Oxygen-catalysed sequential singlet fission

Nikolaus Wollscheid, J. Luis Pérez Lustres, Oskar Kefer, Sebastian Hahn, Victor Brosius, Uwe H. F. Bunz, Marcus Motzkus () and Tiago Buckup ()
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Nikolaus Wollscheid: Ruprecht-Karls University, Im Neuenheimer Feld 229
J. Luis Pérez Lustres: Ruprecht-Karls University, Im Neuenheimer Feld 229
Oskar Kefer: Ruprecht-Karls University, Im Neuenheimer Feld 229
Sebastian Hahn: University of Heidelberg, Im Neuenheimer Feld 225
Victor Brosius: University of Heidelberg, Im Neuenheimer Feld 225
Uwe H. F. Bunz: University of Heidelberg, Im Neuenheimer Feld 225
Marcus Motzkus: Ruprecht-Karls University, Im Neuenheimer Feld 229
Tiago Buckup: Ruprecht-Karls University, Im Neuenheimer Feld 229

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-13202-5

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