期刊
NATURE COMMUNICATIONS
卷 10, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-09872-w
关键词
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资金
- Next Generation Carbon Upcycling Project through the National Research Foundation (NRF) - Ministry of Science and ICT, Republic of Korea [2017M1A2A2046736]
- KRICT [2017M1A2A2046736]
- Ministry of Science, ICT and Future Planning (MSIP) through the National Research Foundation of Korea (NRF) [NRF-2015M1A2A2053003]
- Korea Institute of Energy Research (KIER) [B9-2434-03]
- [IBS-R004]
Covalent organic frameworks (COFs) have emerged as a promising light-harvesting module for artificial photosynthesis and photovoltaics. For efficient generation of free charge carriers, the donor-acceptor (D-A) conjugation has been adopted for two-dimensional (2D) COFs recently. In the 2D D-A COFs, photoexcitation would generate a polaron pair, which is a precursor to free charge carriers and has lower binding energy than an exciton. Although the character of the primary excitation species is a key factor in determining optoelectronic properties of a material, excited-state dynamics leading to the creation of a polaron pair have not been investigated yet. Here, we investigate the dynamics of photogenerated charge carriers in 2D D-A COFs by combining femtosecond optical spectroscopy and non-adiabatic molecular dynamics simulation. From this investigation, we elucidate that the polaron pair is formed through ultrafast intra-layer hole transfer coupled with coherent vibrations of the 2D lattice, suggesting a mechanism of phonon-assisted charge transfer.
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