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Oxygen-catalysed sequential singlet fission

Author

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  • Nikolaus Wollscheid

    (Ruprecht-Karls University, Im Neuenheimer Feld 229
    University of Heidelberg, Im Neuenheimer Feld 225)

  • J. Luis Pérez Lustres

    (Ruprecht-Karls University, Im Neuenheimer Feld 229
    University of Heidelberg, Im Neuenheimer Feld 225)

  • Oskar Kefer

    (Ruprecht-Karls University, Im Neuenheimer Feld 229
    University of Heidelberg, Im Neuenheimer Feld 225)

  • Sebastian Hahn

    (University of Heidelberg, Im Neuenheimer Feld 225
    Ruprecht-Karls University, Im Neuenheimer Feld 270)

  • Victor Brosius

    (University of Heidelberg, Im Neuenheimer Feld 225
    Ruprecht-Karls University, Im Neuenheimer Feld 270)

  • Uwe H. F. Bunz

    (University of Heidelberg, Im Neuenheimer Feld 225
    Ruprecht-Karls University, Im Neuenheimer Feld 270)

  • Marcus Motzkus

    (Ruprecht-Karls University, Im Neuenheimer Feld 229
    University of Heidelberg, Im Neuenheimer Feld 225)

  • Tiago Buckup

    (Ruprecht-Karls University, Im Neuenheimer Feld 229
    University of Heidelberg, Im Neuenheimer Feld 225)

Abstract

Singlet fission is the photoinduced conversion of a singlet exciton into two triplet states of half-energy. This multiplication mechanism has been successfully applied to improve the efficiency of single-junction solar cells in the visible spectral range. Here we show that singlet fission may also occur via a sequential mechanism, where the two triplet states are generated consecutively by exploiting oxygen as a catalyst. This sequential formation of carriers is demonstrated for two acene-like molecules in solution. First, energy transfer from the excited acene to triplet oxygen yields one triplet acene and singlet oxygen. In the second stage, singlet oxygen combines with a ground-state acene to complete singlet fission. This yields a second triplet molecule. The sequential mechanism accounts for approximately 40% of the triplet quantum yield in the studied molecules; this process occurs in dilute solutions and under atmospheric conditions, where the single-step SF mechanism is inactive.

Suggested Citation

  • Nikolaus Wollscheid & J. Luis Pérez Lustres & Oskar Kefer & Sebastian Hahn & Victor Brosius & Uwe H. F. Bunz & Marcus Motzkus & Tiago Buckup, 2019. "Oxygen-catalysed sequential singlet fission," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-13202-5
    DOI: 10.1038/s41467-019-13202-5
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    Cited by:

    1. Stevens, Nicolas & Papavasiliou, Anthony, 2022. "Application of the Level Method for Computing Locational Convex Hull Prices," LIDAM Discussion Papers CORE 2022002, Université catholique de Louvain, Center for Operations Research and Econometrics (CORE).

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