Thermodynamic Control of Intramolecular Singlet Fission and Exciton Transport in Linear Tetracene Oligomers

Shunta Nakamura, Hayato Sakai, Masaaki Fuki, Rikuto Ooie, Fumitaka Ishiwari, Akinori Saeki, Nikolai V. Tkachenko, Yasuhiro Kobori, Taku Hasobe

Research output: Contribution to journalArticlepeer-review

2 Citations (Scopus)

Abstract

We newly synthesized a series of homo- and hetero-tetracene (Tc) oligomers to propose a molecular design strategy for the efficient exciton transport in linear oligomers by promoting correlated triplet pair (TT) dissociation and controlling sequential exciton trapping process of individual doubled triplet excitons (T+T) by intramolecular singlet fission. First, entropic gain effects on the number of Tc units are examined by comparing Tc-homo-oligomers [(Tc)n: n=2, 4, 6]. Then, a comparison of (Tc)n and Tc-hetero-oligomer [TcF3-(Tc)4-TcF3] reveals the vibronic coupling effect for entropic gain. Observed entropic effects on the T+T formation indicated that the exciton migration is rationalized by number of possible TT states increased both by increasing the number of Tc units and by the vibronic levels at the terminal TcF3 units. Finally, we successfully observed high-yield exciton trapping process (trapped triplet yield: ΦTrT=176 %).

Original languageEnglish
Article numbere202217704
JournalAngewandte Chemie - International Edition
Volume62
Issue number8
DOIs
Publication statusPublished - 2023 Feb 13

Keywords

  • Exciton Transport
  • Oligomers
  • Singlet Fission
  • Tetracene
  • Vibronic Coupling

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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