Abstract Since its first demonstration in sixties, coherent anti-Stokes Raman scattering has become a powerful spectroscopic tool. However, it is a multilinear four-wave mixing process that often leads to lack of quantitative analytical expressions. In this letter, we observe how signal builds up gradually and how it can be controlled with laser-pulse shaping for time-resolved three-color coherent anti-Stokes Raman scattering processes. Two driving pulses are tuned to the Raman-resonance of the vibrational ring modes for pyridine and benzene molecules. With off-resonant driving for water molecules this effect, in contrary, does not occur. The results are validated by the all-Gaussian analysis.

中文翻译：

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三色相干反斯托克斯拉曼散射中的定量时间分辨累积

摘要 相干反斯托克斯拉曼散射自六十年代首次展示以来，已成为一种强大的光谱工具。然而，它是一个多线性四波混频过程，往往会导致缺乏定量的解析表达式。在这封信中，我们观察了信号如何逐渐建立，以及如何通过激光脉冲整形来控制时间分辨三色相干反斯托克斯拉曼散射过程。两个驱动脉冲被调谐到吡啶和苯分子的振动环模式的拉曼共振。相反，对于水分子的偏共振驱动不会发生这种效果。结果通过全高斯分析得到验证。