Quantitative time-resolved buildup in three-color coherent anti-Stokes Raman scattering

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.