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Kong, Fan-Fang; Tian, Xiao-Jun; Zhang, Yang; Yu, Yun-Jie; Jing, Shi-Hao; Zhang, Yao; Tian, Guang-Jun; Luo, Yi; Yang, Jin-Long; Dong, Zhen-Chao; Hou, J G
Nature communications, 02/2021, Letnik: 12, Številka: 1Journal Article
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.
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