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Article: Ultrafast Photoinduced Symmetry-Breaking Charge Separation and Electron Sharing in Perylenediimide Molecular Triangles

TitleUltrafast Photoinduced Symmetry-Breaking Charge Separation and Electron Sharing in Perylenediimide Molecular Triangles
Authors
Issue Date2015
Citation
Journal of the American Chemical Society, 2015, v. 137, n. 41, p. 13236-13239 How to Cite?
AbstractWe report on a visible-light-absorbing chiral molecular triangle composed of three covalently linked 1,6,7,12-tetra(phenoxy)perylene-3,4:9,10-bis(dicarboximide) (PDI) units. The rigid triangular architecture reduces the electronic coupling between the PDIs, so ultrafast symmetry-breaking charge separation is kinetically favored over intramolecular excimer formation, as revealed by femtosecond transient absorption spectroscopy. Photoexcitation of the PDI triangle dissolved in CH2Cl2 gives PDI+•-PDI-• in ΔCS = 12.0 ± 0.2 ps. Fast subsequent intramolecular electron/hole hopping can equilibrate the six possible energetically degenerate ion-pair states, as suggested by electron paramagnetic resonance/electron-nuclear double resonance spectroscopy, which shows that one-electron reduction of the PDI triangle results in complete electron sharing among the three PDIs. Charge recombination of PDI+•-PDI-• to the ground state occurs in ΔCR = 1.12 ± 0.01 ns with no evidence of triplet excited state formation.
Persistent Identifierhttp://hdl.handle.net/10722/333689
ISSN
2023 Impact Factor: 14.4
2023 SCImago Journal Rankings: 5.489
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorWu, Yilei-
dc.contributor.authorYoung, Ryan M.-
dc.contributor.authorFrasconi, Marco-
dc.contributor.authorSchneebeli, Severin T.-
dc.contributor.authorSpenst, Peter-
dc.contributor.authorGardner, Daniel M.-
dc.contributor.authorBrown, Kristen E.-
dc.contributor.authorWürthner, Frank-
dc.contributor.authorStoddart, J. Fraser-
dc.contributor.authorWasielewski, Michael R.-
dc.date.accessioned2023-10-06T05:21:37Z-
dc.date.available2023-10-06T05:21:37Z-
dc.date.issued2015-
dc.identifier.citationJournal of the American Chemical Society, 2015, v. 137, n. 41, p. 13236-13239-
dc.identifier.issn0002-7863-
dc.identifier.urihttp://hdl.handle.net/10722/333689-
dc.description.abstractWe report on a visible-light-absorbing chiral molecular triangle composed of three covalently linked 1,6,7,12-tetra(phenoxy)perylene-3,4:9,10-bis(dicarboximide) (PDI) units. The rigid triangular architecture reduces the electronic coupling between the PDIs, so ultrafast symmetry-breaking charge separation is kinetically favored over intramolecular excimer formation, as revealed by femtosecond transient absorption spectroscopy. Photoexcitation of the PDI triangle dissolved in CH2Cl2 gives PDI+•-PDI-• in ΔCS = 12.0 ± 0.2 ps. Fast subsequent intramolecular electron/hole hopping can equilibrate the six possible energetically degenerate ion-pair states, as suggested by electron paramagnetic resonance/electron-nuclear double resonance spectroscopy, which shows that one-electron reduction of the PDI triangle results in complete electron sharing among the three PDIs. Charge recombination of PDI+•-PDI-• to the ground state occurs in ΔCR = 1.12 ± 0.01 ns with no evidence of triplet excited state formation.-
dc.languageeng-
dc.relation.ispartofJournal of the American Chemical Society-
dc.titleUltrafast Photoinduced Symmetry-Breaking Charge Separation and Electron Sharing in Perylenediimide Molecular Triangles-
dc.typeArticle-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1021/jacs.5b08386-
dc.identifier.pmid26418462-
dc.identifier.scopuseid_2-s2.0-84945288416-
dc.identifier.volume137-
dc.identifier.issue41-
dc.identifier.spage13236-
dc.identifier.epage13239-
dc.identifier.eissn1520-5126-
dc.identifier.isiWOS:000363438600007-

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