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Charge transfer from photoexcited semiconducting single-walled carbon nanotubes to wide-bandgap wrapping polymer

As narrow optical bandgap materials, semiconducting single-walled carbon nanotubes (SWCNTs) are rarely regarded as charge donors in photoinduced charge-transfer (PCT) reactions. However, the unique band structure and unusual exciton dynamics of SWCNTs add more possibilities to the classical PCT mech...

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Main Authors: Kuang, Zhuoran (Author) , Berger, Felix J. (Author) , Pérez Lustres, José Luis (Author) , Wollscheid, Nikolaus (Author) , Li, Han (Author) , Lüttgens, Jan (Author) , Leinen, Merve (Author) , Flavel, Benjamin S. (Author) , Zaumseil, Jana (Author) , Buckup, Tiago (Author)
Format: Article (Journal)
Language:English
Published: April 14, 2021
In: The journal of physical chemistry. C, Energy, materials, and catalysis
Year: 2021, Volume: 125, Issue: 15, Pages: 8125-8136
ISSN:1932-7455
DOI:10.1021/acs.jpcc.0c10171
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.jpcc.0c10171
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Author Notes:Zhuoran Kuang, Felix J. Berger, Jose Luis Pérez Lustres, Nikolaus Wollscheid, Han Li, Jan Lüttgens, Merve Balcı Leinen, Benjamin S. Flavel, Jana Zaumseil, and Tiago Buckup
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Summary:As narrow optical bandgap materials, semiconducting single-walled carbon nanotubes (SWCNTs) are rarely regarded as charge donors in photoinduced charge-transfer (PCT) reactions. However, the unique band structure and unusual exciton dynamics of SWCNTs add more possibilities to the classical PCT mechanism. In this work, we demonstrate PCT from photoexcited semiconducting (6,5) SWCNTs to a wide-bandgap wrapping poly-[(9,9-dioctylfluorenyl-2,7-diyl)-alt-(6,6′)-(2,2′-bipyridine)] (PFO-BPy) via femtosecond transient absorption spectroscopy. By monitoring the spectral dynamics of the SWCNT polaron, we show that charge transfer from photoexcited SWCNTs to PFO-BPy can be driven not only by the energetically favorable E33 transition but also by the energetically unfavorable E22 excitation under high pump fluence. This unusual PCT from narrow-bandgap SWCNTs toward a wide-bandgap polymer originates from the up-converted high-energy excitonic state (E33 or higher) that is promoted by the Auger recombination of excitons and charge carriers in SWCNTs. These insights provide new pathways for charge separation in SWCNT-based photodetectors and photovoltaic cells.
Item Description:Gesehen am 25.06.2021
Physical Description:Online Resource
ISSN:1932-7455
DOI:10.1021/acs.jpcc.0c10171

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