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.
| Original language | English |
|---|---|
| Article number | 4488 |
| Journal | Nature communications |
| Volume | 13 |
| Issue number | 1 |
| DOIs | |
| Publication status | Published - 2022 Dec |
Bibliographical note
Funding Information:We acknowledge financial support from the Bavarian Ministry of Science and the Arts for the Solar Technology go Hybrid research program and the National Research Foundation of Korea (NRF) through a grant funded by the South Korean government (MEST) (No. 2021R1A2C300630811) (Y.H., J.K., and D.K.) and by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2020R1A5A1019141) (M.K., T. J., and D.K.). The work at Incheon National University was financially supported by the National Research Foundation of Korea (2022R1C1C1010670) and Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (NRF2017R1A6A1A06015181) (H.K.). Quantum mechanical calculations were supported by the National Institute of Supercomputing and Network (NISN)/Korea Institute of Science and Technology Information (KISTI) with needed supercomputing resources, including technical support (KSC-2019-CRE-0201) (Y.H. and D.K.). DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, is acknowledged for providing experimental facilities at PETRA III (proposal No STP-20010322) (M.Ru., T.S., A.-M. K., K.S., D.B., M.R., and F.W.). We thank Johanna Hakanpää for assistance in using beamline P11.
Funding Information:
We acknowledge financial support from the Bavarian Ministry of Science and the Arts for the Solar Technology go Hybrid research program and the National Research Foundation of Korea (NRF) through a grant funded by the South Korean government (MEST) (No. 2021R1A2C300630811) (Y.H., J.K., and D.K.) and by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2020R1A5A1019141) (M.K., T. J., and D.K.). The work at Incheon National University was financially supported by the National Research Foundation of Korea (2022R1C1C1010670) and Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (NRF2017R1A6A1A06015181) (H.K.). Quantum mechanical calculations were supported by the National Institute of Supercomputing and Network (NISN)/Korea Institute of Science and Technology Information (KISTI) with needed supercomputing resources, including technical support (KSC-2019-CRE-0201) (Y.H. and D.K.). DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, is acknowledged for providing experimental facilities at PETRA III (proposal No STP-20010322) (M.Ru., T.S., A.-M. K., K.S., D.B., M.R., and F.W.). We thank Johanna Hakanpää for assistance in using beamline P11.
Publisher Copyright:
© 2022, The Author(s).
All Science Journal Classification (ASJC) codes
- Chemistry(all)
- Biochemistry, Genetics and Molecular Biology(all)
- General
- Physics and Astronomy(all)
