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 |
| 巻 | 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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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
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TY - JOUR
T1 - Critical role of intermediate electronic states for spin-flip processes in charge-transfer-type organic molecules with multiple donors and acceptors
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
PY - 2019/10/1
Y1 - 2019/10/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85072185706&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85072185706&partnerID=8YFLogxK
U2 - 10.1038/s41563-019-0465-6
DO - 10.1038/s41563-019-0465-6
M3 - Article
C2 - 31477903
AN - SCOPUS:85072185706
VL - 18
SP - 1084
EP - 1090
JO - Nature Materials
JF - Nature Materials
SN - 1476-1122
IS - 10
ER -