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Quantum theory of (femtosecond) time-resolved stimulated Raman scattering
Sun, Zhigang1; Lu, J.2; Zhang, Dong H.3,4; Lee, Soo-Y.1
Source PublicationJOURNAL OF CHEMICAL PHYSICS
2008-04-14
DOI10.1063/1.2888551
Volume128Issue:14
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectPhysics, Atomic, Molecular & Chemical
WOS Research AreaPhysics
WOS KeywordEXCITED-STATE ; BETA-CAROTENE ; ULTRAFAST DYNAMICS ; SPECTROSCOPY
AbstractWe present a complete perturbation theory of stimulated Raman scattering (SRS), which includes the new experimental technique of femtosecond stimulated Raman scattering (FSRS), where a picosecond Raman pump pulse and a ferntosecond probe pulse simultaneously act on a stationary or nonstationary vibrational state. It is shown that eight terms in perturbation theory are required to account for SRS, with observation along the probe pulse direction, and they can be grouped into four nonlinear-processes which are labeled as stimulated Raman scattering or inverse Raman scattering (IRS): SRS(I), SRS(II), IRS(I), and IRS(II). Previous FSRS theories have used only the SRS(I) process or only the "resonance Raman scattering" term in SRS(I). Each process can be represented by an overlap between a wave packet in the initial electronic state and a wave packet in the excited Raman electronic state. Calculations were performed with Gaussian Raman pump and probe pulses on displaced harmonic potentials to illustrate various features of FSRS, such as high time and frequency resolution; Raman gain for the Stokes line, Raman loss for the anti-Stokes line, and absence of the Rayleigh line in off-resonance FSRS from a stationary or decaying v = 0 state; dispersive line shapes in resonance FSRS; and the possibility of observing vibrational wave packet motion with off-resonance FSRS. (c) 2008 American Institute of Physics.
Language英语
WOS IDWOS:000255470300014
Citation statistics
Cited Times:48[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/141102
Collection中国科学院大连化学物理研究所
Affiliation1.Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore
2.Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
4.Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Theoret & Computat Chem, Dalian 116023, Peoples R China
Recommended Citation
GB/T 7714
Sun, Zhigang,Lu, J.,Zhang, Dong H.,et al. Quantum theory of (femtosecond) time-resolved stimulated Raman scattering[J]. JOURNAL OF CHEMICAL PHYSICS,2008,128(14).
APA Sun, Zhigang,Lu, J.,Zhang, Dong H.,&Lee, Soo-Y..(2008).Quantum theory of (femtosecond) time-resolved stimulated Raman scattering.JOURNAL OF CHEMICAL PHYSICS,128(14).
MLA Sun, Zhigang,et al."Quantum theory of (femtosecond) time-resolved stimulated Raman scattering".JOURNAL OF CHEMICAL PHYSICS 128.14(2008).
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