Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths

Zhang, Ruidan1,2,3; Peng, Xingxing1,2,3; Jiao, Zhirun1,4; Luo, Ting1,4; Zhou, Chuanyao1; Yang, Xueming1,5; Ren, Zefeng1

2019-02-21

10.1063/1.5066580

JOURNAL OF CHEMICAL PHYSICS   影响因子和分区

0021-9606

1089-7690

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.

SCI ; EI

英语

其他

Youth Innovation Promotion Association of CAS[2017224]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:000459402600028

AMER INST PHYSICS

20190806534082

Interferometry ; Spectral resolution ; Spectrum analysis ; Titanium compounds ; Vibrational spectroscopy

Amplifiers:713.1 ; Light/Optics:741.1 ; Optical Variables Measurements:941.4 ; Mechanical Variables Measurements:943.2

CHEMISTRY

Web of Science

1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, 457 Zhongshan Rd, Dalian 116023, Peoples R China
2.Peking Univ, ICQM, 5 Yiheyuan Rd, Beijing 100871, Peoples R China
3.Peking Univ, Sch Phys, 5 Yiheyuan Rd, Beijing 100871, Peoples R China
4.Univ Chinese Acad Sci, 19 A Yuquan Rd, Beijing 100049, Peoples R China
5.Southern Univ Sci & Technol, Dept Chem, 1088 Xueyuan Rd, Shenzhen 518055, Guangdong, Peoples R China

Zhang, Ruidan,Peng, Xingxing,Jiao, Zhirun,et al. Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths[J]. JOURNAL OF CHEMICAL PHYSICS,2019,150(7).

Zhang, Ruidan.,Peng, Xingxing.,Jiao, Zhirun.,Luo, Ting.,Zhou, Chuanyao.,...&Ren, Zefeng.(2019).Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths.JOURNAL OF CHEMICAL PHYSICS,150(7).

Zhang, Ruidan,et al."Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths".JOURNAL OF CHEMICAL PHYSICS 150.7(2019).