Frontiera Renee R, Shim Sangdeok, Mathies Richard A
Department of Chemistry, University of California, Berkeley, California 94720, USA.
J Chem Phys. 2008 Aug 14;129(6):064507. doi: 10.1063/1.2966361.
Femtosecond stimulated Raman spectroscopy is extended to probe ground state anti-Stokes vibrational features. Off resonance, negative anti-Stokes features are seen that are the mirror image of the positive Stokes side spectra. On resonance, the observed dispersive lineshapes are dramatically dependent on the frequencies of the picosecond pump and femtosecond probe pulses used to generate the stimulated Raman spectra. These observations are explained by the contributions of the inverse Raman and hot luminescence four-wave mixing processes discussed by Sun et al. [J. Chem. Phys. 128, 144114 (2008)], which contribute to the overall femtosecond stimulated Raman signal.
飞秒受激拉曼光谱被扩展用于探测基态反斯托克斯振动特征。在非共振情况下，会出现负的反斯托克斯特征，它们是正斯托克斯侧光谱的镜像。在共振时，观察到的色散线形强烈依赖于用于产生受激拉曼光谱的皮秒泵浦脉冲和飞秒探测脉冲的频率。Sun等人[《化学物理杂志》128, 144114 (2008)]讨论的逆拉曼和热发光四波混频过程对整体飞秒受激拉曼信号有贡献，这些观察结果可以用这些贡献来解释。
