Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films
Abstract
Singlet fission in organic semiconductors provides an important opportunity to study high-spin states in electronically coupled chromophores. Photoexcitation of oriented, crystalline films of N,N-bis(pentadec-8-yl)terrylene-3,4:11,12-bis(dicarboximide) (TDI) and N,N-bis (pentadec-8-yl)quaterrylene-3,4:13,14-bis(dicarboximide) (QDI) result in the formation of the correlated triplet pair quintet state, 5(T1T1) and its subsequent dissociation into two triplet (T-1) excitons. Time-resolved electron paramagnetic resonance (TREPR) spectroscopy and X-ray crystallography are used to show that the orientation dependence of 5(T1T1) spin dynamics is retained as it dissociates into two T1 excitons, while such information is lost in a randomly oriented sample. In addition, the spin dynamics depend on how the molecules are oriented relative to the external applied magnetic field. Dissociation of 5(T1T1) to form two T1 excitons is more efficient in TDI and leads to a longer T-1 lifetime than in QDI, making TDI a more viable candidate for photovoltaic applications. Since QDI readily forms a highly oriented film, and the lifetime of its 5(T1T1) state is longer than that of TDI, it may be a good candidate for quantum information science applications that require the generation of a quantum- entangled, four-spin state.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Saitama Univ. (Japan)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1635107
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 18; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Bae, Youn Jue, Zhao, Xingang, Kryzaniak, Matthew D., Nagashima, Hiroki, Strzalka, Joseph, Zhang, Qingteng, and Wasielewski, Michael R. Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcc.0c03189.
Bae, Youn Jue, Zhao, Xingang, Kryzaniak, Matthew D., Nagashima, Hiroki, Strzalka, Joseph, Zhang, Qingteng, & Wasielewski, Michael R. Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films. United States. https://doi.org/10.1021/acs.jpcc.0c03189
Bae, Youn Jue, Zhao, Xingang, Kryzaniak, Matthew D., Nagashima, Hiroki, Strzalka, Joseph, Zhang, Qingteng, and Wasielewski, Michael R. Tue .
"Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films". United States. https://doi.org/10.1021/acs.jpcc.0c03189. https://www.osti.gov/servlets/purl/1635107.
@article{osti_1635107,
title = {Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films},
author = {Bae, Youn Jue and Zhao, Xingang and Kryzaniak, Matthew D. and Nagashima, Hiroki and Strzalka, Joseph and Zhang, Qingteng and Wasielewski, Michael R.},
abstractNote = {Singlet fission in organic semiconductors provides an important opportunity to study high-spin states in electronically coupled chromophores. Photoexcitation of oriented, crystalline films of N,N-bis(pentadec-8-yl)terrylene-3,4:11,12-bis(dicarboximide) (TDI) and N,N-bis (pentadec-8-yl)quaterrylene-3,4:13,14-bis(dicarboximide) (QDI) result in the formation of the correlated triplet pair quintet state, 5(T1T1) and its subsequent dissociation into two triplet (T-1) excitons. Time-resolved electron paramagnetic resonance (TREPR) spectroscopy and X-ray crystallography are used to show that the orientation dependence of 5(T1T1) spin dynamics is retained as it dissociates into two T1 excitons, while such information is lost in a randomly oriented sample. In addition, the spin dynamics depend on how the molecules are oriented relative to the external applied magnetic field. Dissociation of 5(T1T1) to form two T1 excitons is more efficient in TDI and leads to a longer T-1 lifetime than in QDI, making TDI a more viable candidate for photovoltaic applications. Since QDI readily forms a highly oriented film, and the lifetime of its 5(T1T1) state is longer than that of TDI, it may be a good candidate for quantum information science applications that require the generation of a quantum- entangled, four-spin state.},
doi = {10.1021/acs.jpcc.0c03189},
journal = {Journal of Physical Chemistry. C},
number = 18,
volume = 124,
place = {United States},
year = {Tue Apr 14 00:00:00 EDT 2020},
month = {Tue Apr 14 00:00:00 EDT 2020}
}
Web of Science
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