Correlated High-Frequency Molecular Motions in Neat Liquid Probed with Ultrafast Overtone Two-Dimensional Infrared Spectroscopy

doi:10.1021/jz301652v

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	Correlated High-Frequency Molecular Motions in Neat Liquid Probed with Ultrafast Overtone Two-Dimensional Infrared Spectroscopy
	Li, Donghai; Yang, Fan; Han, Chen; Zhao, Juan; Wang, Jianping
刊名	JOURNAL OF PHYSICAL CHEMISTRY LETTERS
	2012-12-06
卷号	3 期号:23 页码:3665-3670
ISSN号	1948-7185
DOI	10.1021/jz301652v
英文摘要	In this work, an overtone two-dimensional infrared (2D IR) method is shown to allow correlated molecular motions at the frequencies of overtone transitions to be studied. Waiting-time-dependent overtone 2D IR results of the C-O stretching in neat liquid methanol reveal that the autocorrelation of the v = 0 -> 2 transition and the cross correlation of the v = 0 -> 2/v = 2 -> 4 transitions differ considerably (relaxation time being 700 fs and 2 ps, respectively), suggesting different spectral diffusion dynamics. Quantum-chemical computations in combination with ab initio molecular dynamics simulations show that the overtone transition frequency of the C-O stretching mode in liquid methanol is of more structural sensitivity than the fundamental frequency. This work demonstrates a new 2D IR approach to examining the structural sensitivities of the anharmonic potential parameters of higher vibrational states, which can be used to gain new insight into the ultrafast structural dynamics particularly for neat liquids.
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000312170600046
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/48573]
专题	中国科学院化学研究所
通讯作者	Wang, Jianping
作者单位	Chinese Acad Sci, Beijing Natl Lab Mol Sci, State Key Lab Mol React Dynam, Inst Chem, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Li, Donghai,Yang, Fan,Han, Chen,et al. Correlated High-Frequency Molecular Motions in Neat Liquid Probed with Ultrafast Overtone Two-Dimensional Infrared Spectroscopy[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2012,3(23):3665-3670.
APA	Li, Donghai,Yang, Fan,Han, Chen,Zhao, Juan,&Wang, Jianping.(2012).Correlated High-Frequency Molecular Motions in Neat Liquid Probed with Ultrafast Overtone Two-Dimensional Infrared Spectroscopy.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,3(23),3665-3670.
MLA	Li, Donghai,et al."Correlated High-Frequency Molecular Motions in Neat Liquid Probed with Ultrafast Overtone Two-Dimensional Infrared Spectroscopy".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 3.23(2012):3665-3670.