Synergetic Role of Conformational Flexibility and Electronic Coupling for Quantitative Intramolecular Singlet Fission

Shunta Nakamura, Hayato Sakai, Hiroki Nagashima, Masaaki Fuki, Kakeru Onishi, Ramsha Khan, Yasuhiro Kobori, Nikolai V. Tkachenko, Taku Hasobe

Tutkimustuotos: ArtikkeliScientificvertaisarvioitu

Abstrakti

We present a novel design concept of molecular dimers for quantitative individual triplet yield (φΤ) through intramolecular singlet fission. We synthesized a series of tetracene (Tc) dimers bridged by different phenylene-based linkers, focusing on the conformational flexibility in addition to the electronic coupling. In transient absorption measurements, a 4,4′-biphenyl-bridged Tc dimer with weaker electronic coupling and larger conformational flexibility exhibited the quantitative φΤ: 196 ± 12% at high excitation energy. Moreover, decoupled spins associated with conformational change were directly characterized by time-resolved electron paramagnetic resonance. Strong interplay of the geometry change and electronic localization was revealed on the triplet pair dissociation through magnitudes of spin-spin exchange couplings. Thus, a synergetic role of conformational flexibility and electronic coupling in quantitative φΤ was clarified.

AlkuperäiskieliEnglanti
Sivut18287-18296
Sivumäärä10
JulkaisuJournal of Physical Chemistry C
Vuosikerta125
Numero33
DOI - pysyväislinkit
TilaJulkaistu - 2021
OKM-julkaisutyyppiA1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

Julkaisufoorumi-taso

  • Jufo-taso 2

!!ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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