Abstract
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.
Original language | English |
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Pages (from-to) | 18287-18296 |
Number of pages | 10 |
Journal | Journal of Physical Chemistry C |
Volume | 125 |
Issue number | 33 |
DOIs | |
Publication status | Published - 2021 |
Publication type | A1 Journal article-refereed |
Publication forum classification
- Publication forum level 2
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- General Energy
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films
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