergweg 10-14, 55128 Mainz (Germany), Fax: (+49) 6131-39-27-277.)
Abstract	The synergy of push–pull substitution and enlarged ligand bite angles has been used in functionalized heteroleptic bis(tridentate) polypyridine complexes of ruthenium(II) to shift the $^{1}MLCT$ absorption and the $^{3}MLCT$ emission to lower energy, enhance the emission quantum yield, and to prolong the $^{3}MLCT$ excited-state lifetime. In these complexes, that is, $[Ru(ddpd)(EtOOC-tpy)][PF_{6}]_{2},$ $[Ru(ddpd-NH_{2})(EtOOC-tpy)][PF_{6}]_{2},$ $[Ru(ddpd)\{(MeOOC)_{3}-tpy\}][PF_{6}]_{2},$ and $[Ru(ddpd-NH_{2})\{(EtOOC)_{3}-tpy\}][PF_{6}]_{2}$ the combination of the electron-accepting 2,2′;6′,2′′-terpyridine (tpy) ligand equipped with one or three COOR substituents with the electron-donating N,N′-dimethyl-N,N′-dipyridin-2-ylpyridine-2,6-diamine (ddpd) ligand decorated with none or one $NH_{2}$ group enforces spatially separated and orthogonal frontier orbitals with a small HOMO–LUMO gap resulting in low-energy $^{1}MLCT$ and $^{3}MLCT$ states. The extended bite angle of the ddpd ligand increases the ligand field splitting and pushes the deactivating $^{3}MC$ state to higher energy. The properties of the new isomerically pure mixed ligand complexes have been studied by using electrochemistry, UV/Vis absorption spectroscopy, static and time-resolved luminescence spectroscopy, and transient absorption spectroscopy. The experimental data were rationalized by using density functional calculations on differently charged species (charge n=0–4) and on triplet excited states $(^{3}MLCT$ and $^{3}MC)$ as well as by time-dependent density functional calculations (excited singlet states).
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	41
Volume Number	19
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2013-10-04
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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