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• W4312214641 endingPage "48599" @default.
• W4312214641 startingPage "48583" @default.
• W4312214641 abstract "A series of π-aromatic-rich cyclometalated ruthenium(II)-(2,2'-bipyridine) complexes ([Ru(bpy)2(πAr-CM)]+) in which πAr-CM is diphenylpyrazine or 1-phenylisoquinoline were prepared. The [Ru(bpy)2(πAr-CM)]+ complexes had remarkably high phosphorescence rate constants, kRAD(p), and the intrinsic phosphorescence efficiencies (ιem(p) = kRAD(p)/(νem(p))3) of these complexes were found to be twice the magnitudes of simply constructed cyclometalated ruthenium(II) complexes ([Ru(bpy)2(sc-CM)]+), where νem(p) is the phosphorescence frequency and sc-CM is 2-phenylpyridine, benzo[h]quinoline, or 2-phenylpyrimidine. Density functional theory (DFT) modeling of the [Ru(bpy)2(CM)]+ complexes indicated numerous singlet metal-to-ligand charge transfers for 1MLCT-(Ru-bpy) and 1MLCT-(Ru-CM), excited states in the low-energy absorption band and 1ππ*-(aromatic ligand) (1ππ*-LAr) excited states in the high-energy band. DFT modeling of these complexes also indicated phosphorescence-emitting state (Te) configurations with primary MLCT-(Ru-bpy) characteristics. The variation in ιem(p) for the spin-forbidden Te (3MLCT-(Ru-bpy)) excited state of the complex system that was examined in this study can be understood through the spin-orbit coupling (SOC)-mediated sum of intensity stealing (∑SOCM-IS) contribution from the primary intensity of the low-energy 1MLCT states and second-order intensity perturbation from the significant configuration between the low-energy 1MLCT and high-energy intense 1ππ*-LAr states. In addition, the observation of unusually high ιem(p) magnitudes for these [Ru(bpy)2(πAr-CM)]+ complexes can be attributed to the values for both intensity factors in the ∑SOCM-IS formalism being individually greater than those for [Ru(bpy)2(sc-CM)]+ ions." @default.
• W4312214641 created "2023-01-04" @default.
• W4312214641 creator A5030122689 @default.
• W4312214641 creator A5051163090 @default.
• W4312214641 creator A5058994610 @default.
• W4312214641 creator A5059605981 @default.
• W4312214641 date "2022-12-14" @default.
• W4312214641 modified "2023-09-26" @default.
• W4312214641 title "High Intrinsic Phosphorescence Efficiency and Density Functional Theory Modeling of Ru(II)-Bipyridine Complexes with π-Aromatic-Rich Cyclometalated Ligands: Attributions of Spin–Orbit Coupling Perturbation and Efficient Configurational Mixing of Singlet Excited States" @default.
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