Quantum theory of (femtosecond) time-resolved stimulated Raman scattering.
Quantum theory of (femtosecond) time-resolved stimulated Raman scattering.
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（飞秒）时间分辨受激拉曼散射的量子理论。
DOI：
10.1063/1.2888551
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发表时间：
2008
期刊：
影响因子：
--
通讯作者：
Soo
中科院分区：
文献类型：
--
作者：
Zhigang Sun;J. Lu;Dong H. Zhang;Soo
提出了完整的受激拉曼散射（SRS）微扰理论，其中包括飞秒受激拉曼散射（FSRS）实验新技术，即皮秒拉曼泵浦脉冲和飞秒探测脉冲同时作用于一个稳态或非稳态振动态。结果表明，在沿着探测脉冲方向观测的情况下，受激喇曼散射（SRS）需要用微扰理论中的8个项来描述，它们可以被归为4个非线性过程，称为受激拉曼散射或逆拉曼散射（IRS）：SRS（I）、SRS（II）、IRS（I）和IRS（II）。先前的FSRS理论仅使用SRS（I）过程或仅使用SRS（I）中的“共振拉曼散射”项。每个过程可以由初始电子态中的波包和激发的拉曼电子态中的波包之间的重叠来表示。利用高斯拉曼泵浦和探测脉冲对位移谐波势进行计算，以说明FSRS的各种特性，如高的时间和频率分辨率，Stokes线的拉曼增益，反Stokes线的拉曼损耗，以及在非共振FSRS中不存在瑞利线，共振FSRS中的色散线形状，共振FSRS中的色散线形状。以及用非共振FSRS观测振动波包运动的可能性。
We 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 femtosecond 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.
影响因子：
4.4
作者：
Lee, SY;Zhang, DH;Mathies, RA
通讯作者：
Mathies, RA
影响因子：
1.6
作者：
McCamant, DW;Kukura, P;Mathies, RA
通讯作者：
Mathies, RA