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

Kim, Tae Wu; Jun, Sunhong; Ha, Yoonhoo; Yadav, Rajesh K.; Kumar, Abhishek; Yoo, Chung-Yul; Oh, Inhwan; Lim, Hyung-Kyu; Shin, Jae Won; Ryoo, Ryong; Kim, Hyungjun; Kim, Jeongho; Baeg, Jin-Ook; Ihee, Hyotcherl

doi:10.1038/s41467-019-09872-w

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

Journal Article · Tue Apr 23 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-09872-w· OSTI ID:1624153

^[1]; Jun, Sunhong ^[2]; ^[3]; Yadav, Rajesh K. ^[4]; ^[4]; ^[5]; ^[6]; Lim, Hyung-Kyu ^[7]; Shin, Jae Won ^[2]; Ryoo, Ryong ^[8]; Kim, Hyungjun ^[3]; ^[9]; ^[4]; ^[6]

Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Chemistry; Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). KI for BioCentry; Inst. for Basic Science (IBS), Daejeon (Korea, Republic of). Center for Nanomaterials and Chemical Reactions; DOE/OSTI
Inst. for Basic Science (IBS), Daejeon (Korea, Republic of). Center for Nanomaterials and Chemical Reactions
Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Chemistry
Korea Research Inst. of Chemistry Technology (KRICT), Daejeon (Korea, Republic of). Artificial Photosynthesis Research Group
Korea Inst of Energy Research (KIER), Daejeon (Korea, Republic of)
Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Chemistry; Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). KI for BioCentry; Inst. for Basic Science (IBS), Daejeon (Korea, Republic of). Center for Nanomaterials and Chemical Reactions
Kangwon National Univ., Gangwon-do (Korea, Republic of). Dept. of Chemical Engineering
Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Chemistry; Inst. for Basic Science (IBS), Daejeon (Korea, Republic of). Center for Nanomaterials and Chemical Reactions
Inha Univ., Incheon (Korea, Republic of). Dept. of Chemistry

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

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1624153

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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