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题名: Theoretical investigation of the direct observation of anharmonic coupling in CDCl3 in the time domain with femtosecond stimulated Raman scattering
作者: Sun, Zhigang1, 2;  Fu, Bina3, 4;  Zhang, Dong H.3, 4;  Lee, Soo-Y.1, 2
通讯作者: 李仕仁
关键词: ab initio calculations ;  ground states ;  molecular configurations ;  molecular moments ;  molecule-photon collisions ;  optical pumping ;  organic compounds ;  potential energy surfaces ;  stimulated Raman scattering ;  transition moments ;  vibrational states
刊名: JOURNAL OF CHEMICAL PHYSICS
发表日期: 2009-01-28
DOI: 10.1063/1.3068709
卷: 130, 期:4, 页:044312-044312
收录类别: SCI
文章类型: Article
部门归属: 11
项目归属: 1102
产权排名: 2;1
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Physics
英文摘要: The femtosecond stimulated Raman scattering (FSRS) difference spectra of CDCl3 from the ground potential energy surface, with and without off-resonance impulsive stimulated Raman pumping, taken at various delay times from the impulsive pump by Kukura [Phys. Rev. Lett. 96, 238303 (2006)], showed sidebands of the C-Cl bends with periodic changes in phase as well as having an inversion symmetry to the high and low frequency sides of the Stokes C-D stretch at 2255 cm(-1). The semiclassical coupled-wave approach and a one-dimensional (1D) oscillator model for the C-D stretch whose frequency is modulated in time by the C-Cl bends could account for some features of the experimental results. Here, a quantum mechanical investigation is made of the FSRS difference spectra with a modulated 1D oscillator and three-dimensional (3D) harmonic and anharmonic potentials. It is shown that (i) the sidebands are allowed, with or without anharmonic coupling between the C-D stretch and the C-Cl bends, (ii) in the 3D harmonic model the sidebands have mirror symmetry about the Stokes C-D stretch, (iii) in the 3D anharmonic model with appropriate coupling terms between the C-D stretch and the C-Cl bends, the experimental results are well accounted for in both the phase changes in the FSRS difference spectra with time delay as well as the inversion symmetry of the sidebands for the C-Cl bends about the Stokes C-D stretch, (iv) there is a correspondence between the phase changes in the FSRS difference spectra and the wavepacket motion induced by the impulsive pump pulse on the ground potential energy surface as a function of the delay time, and (v) changing the polarization of the impulsive pump pulse, say, directly affects the coordinate dependence of the linear transition dipole moment in the asymmetric mode and hence its phase in the FSRS difference spectra, but not so for the symmetric modes where the displacement of the excited state surface governs the FSRS difference spectra more than the transition dipole moment. This work illustrates the potential of off-resonance FSRS in studying polyatomic molecular dynamics.
关键词[WOS]: DYNAMIC ABSORPTION-SPECTRA ;  PUMP-PROBE SPECTROSCOPY ;  VIBRATIONAL SPECTROSCOPY ;  MOLECULAR-DYNAMICS
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000262965000023
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/101605
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Nanyang Technol Univ, Sch Phys & Math Sci, Div Chem & Biol Chem, Singapore 637371, Singapore
2.Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore
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:
Sun, Zhigang,Fu, Bina,Zhang, Dong H.,et al. Theoretical investigation of the direct observation of anharmonic coupling in CDCl3 in the time domain with femtosecond stimulated Raman scattering[J]. JOURNAL OF CHEMICAL PHYSICS,2009,130(4):044312-044312.
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