期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 15, 页码 8125-8136出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c10171
关键词
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资金
- European Research Council under the European Union's Horizon 2020 research and innovation programme [817494]
- Volkswagenstiftung [93404]
- Deutsche Forschungs gemeinschaft (DFG) [ZA 638/7, FL 834/2-2, FL 834/5-1, FL 834/7-1]
- European Research Council (ERC) [817494] Funding Source: European Research Council (ERC)
This study demonstrates charge transfer from photoexcited narrow bandgap SWCNTs to wide bandgap PFO-BPy, providing new pathways for charge separation in SWCNT-based photodetectors and photovoltaic cells.
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 E, transition but also by the energetically unfavorable E-22 excitation under high pump fluence. This unusual PCT from narrowbandgap SWCNTs toward a wide-bandgap polymer originates from the up-converted high-energy excitonic state (E-33 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.
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