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• W4311607471 startingPage "70" @default.
• W4311607471 abstract "Charge-transfer dynamics and interligand electron transfer (ILET) phenomena play a pivotal role in dye-sensitizers, mostly represented by the Ru-based polypyridyl complexes, for TiO2 and ZnO-based solar cells. Starting from metal-to-ligand charge-transfer (MLCT) excited states, charge dynamics and ILET can influence the overall device efficiency. In this letter, we focus on N34- dye ( [Ru(dcbpy)2(NCS)2]4-, dcbpy = 4,4'-dicarboxy-2,2'-bipyridine) to provide a first direct observation with high time resolution (<20 fs) of the ultrafast electron exchange between bpy-like ligands. ILET is observed in water solution after photoexcitation in the ∼400 nm MLCT band, and assessment of its ultrafast time-scale is here given through a real-time electronic dynamics simulation on the basis of state-of-the-art electronic structure methods. Indirect effects of water at finite temperature are also disentangled by investigating the system in a symmetric gas-phase structure. As main result, remarkably, the ILET mechanism appears to be based upon a purely electronic evolution among the dense, experimentally accessible, MLCT excited states manifold at ∼400 nm, which rules out nuclear-electronic couplings and proves further the importance of the dense electronic manifold in improving the efficiency of dye sensitizers in solar cell devices." @default.
• W4311607471 created "2022-12-27" @default.
• W4311607471 creator A5009916566 @default.
• W4311607471 creator A5018498770 @default.
• W4311607471 creator A5021996885 @default.
• W4311607471 creator A5030929196 @default.
• W4311607471 date "2022-12-15" @default.
• W4311607471 modified "2023-10-18" @default.
• W4311607471 title "Nature of the Ultrafast Interligands Electron Transfers in Dye-Sensitized Solar Cells" @default.
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