High-resolution measurements of saturated coherent anti-Stokes Raman spectroscopy line shapes

Abstract

We report the first measurements to our knowledge of the effects of two-photon Raman saturation on fully resolved, homogeneously broadened coherent anti-Stokes Raman spectroscopy (CARS) line shapes. Saturation dips and line broadening were observed with a high-resolution scanning CARS experiment using a single-mode, frequency-doubled Nd:YAG laser and a pulse-amplified cw dye laser. Saturated line shapes are compared with the results of numerical solutions of the time-dependent density matrix equations.