2017年10月1日
Coherent singlet fission activated by symmetry breaking
Nature Chemistry
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- 巻
- 9
- 号
- 10
- 開始ページ
- 983
- 終了ページ
- 989
- 記述言語
- 英語
- 掲載種別
- 研究論文(学術雑誌)
- DOI
- 10.1038/nchem.2784
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved. Singlet fission, in which a singlet exciton is converted to two triplet excitons, is a process that could be beneficial in photovoltaic applications. A full understanding of the dynamics of singlet fission in molecular systems requires detailed knowledge of the relevant potential energy surfaces and their (conical) intersections. However, obtaining such information is a nontrivial task, particularly for molecular aggregates. Here we investigate singlet fission in rubrene crystals using transient absorption spectroscopy and state-of-the-art quantum chemical calculations. We observe a coherent and ultrafast singlet-fission channel as well as the well-known and conventional thermally assisted incoherent channel. This coherent channel is accessible because the conical intersection for singlet fission on the excited-state potential energy surface is located very close to the equilibrium position of the ground-state potential energy surface and also because of the excitation of an intermolecular symmetry-breaking mode, which activates the electronic coupling necessary for singlet fission.
- リンク情報
- ID情報
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- DOI : 10.1038/nchem.2784
- ISSN : 1755-4330
- eISSN : 1755-4349
- PubMed ID : 28937675
- SCOPUS ID : 85029762307