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Published on: September 18, 2019
Singlet Fission among Two Single Molecules
Sumanta Paul1, Oleksandr Yampolskyy1, Zehua Wu1
1Department of Chemistry, Johannes Gutenberg-Universität, Mainz 55128, Germany.
Single molecule spectroscopy reveals complex dynamics in singlet fission (SF). This study quanties the rates of triplet state formation and decay in terrylenediimide dimers, offering new insights into this solar energy conversion process.
Area of Science:
- Photophysical processes
- Materials science
- Spectroscopy
Background:
- Singlet fission (SF) generates two triplet excited states from one singlet excitation, enhancing exciton multiplication for solar energy applications.
- SF typically outcompetes radiative decay, making single-molecule studies challenging.
Purpose of the Study:
- To investigate the mechanistic details of singlet fission at the single-molecule level.
- To analyze the dynamics and heterogeneities of SF in terrylenediimide (TDI) dimers.
Main Methods:
- Single-molecule spectroscopy was employed to study TDI dimers at room and cryogenic temperatures.
- Photon emission streams from individual dimers were analyzed to determine SF rates.
Main Results:
- Static and dynamic heterogeneities in SF rates were observed, indicated by broad rate distributions and fluctuations.
- Delayed fluorescence and occasional rate fluctuations during spin evolution were detected.
- Cryogenic experiments suggested the formation of a coherent multiexciton superposition state.
Conclusions:
- Single-molecule spectroscopy provides a new approach to study SF mechanisms obscured by ensemble averaging.
- The findings offer detailed insights into the complex kinetics and quantum phenomena governing singlet fission.
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