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

Author

Listed:
  • Tae Wu Kim

    (Korea Advanced Institute of Science and Technology (KAIST)
    Korea Advanced Institute of Science and Technology (KAIST)
    Institute for Basic Science (IBS)
    Argonne National Laboratory)

  • Sunhong Jun

    (Institute for Basic Science (IBS)
    Memory Business, Samsung Electronics)

  • 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)
    Korea Advanced Institute of Science and Technology (KAIST)
    Institute for Basic Science (IBS))

  • Hyung-Kyu Lim

    (Kangwon National University)

  • Jae Won Shin

    (Institute for Basic Science (IBS))

  • Ryong Ryoo

    (Korea Advanced Institute of Science and Technology (KAIST)
    Institute for Basic Science (IBS))

  • 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)
    Korea Advanced Institute of Science and Technology (KAIST)
    Institute for Basic Science (IBS))

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.

Suggested Citation

  • 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 & Hyotcherl, 2019. "Ultrafast charge transfer coupled with lattice phonons in two-dimensional covalent organic frameworks," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09872-w
    DOI: 10.1038/s41467-019-09872-w
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    Cited by:

    1. Rengan Luo & Haifeng Lv & Qiaobo Liao & Ningning Wang & Jiarui Yang & Yang Li & Kai Xi & Xiaojun Wu & Huangxian Ju & Jianping Lei, 2021. "Intrareticular charge transfer regulated electrochemiluminescence of donor–acceptor covalent organic frameworks," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Qinying Pan & Mohamed Abdellah & Yuehan Cao & Weihua Lin & Yang Liu & Jie Meng & Quan Zhou & Qian Zhao & Xiaomei Yan & Zonglong Li & Hao Cui & Huili Cao & Wenting Fang & David Ackland Tanner & Mahmoud, 2022. "Ultrafast charge transfer dynamics in 2D covalent organic frameworks/Re-complex hybrid photocatalyst," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    3. Fuyang Liu & Peng Zhou & Yanghui Hou & Hao Tan & Yin Liang & Jialiang Liang & Qing Zhang & Shaojun Guo & Meiping Tong & Jinren Ni, 2023. "Covalent organic frameworks for direct photosynthesis of hydrogen peroxide from water, air and sunlight," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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