Critical role of intermediate electronic states for spin-flip processes in charge-transfer-type organic molecules with multiple donors and acceptors

Hiroki Noda, Xian Kai Chen, Hajime Nakanotani, Takuya Hosokai, Momoka Miyajima, Naoto Notsuka, Yuuki Kashima, Jean Luc Brédas, Chihaya Adachi

研究成果: ジャーナルへの寄稿記事

2 引用 (Scopus)

抄録

Spin-flip in purely organic molecular systems is often described as a forbidden process; however, it is commonly observed and utilized to harvest triplet excitons in a wide variety of organic material-based applications. Although the initial and final electronic states of spin-flip between the lowest singlet and lowest triplet excited state are self-evident, the exact process and the role of intermediate states through which spin-flip occurs are still far from being comprehensively determined. Here, via experimental photo-physical investigations in solution combined with first-principles quantum-mechanical calculations, we show that efficient spin-flip in multiple donor–acceptor charge-transfer-type organic molecular systems involves the critical role of an intermediate triplet excited state that corresponds to a partial molecular structure of the system. Our proposed mechanism unifies the understanding of the intersystem crossing mechanism in a wide variety of charge-transfer-type molecular systems, opening the way to greater control over spin-flip rates.

元の言語英語
ページ(範囲)1084-1090
ページ数7
ジャーナルNature Materials
18
発行部数10
DOI
出版物ステータス出版済み - 10 1 2019

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Electronic states
Excited states
Charge transfer
charge transfer
Molecules
electronics
Excitons
Molecular structure
molecules
organic materials
excitation
molecular structure
excitons
LDS 751

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering

これを引用

Critical role of intermediate electronic states for spin-flip processes in charge-transfer-type organic molecules with multiple donors and acceptors. / Noda, Hiroki; Chen, Xian Kai; Nakanotani, Hajime; Hosokai, Takuya; Miyajima, Momoka; Notsuka, Naoto; Kashima, Yuuki; Brédas, Jean Luc; Adachi, Chihaya.

:: Nature Materials, 巻 18, 番号 10, 01.10.2019, p. 1084-1090.

研究成果: ジャーナルへの寄稿記事

Noda, Hiroki ; Chen, Xian Kai ; Nakanotani, Hajime ; Hosokai, Takuya ; Miyajima, Momoka ; Notsuka, Naoto ; Kashima, Yuuki ; Brédas, Jean Luc ; Adachi, Chihaya. / Critical role of intermediate electronic states for spin-flip processes in charge-transfer-type organic molecules with multiple donors and acceptors. :: Nature Materials. 2019 ; 巻 18, 番号 10. pp. 1084-1090.
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abstract = "Spin-flip in purely organic molecular systems is often described as a forbidden process; however, it is commonly observed and utilized to harvest triplet excitons in a wide variety of organic material-based applications. Although the initial and final electronic states of spin-flip between the lowest singlet and lowest triplet excited state are self-evident, the exact process and the role of intermediate states through which spin-flip occurs are still far from being comprehensively determined. Here, via experimental photo-physical investigations in solution combined with first-principles quantum-mechanical calculations, we show that efficient spin-flip in multiple donor–acceptor charge-transfer-type organic molecular systems involves the critical role of an intermediate triplet excited state that corresponds to a partial molecular structure of the system. Our proposed mechanism unifies the understanding of the intersystem crossing mechanism in a wide variety of charge-transfer-type molecular systems, opening the way to greater control over spin-flip rates.",
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AU - Noda, Hiroki

AU - Chen, Xian Kai

AU - Nakanotani, Hajime

AU - Hosokai, Takuya

AU - Miyajima, Momoka

AU - Notsuka, Naoto

AU - Kashima, Yuuki

AU - Brédas, Jean Luc

AU - Adachi, Chihaya

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