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

研究成果: Article査読

4 被引用数 (Scopus)

抄録

We present a novel design concept of molecular dimers for quantitative individual triplet yield (φT) 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 φT: 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 φT was clarified.

本文言語English
ページ(範囲)18287-18296
ページ数10
ジャーナルJournal of Physical Chemistry C
125
33
DOI
出版ステータスPublished - 2021 8月 26

ASJC Scopus subject areas

  • 電子材料、光学材料、および磁性材料
  • エネルギー(全般)
  • 物理化学および理論化学
  • 表面、皮膜および薄膜

フィンガープリント

「Synergetic Role of Conformational Flexibility and Electronic Coupling for Quantitative Intramolecular Singlet Fission」の研究トピックを掘り下げます。これらがまとまってユニークなフィンガープリントを構成します。

引用スタイル