The difficulty in achieving high spectral resolution and accurate line shape in sum-frequency generation vibrational spectroscopy (SFG-VS) has restricted its use in applications requiring precise detection and quantitative analysis. Recently, the development of high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS) with sub-wavenumber resolution generated by synchronizing two independent amplifier lasers have opened new opportunities for probing an intrinsic SFG response. Here, we present a new flexible approach to achieve HR-BB-SFG-VS. In this system, two regeneration amplifiers shared the same oscillator laser as the seed, and a time-asymmetric visible pulse with a nearly Lorentzian line shape filtered by an etalon was used to overlap with a femtosecond broadband infrared pulse. This Lorentzian line shape of the visible pulse can greatly simplify the spectral fitting and analysis. We also demonstrated that the single-sided long visible pulse provided both high spectral resolution (1.4 cm−1) and effective suppression of the non-resonant background by detuning the time delay between visible and infrared pulses in SFG-VS measurements. With this new SFG setup, a pair of spectral splittings by 3.1 ± 0.7 and 3 ± 0.2 cm−1 for the symmetric and antisymmetric stretching of the CH3 group was resolved at the CH3CN/TiO2(110) surface, which are tentatively attributed to two different orientational methyl groups. These technological advancements can help broaden the applications of HR-BB-SFG-VS and provide solid ground for a better understanding of complex molecular structures and dynamics at interfaces.
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21 February 2019
Research Article|
February 15 2019
Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths
Special Collection:
Nonlinear Spectroscopy and Interfacial Structure and Dynamics
Ruidan Zhang;
Ruidan Zhang
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
International Center for Quantum Materials (ICQM) and School of Physics, Peking University
, 5 Yiheyuan Road, Beijing 100871, People’s Republic of China
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Xingxing Peng;
Xingxing Peng
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
International Center for Quantum Materials (ICQM) and School of Physics, Peking University
, 5 Yiheyuan Road, Beijing 100871, People’s Republic of China
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Zhirun Jiao;
Zhirun Jiao
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
University of Chinese Academy of Sciences
, 19 A Yuquan Road, Beijing 100049, People’s Republic of China
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Ting Luo;
Ting Luo
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
University of Chinese Academy of Sciences
, 19 A Yuquan Road, Beijing 100049, People’s Republic of China
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Chuanyao Zhou;
Chuanyao Zhou
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;
Xueming Yang
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 Chemistry, Southern University of Science and Technology
, 1088 Xueyuan Road, Guangdong, Shenzhen 518055, China
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Zefeng Ren
Zefeng Ren
a)
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: zfren@dicp.ac.cn
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a)Author to whom correspondence should be addressed: zfren@dicp.ac.cn
Note: This article is part of the Special Topic “Nonlinear Spectroscopy and Interfacial Structure and Dynamics” in J. Chem. Phys.
J. Chem. Phys. 150, 074702 (2019)
Article history
Received:
October 15 2018
Accepted:
January 25 2019
Citation
Ruidan Zhang, Xingxing Peng, Zhirun Jiao, Ting Luo, Chuanyao Zhou, Xueming Yang, Zefeng Ren; Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths. J. Chem. Phys. 21 February 2019; 150 (7): 074702. https://doi.org/10.1063/1.5066580
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