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

doi:10.1063/1.5066580

	Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths
	Ren, Zefeng 1; Zhang, Ruidan 1,2,3; Peng, Xingxing 1,2,3; Jiao, Zhirun 1,4; Luo, Ting 1,4; Zhou, Chuanyao 1; Yang, Xueming 1,5
刊名	JOURNAL OF CHEMICAL PHYSICS
	2019-02-21
卷号	150 期号:7 页码:12
ISSN号	0021-9606
DOI	10.1063/1.5066580
通讯作者	Ren, Zefeng(zfren@dicp.ac.cn)
英文摘要	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.
资助项目	National Key RD Program[2018YFA0208700] ; National Key RD Program[2016YFA0200602] ; National Natural Science Foundation of China[91645125] ; National Natural Science Foundation of China[21688102] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB17000000] ; Youth Innovation Promotion Association of CAS[2017224]
WOS关键词	WATER ; SFG ; ACETONITRILE ; DISSOCIATION ; ADSORPTION ; INTERFACE ; SURFACES ; METHANOL ; PROBE ; CO
WOS研究方向	Chemistry ; Physics
语种	英语
出版者	AMER INST PHYSICS
WOS记录号	WOS:000459402600028
资助机构	National Key RD Program ; National Key RD Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of CAS ; Youth Innovation Promotion Association of CAS ; National Key RD Program ; National Key RD Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of CAS ; Youth Innovation Promotion Association of CAS ; National Key RD Program ; National Key RD Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of CAS ; Youth Innovation Promotion Association of CAS ; National Key RD Program ; National Key RD Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of CAS ; Youth Innovation Promotion Association of CAS
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/166018]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Ren, Zefeng
作者单位	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
推荐引用方式 GB/T 7714	Ren, Zefeng,Zhang, Ruidan,Peng, Xingxing,et al. Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths[J]. JOURNAL OF CHEMICAL PHYSICS,2019,150(7):12.
APA	Ren, Zefeng.,Zhang, Ruidan.,Peng, Xingxing.,Jiao, Zhirun.,Luo, Ting.,...&Yang, Xueming.(2019).Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths.JOURNAL OF CHEMICAL PHYSICS,150(7),12.
MLA	Ren, Zefeng,et al."Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths".JOURNAL OF CHEMICAL PHYSICS 150.7(2019):12.