Ultrafast charge transfer coupled with lattice phonons in two-dimensional covalent organic frameworks

Tae Wu Kim, Sunhong Jun, Yoonhoo Ha, Rajesh K. Yadav, Abhishek Kumar, Chung-Yul Yoo, Inhwan Oh, Hyung-Kyu Lim, Jae Won Shin, Ryong Ryoo, Hyungjun Kim (), Jeongho Kim (), Jin-Ook Baeg () and Hyotcherl Ihee ()
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Tae Wu Kim: Korea Advanced Institute of Science and Technology (KAIST)
Sunhong Jun: Institute for Basic Science (IBS)
Yoonhoo Ha: Korea Advanced Institute of Science and Technology (KAIST)
Rajesh K. Yadav: Korea Research Institute of Chemical Technology (KRICT)
Abhishek Kumar: Korea Research Institute of Chemical Technology (KRICT)
Chung-Yul Yoo: Korea Institute of Energy Research (KIER)
Inhwan Oh: Korea Advanced Institute of Science and Technology (KAIST)
Hyung-Kyu Lim: Kangwon National University
Jae Won Shin: Institute for Basic Science (IBS)
Ryong Ryoo: Korea Advanced Institute of Science and Technology (KAIST)
Hyungjun Kim: Korea Advanced Institute of Science and Technology (KAIST)
Jeongho Kim: Inha University
Jin-Ook Baeg: Korea Research Institute of Chemical Technology (KRICT)
Hyotcherl Ihee: Korea Advanced Institute of Science and Technology (KAIST)

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract 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.

Date: 2019
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DOI: 10.1038/s41467-019-09872-w

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