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

Research output: Contribution to journalArticlepeer-review

57 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)1084-1090
Number of pages7
JournalNature Materials
Volume18
Issue number10
DOIs
Publication statusPublished - Oct 1 2019

All Science Journal Classification (ASJC) codes

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

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