Orbital-resolved observation of singlet fission

Alexander Neef (), Samuel Beaulieu, Sebastian Hammer, Shuo Dong, Julian Maklar, Tommaso Pincelli, R. Patrick Xian, Martin Wolf, Laurenz Rettig, Jens Pflaum and Ralph Ernstorfer ()
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Alexander Neef: Fritz Haber Institute of the Max Planck Society
Samuel Beaulieu: Fritz Haber Institute of the Max Planck Society
Sebastian Hammer: Julius-Maximilian University Wuerzburg
Shuo Dong: Fritz Haber Institute of the Max Planck Society
Julian Maklar: Fritz Haber Institute of the Max Planck Society
Tommaso Pincelli: Fritz Haber Institute of the Max Planck Society
R. Patrick Xian: Fritz Haber Institute of the Max Planck Society
Martin Wolf: Fritz Haber Institute of the Max Planck Society
Laurenz Rettig: Fritz Haber Institute of the Max Planck Society
Jens Pflaum: Julius-Maximilian University Wuerzburg
Ralph Ernstorfer: Fritz Haber Institute of the Max Planck Society

Nature, 2023, vol. 616, issue 7956, 275-279

Abstract: Abstract Singlet fission1–13 may boost photovoltaic efficiency14–16 by transforming a singlet exciton into two triplet excitons and thereby doubling the number of excited charge carriers. The primary step of singlet fission is the ultrafast creation of the correlated triplet pair17. Whereas several mechanisms have been proposed to explain this step, none has emerged as a consensus. The challenge lies in tracking the transient excitonic states. Here we use time- and angle-resolved photoemission spectroscopy to observe the primary step of singlet fission in crystalline pentacene. Our results indicate a charge-transfer mediated mechanism with a hybridization of Frenkel and charge-transfer states in the lowest bright singlet exciton. We gained intimate knowledge about the localization and the orbital character of the exciton wave functions recorded in momentum maps. This allowed us to directly compare the localization of singlet and bitriplet excitons and decompose energetically overlapping states on the basis of their orbital character. Orbital- and localization-resolved many-body dynamics promise deep insights into the mechanics governing molecular systems18–20 and topological materials21–23.

Date: 2023
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DOI: 10.1038/s41586-023-05814-1

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