Probing intramolecular vibronic coupling through vibronic-state imaging

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 () and J. G. Hou
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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
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
Guang-Jun Tian: Yanshan University
Yi Luo: University of Science and Technology of China
Jin-Long Yang: University of Science and Technology of China
Zhen-Chao Dong: University of Science and Technology of China
J. G. Hou: University of Science and Technology of China

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-21571-z

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