Steering the multiexciton generation in slip-stacked perylene dye array via exciton coupling

Yongseok Hong, Maximilian Rudolf, Munnyon Kim, Juno Kim, Tim Schembri, Ana-Maria Krause, Kazutaka Shoyama, David Bialas, Merle I. S. Röhr (), Taiha Joo (), Hyungjun Kim (), Dongho Kim () and Frank Würthner ()
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Yongseok Hong: Yonsei University
Maximilian Rudolf: Universitat Würzburg, Institut für Organische Chemie, Am Hubland
Munnyon Kim: Pohang University of Science and Technology (POSTECH)
Juno Kim: Yonsei University
Tim Schembri: Universität Würzburg, Center for Nanosystems Chemistry, Theodor-Boveri Weg
Ana-Maria Krause: Universität Würzburg, Center for Nanosystems Chemistry, Theodor-Boveri Weg
Kazutaka Shoyama: Universität Würzburg, Center for Nanosystems Chemistry, Theodor-Boveri Weg
David Bialas: Universitat Würzburg, Institut für Organische Chemie, Am Hubland
Merle I. S. Röhr: Universität Würzburg, Center for Nanosystems Chemistry, Theodor-Boveri Weg
Taiha Joo: Pohang University of Science and Technology (POSTECH)
Hyungjun Kim: Incheon National University
Dongho Kim: Yonsei University
Frank Würthner: Universitat Würzburg, Institut für Organische Chemie, Am Hubland

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Dye arrays from dimers up to larger oligomers constitute the functional units of natural light harvesting systems as well as organic photonic and photovoltaic materials. Whilst in the past decades many photophysical studies were devoted to molecular dimers for deriving structure-property relationship to unravel the design principles for ideal optoelectronic materials, they fail to accomplish the subsequent processes of charge carrier generation or the detachment of two triplet species in singlet fission (SF). Here, we present a slip-stacked perylene bisimide trimer, which constitutes a bridge between hitherto studied dimer and solid-state materials, to investigate SF mechanisms. This work showcases multiple pathways towards the multiexciton state through direct or excimer-mediated mechanisms by depending upon interchromophoric interaction. These results suggest the comprehensive role of the exciton coupling, exciton delocalization, and excimer state to facilitate the SF process. In this regard, our observations expand the fundamental understanding the structure-property relationship in dye arrays.

Date: 2022
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DOI: 10.1038/s41467-022-31958-1

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