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Probing intramolecular vibronic coupling through vibronic-state imaging

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  • Fan-Fang Kong

    (University of Science and Technology of China)

  • Xiao-Jun Tian

    (University of Science and Technology of China)

  • Yang Zhang

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Yun-Jie Yu

    (University of Science and Technology of China)

  • Shi-Hao Jing

    (University of Science and Technology of China)

  • Yao Zhang

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Guang-Jun Tian

    (Yanshan University)

  • Yi Luo

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Jin-Long Yang

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Zhen-Chao Dong

    (University of Science and Technology of China
    University of Science and Technology of China)

  • J. G. Hou

    (University of Science and Technology of China)

Abstract

Vibronic coupling is a central issue in molecular spectroscopy. Here we investigate vibronic coupling within a single pentacene molecule in real space by imaging the spatial distribution of single-molecule electroluminescence via highly localized excitation of tunneling electrons in a controlled plasmonic junction. The observed two-spot orientation for certain vibronic-state imaging is found to be evidently different from the purely electronic 0–0 transition, rotated by 90°, which reflects the change in the transition dipole orientation from along the molecular short axis to the long axis. Such a change reveals the occurrence of strong vibronic coupling associated with a large Herzberg–Teller contribution, going beyond the conventional Franck–Condon picture. The emergence of large vibration-induced transition charges oscillating along the long axis is found to originate from the strong dynamic perturbation of the anti-symmetric vibration on those carbon atoms with large transition density populations during electronic transitions.

Suggested Citation

  • Fan-Fang Kong & Xiao-Jun Tian & Yang Zhang & Yun-Jie Yu & Shi-Hao Jing & Yao Zhang & Guang-Jun Tian & Yi Luo & Jin-Long Yang & Zhen-Chao Dong & J. G. Hou, 2021. "Probing intramolecular vibronic coupling through vibronic-state imaging," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21571-z
    DOI: 10.1038/s41467-021-21571-z
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    Cited by:

    1. Chao Li & Christoph Kaspar & Ping Zhou & Jung-Ching Liu & Outhmane Chahib & Thilo Glatzel & Robert Häner & Ulrich Aschauer & Silvio Decurtins & Shi-Xia Liu & Michael Thoss & Ernst Meyer & Rémy Pawlak, 2023. "Strong signature of electron-vibration coupling in molecules on Ag(111) triggered by tip-gated discharging," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    2. Vibhuti Rai & Nico Balzer & Gabriel Derenbach & Christof Holzer & Marcel Mayor & Wulf Wulfhekel & Lukas Gerhard & Michal Valášek, 2023. "Hot luminescence from single-molecule chromophores electrically and mechanically self-decoupled by tripodal scaffolds," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Junyuan Liu & Yunhui Zhu & Taiju Tsuboi & Chao Deng & Weiwei Lou & Dan Wang & Tiangeng Liu & Qisheng Zhang, 2022. "Toward a BT.2020 green emitter through a combined multiple resonance effect and multi-lock strategy," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    4. Mingu Kang & Hyunwoo Kim & Elham Oleiki & Yeonjeong Koo & Hyeongwoo Lee & Huitae Joo & Jinseong Choi & Taeyong Eom & Geunsik Lee & Yung Doug Suh & Kyoung-Duck Park, 2022. "Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    5. Yang Luo & Fan-Fang Kong & Xiao-Jun Tian & Yun-Jie Yu & Shi-Hao Jing & Chao Zhang & Gong Chen & Yang Zhang & Yao Zhang & Xiao-Guang Li & Zhen-Yu Zhang & Zhen-Chao Dong, 2024. "Anomalously bright single-molecule upconversion electroluminescence," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

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