摘要
从量子力学密度矩阵出发,得出了考虑激光偏振条件下pump-probe光谱在时间域和频率域的普遍非线性响应函数,利用Liouville算符讨论了其具体计算过程.为适应时间分辨和频率分辨测量,将三阶极化强度在时间域和频率域内表示.将结果应用到激光喇曼诱导偏振光谱基态和激发态相干,考虑了两脉冲重叠情况,同时用图示法表示了激光作用的物理过程.
A unified nonlinear response function for pump-probe polarization spectroscopy is developed. The response function is expressed in time-domain and frequency-domain and is evaluated with Liouville space operator. These are applied to femtosecond Raman-induced polarization spectroscopy of rotational coherence in ground and excited electronic state,in which the superposition of the pulses is considered. The diagrammatic representation of the third order polarization is also given.
