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Designing Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates
Author(s) -
Limosani Francesca,
Kaur Ramandeep,
Cataldo Antonino,
Bellucci Stefano,
Micciulla Federico,
Zai Robertino,
Lembo Angelo,
Wang Bingzhe,
Pizzoferrato Roberto,
Guldi Dirk M.,
Tagliatesta Pietro
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202008820
Subject(s) - delocalized electron , electron transfer , photoexcitation , chemistry , context (archaeology) , nanosecond , graphene , ultrafast laser spectroscopy , photochemistry , chemical physics , absorption (acoustics) , materials science , nanotechnology , atomic physics , spectroscopy , organic chemistry , laser , physics , paleontology , quantum mechanics , optics , composite material , biology , excited state
Abstract A novel family of nanocarbon‐based materials was designed, synthesized, and probed within the context of charge‐transfer cascades. We integrated electron‐donating ferrocenes with light‐harvesting/electron‐donating (metallo)porphyrins and electron‐accepting graphene nanoplates (GNP) into multicomponent conjugates. To control the rate of charge flow between the individual building blocks, we bridged them via oligo‐ p ‐phenyleneethynylenes of variable lengths by β‐linkages and the Prato–Maggini reaction. With steady‐state absorption, fluorescence, Raman, and XPS measurements we realized the basic physico‐chemical characterization of the photo‐ and redox‐active components and the multicomponent conjugates. Going beyond this, we performed transient absorption measurements and corroborated by single wavelength and target analyses that the selective (metallo)porphyrin photoexcitation triggers a cascade of charge transfer events, that is, charge separation, charge shift, and charge recombination, to enable the directed charge flow. The net result is a few nanosecond‐lived charge‐separated state featuring a GNP‐delocalized electron and a one‐electron oxidized ferrocenium.