Parallel triplet formation pathways in a singlet fission material

Nilabja Maity, Woojae Kim, Naitik A. Panjwani, Arup Kundu, Kanad Majumder, Pranav Kasetty, Divji Mishra, Robert Bittl (), Jayashree Nagesh (), Jyotishman Dasgupta (), Andrew J. Musser () and Satish Patil ()
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Nilabja Maity: Indian Institute of Science
Woojae Kim: Cornell University
Naitik A. Panjwani: Freie Universität Berlin
Arup Kundu: Tata Institute of Fundamental Research
Kanad Majumder: Indian Institute of Science
Pranav Kasetty: Indian Institute of Science
Divji Mishra: Indian Institute of Science
Robert Bittl: Freie Universität Berlin
Jayashree Nagesh: Indian Institute of Science
Jyotishman Dasgupta: Tata Institute of Fundamental Research
Andrew J. Musser: Cornell University
Satish Patil: Indian Institute of Science

Nature Communications, 2022, vol. 13, issue 1, 1-14

Abstract: Abstract Harvesting long-lived free triplets in high yields by utilizing organic singlet fission materials can be the cornerstone for increasing photovoltaic efficiencies potentially. However, except for polyacenes, which are the most studied systems in the singlet fission field, spin-entangled correlated triplet pairs and free triplets born through singlet fission are relatively poorly characterized. By utilizing transient absorption and photoluminescence spectroscopy in supramolecular aggregate thin films consisting of Hamilton-receptor-substituted diketopyrrolopyrrole derivatives, we show that photoexcitation gives rise to the formation of spin-0 correlated triplet pair 1(TT) from the lower Frenkel exciton state. The existence of 1(TT) is proved through faint Herzberg-Teller emission that is enabled by vibronic coupling and correlated with an artifact-free triplet-state photoinduced absorption in the near-infrared. Surprisingly, transient electron paramagnetic resonance reveals that long-lived triplets are produced through classical intersystem crossing instead of 1(TT) dissociation, with the two pathways in competition. Moreover, comparison of the triplet-formation dynamics in J-like and H-like thin films with the same energetics reveals that spin-orbit coupling mediated intersystem crossing persists in both. However, 1(TT) only forms in the J-like film, pinpointing the huge impact of intermolecular coupling geometry on singlet fission dynamics.

Date: 2022
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DOI: 10.1038/s41467-022-32844-6

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