Doubly resonant sum frequency generation (DR-SFG) serves as a potent characteristic technique for probing the electronic spectra and vibronic coupling of molecules on surfaces. In this study, we successfully developed a novel infrared (IR)–white light (WL) DR-SFG spectroscopy based on narrowband IR and tunable broadband WL. This novel method was employed to explore the excitation spectrum and vibronic couplings of sub-monolayer Rhodamine 6G molecules. Our findings elucidate that the xanthene skeleton vibrational modes exhibit strong coupling with the S0–S1 electronic transition. Notably, we observed not only the 0–0 transition of the S0–S1 electronic continuum but also the 0–1 transition, a first time observation in the realm of DR-SFG spectroscopy. This advanced DR-SFG spectroscopy methodology facilitates a more sensitive examination of electronic spectra and the coupling between electronic transitions and vibrational modes, heralding a significant advancement in the understanding of molecular interactions on surfaces.
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Vibronic coupling of Rhodamine 6G molecules studied by doubly resonant sum frequency generation spectroscopy with narrowband infrared and broadband visible
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14 January 2024
Research Article|
January 11 2024
Vibronic coupling of Rhodamine 6G molecules studied by doubly resonant sum frequency generation spectroscopy with narrowband infrared and broadband visible
Special Collection:
Recent Developments in Nonlinear Optics at Interfaces
Wei-Wang Zeng (曾维旺)
;
Wei-Wang Zeng (曾维旺)
(Conceptualization, Data curation, Formal analysis, Writing – original draft, Writing – review & editing)
1
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
, 457 Zhongshan Road, Dalian 116023, People’s Republic of China
2
University of Chinese Academy of Sciences
, 19A Yuquan Road, Beijing 100049, People’s Republic of China
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Ting Luo (罗婷);
Ting Luo (罗婷)
(Formal analysis)
1
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
, 457 Zhongshan Road, Dalian 116023, People’s Republic of China
3
Research Center for Industries of the Future and School of Engineering, Westlake University
, Hangzhou 310030, People’s Republic of China
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Peng Xu (徐鹏);
Peng Xu (徐鹏)
(Data curation, Formal analysis)
1
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
, 457 Zhongshan Road, Dalian 116023, People’s Republic of China
4
Department of Chemical Physics, University of Science and Technology of China
, Hefei 230026, People’s Republic of China
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Chuanyao Zhou (周传耀)
;
Chuanyao Zhou (周传耀)
(Writing – review & editing)
1
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
, 457 Zhongshan Road, Dalian 116023, People’s Republic of China
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Xueming Yang (杨学明);
Xueming Yang (杨学明)
(Funding acquisition, Writing – review & editing)
1
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
, 457 Zhongshan Road, Dalian 116023, People’s Republic of China
5
Department of Chemistry, Southern University of Science and Technology
, 1088 Xueyuan Road, Guangdong, Shenzhen 518055, People’s Republic of China
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Zefeng Ren (任泽峰)
Zefeng Ren (任泽峰)
a)
(Conceptualization, Formal analysis, Funding acquisition, Supervision, Writing – original draft, Writing – review & editing)
1
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
, 457 Zhongshan Road, Dalian 116023, People’s Republic of China
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 160, 024705 (2024)
Article history
Received:
October 05 2023
Accepted:
November 30 2023
Citation
Wei-Wang Zeng, Ting Luo, Peng Xu, Chuanyao Zhou, Xueming Yang, Zefeng Ren; Vibronic coupling of Rhodamine 6G molecules studied by doubly resonant sum frequency generation spectroscopy with narrowband infrared and broadband visible. J. Chem. Phys. 14 January 2024; 160 (2): 024705. https://doi.org/10.1063/5.0179871
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