| Title | Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths |
| Authors | Zhang, Ruidan Peng, Xingxing Jiao, Zhirun Luo, Ting Zhou, Chuanyao Yang, Xueming Ren, Zefeng |
| Affiliation | Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, 457 Zhongshan Rd, Dalian 116023, Peoples R China Peking Univ, ICQM, 5 Yiheyuan Rd, Beijing 100871, Peoples R China Peking Univ, Sch Phys, 5 Yiheyuan Rd, Beijing 100871, Peoples R China Univ Chinese Acad Sci, 19 A Yuquan Rd, Beijing 100049, Peoples R China Southern Univ Sci & Technol, Dept Chem, 1088 Xueyuan Rd, Shenzhen 518055, Guangdong, Peoples R China |
| Issue Date | 2019 |
| Publisher | JOURNAL OF CHEMICAL PHYSICS |
| Abstract | 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. Published under license by AIP Publishing. |
| URI | http://hdl.handle.net/20.500.11897/550560 |
| ISSN | 0021-9606 |
| DOI | 10.1063/1.5066580 |
| Indexed | SCI(E) EI |
| Appears in Collections: | 物理学院 |
