dc.contributor.author
Maity, Nilabja
dc.contributor.author
Kim, Woojae
dc.contributor.author
Panjwani, Naitik A.
dc.contributor.author
Kundu, Arup
dc.contributor.author
Majumder, Kanad
dc.contributor.author
Kasetty, Pranav
dc.contributor.author
Mishra, Divji
dc.contributor.author
Bittl, Robert
dc.contributor.author
Nagesh, Jayashree
dc.contributor.author
Dasgupta, Jyotishman
dc.date.accessioned
2022-11-11T14:09:14Z
dc.date.available
2022-11-11T14:09:14Z
dc.identifier.uri
https://refubium.fu-berlin.de/handle/fub188/36834
dc.identifier.uri
http://dx.doi.org/10.17169/refubium-36547
dc.description.abstract
Harvesting long-lived free triplets in high yields by utilizing organic singlet fission materials can be the cornerstone for increasing photovoltaic efficiencies potentially. However, except for polyacenes, which are the most studied systems in the singlet fission field, spin-entangled correlated triplet pairs and free triplets born through singlet fission are relatively poorly characterized. By utilizing transient absorption and photoluminescence spectroscopy in supramolecular aggregate thin films consisting of Hamilton-receptor-substituted diketopyrrolopyrrole derivatives, we show that photoexcitation gives rise to the formation of spin-0 correlated triplet pair 1(TT) from the lower Frenkel exciton state. The existence of 1(TT) is proved through faint Herzberg-Teller emission that is enabled by vibronic coupling and correlated with an artifact-free triplet-state photoinduced absorption in the near-infrared. Surprisingly, transient electron paramagnetic resonance reveals that long-lived triplets are produced through classical intersystem crossing instead of 1(TT) dissociation, with the two pathways in competition. Moreover, comparison of the triplet-formation dynamics in J-like and H-like thin films with the same energetics reveals that spin-orbit coupling mediated intersystem crossing persists in both. However, 1(TT) only forms in the J-like film, pinpointing the huge impact of intermolecular coupling geometry on singlet fission dynamics.
en
dc.format.extent
14 Seiten
dc.rights.uri
https://creativecommons.org/licenses/by/4.0/
dc.subject
Energy and society
en
dc.subject
Optics and photonics
en
dc.subject.ddc
500 Naturwissenschaften und Mathematik::540 Chemie::540 Chemie und zugeordnete Wissenschaften
dc.title
Parallel triplet formation pathways in a singlet fission material
dc.type
Wissenschaftlicher Artikel
dcterms.bibliographicCitation.articlenumber
5244
dcterms.bibliographicCitation.doi
10.1038/s41467-022-32844-6
dcterms.bibliographicCitation.journaltitle
Nature Communications
dcterms.bibliographicCitation.volume
13
dcterms.bibliographicCitation.url
https://doi.org/10.1038/s41467-022-32844-6
refubium.affiliation
Physik
refubium.resourceType.isindependentpub
no
dcterms.accessRights.openaire
open access
dcterms.isPartOf.eissn
2041-1723
refubium.resourceType.provider
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