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- W2810065470 abstract "Various modern solar light-harvesting systems, including those used in photovoltaics and solar fuel production, depend on efficient electron transfer from a surface-bound molecular dye to nanoscopic semiconductor particles. However, the productive electron transfer competes with a variety of other relaxation pathways for the dye, and the dominant pathway can change dramatically depending on its environment. A new sulfur-substituted thiorhodamine dye was synthesized having exceptional light-harvesting qualities for solar energy applications and for solar hydrogen production in particular. The dye was created with a thiophene spacer bearing a phosphonate-ester (1-Ester) or phosphonic-acid (1-Acid) allowing for excellent solubility in MeCN or the ability to functionalize metal oxide semiconductor nanoparticles such as TiO2. While 1-Ester is found to be fully monomeric in MeCN, 1-Acid readily forms H-aggregated dimers which, upon photoexcitation, undergo charge separation to an ion pair (IP) in 1.5 ps. For 1-Acid dimers, the stabilization of the IP causes an increase in lifetime to 270 ps compared to the 75 ps lifetime of the monomer. When 1-Acid is attached to TiO2, the inhomogeneous surface creates a distribution of chromophore packing structures where a range of transition dipole coupling environments is present such that both excimers and IPs can form. In a variety of solvent environments, ultrafast electron injection was found to occur in <300 fs from the dye to the semiconductor while IP formation occurs in 2–4 ps. For all aggregates studied, the photophysics was the same whether pumped at 620 nm, exciting to the 0–0 absorption band, or at 565 nm to the 0–1 transition that is dramatically enhanced by transition-dipole coupling in the H-aggregate. Surprisingly, the long-time, >2 ns, persistent formation of the charge-separated state following charge injection to TiO2 only accounts for ∼10% of the photoexcited population, with the dominant relaxation pathways being IP and excimer formation. IP and excimer formation lower the total energy of the aggregate below the conduction band edge of TiO2, deactivating the electron transfer process. The implications of IP and excimer formation in systems for solar light harvesting are discussed." @default.
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- W2810065470 date "2018-06-27" @default.
- W2810065470 modified "2023-10-16" @default.
- W2810065470 title "Intermolecular Charge Separation in Aggregated Rhodamine Dyes Used in Solar Hydrogen Production" @default.
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- W2810065470 doi "https://doi.org/10.1021/acs.jpcc.8b03045" @default.
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