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Spectrally Resolved Exciton Polarizability for Understanding Charge Generation in Organic Bulk Hetero-Junction Diodes

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2024, 146, 21, 14724-14733
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    Spectrally Resolved Exciton Polarizability for Understanding Charge Generation in Organic Bulk Hetero-Junction Diodes
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    • Enoch Go
      Enoch Go
      Advanced Photovoltaics Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
      Graduate School of Energy and Environment (KU-KIST GREEN SCHOOL), Korea University, Seoul 02841, Republic of Korea
      More by Enoch Go
    • Hyunjung Jin
      Hyunjung Jin
      Advanced Photovoltaics Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
      Graduate School of Energy and Environment (KU-KIST GREEN SCHOOL), Korea University, Seoul 02841, Republic of Korea
      More by Hyunjung Jin
    • Seongwon Yoon
      Seongwon Yoon
      Advanced Photovoltaics Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
      More by Seongwon Yoon
    • Hyungju Ahn
      Hyungju Ahn
      Pohang Accelerator Laboratory, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
      More by Hyungju Ahn
    • Joonsoo Kim
      Joonsoo Kim
      Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
      More by Joonsoo Kim
    • Chanwoo Lim
      Chanwoo Lim
      Advanced Photovoltaics Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
      More by Chanwoo Lim
    • Ji-Hee Kim
      Ji-Hee Kim
      Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
      Department of Physics, Pusan National University, Busan 46241, Republic of Korea
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      Orcidhttps://orcid.org/0000-0001-7689-4619
    • Haleem Ud Din
      Haleem Ud Din
      Computational Science Research Center, KIST, Seoul 02792, Republic of Korea
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    • Jung-Hoon Lee
      Jung-Hoon Lee
      Computational Science Research Center, KIST, Seoul 02792, Republic of Korea
      More by Jung-Hoon Lee
    • Yongseok Jun
      Yongseok Jun
      Graduate School of Energy and Environment (KU-KIST GREEN SCHOOL), Korea University, Seoul 02841, Republic of Korea
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      Orcidhttps://orcid.org/0000-0003-1463-6723
    • Hyeonggeun Yu*
      Hyeonggeun Yu
      Advanced Photovoltaics Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
      Nanoscience and Technology, KIST School, University of Science and Technology, Seoul 02792, Republic of Korea
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-9125-1320
    • Hae Jung Son*
      Hae Jung Son
      Advanced Photovoltaics Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea
      Graduate School of Energy and Environment (KU-KIST GREEN SCHOOL), Korea University, Seoul 02841, Republic of Korea
      *Email: [email protected]
      More by Hae Jung Son
      Orcidhttps://orcid.org/0000-0002-0912-3483
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 21, 14724–14733
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c02361
    Published May 17, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Despite decades of research, the dominant charge generation mechanism in organic bulk heterojunction (BHJ) devices is not completely understood. While the local dielectric environments of the photoexcited molecules are important for exciton dissociation, conventional characterizations cannot separately measure the polarizability of electron-donor and electron-acceptor, respectively, in their blends, making it difficult to decipher the spectrally different charge generation efficiencies in organic BHJ devices. Here, by spectrally resolved electroabsorption spectroscopy, we report extraction of the excited state polarizability for individual donors and acceptors in a series of organic blend films. Regardless of the donor and acceptor, we discovered that larger exciton polarizability is linked to larger π–π coherence length and faster charge transfer across the heterojunction, which fundamentally explains the origin of the higher charge generation efficiency near 100% in the BHJ photodiodes. We also show that the molecular packing of the donor and acceptor influence each other, resulting in a synergetic enhancement in the exciton polarizability.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.4c02361.

    • Experimental methods; current density–voltage plots for three BHJ photodiodes; contact angles of DI water and ethylene glycol on the IEICO-4F and polymer surfaces; surface energy, solubility parameters, and interaction parameters for various donor polymers and IEICO-4F; EA signals along with the first and second derivatives of device absorbance for each blend; EA fitting parameters; fitting of in-plane and out-of-plane GIWAXS curves for each blend film; reverse-biased IQE for PTB7-Th:IEICO-4F device at different spin-coating rpm; Δp and reverse-biased IQE for PTB7-Th:IEICO-4F and PTB7-Th:IEICO-4Cl devices; calculated interfacial models of PTB7-Th:IEICO-4F and PBDB-T:IEICO-4F; dihedral angles of IEICO-4F with each donor dimer complexes; dihedral angles of donor dimer with IEICO-4F complexes; instrument response function of TA system; built-in potentials for each BHJ blend film; and Supporting Notes 1–4 (calculation of interaction parameters, extraction of spectrally resolved polarizability from EA spectroscopy, fitting parameters from GIWAXS measurements, and computational methods) (PDF)

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    This article is cited by 1 publications.

    1. Sungmin Park, Seongwon Yoon, Hyungju Ahn, Hyeonggeun Yu, Eul-Yong Shin, Kangsik Cho, Yoon Hee Jang, Yongseok Jun, Hae Jung Son. Dielectric additive enables humidity-independent preparation of blend morphology for high-performance, large-area organic photovoltaics. Joule 2025, 9 , 101927. https://doi.org/10.1016/j.joule.2025.101927
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 21, 14724–14733
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c02361
    Published May 17, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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