Resolving power and sensitivity in modulation transfer stimulated resonant Raman spectroscopy

We show that the lineshape and size of the detected signal in ultra-high-resolution stimulated Raman spectroscopy computed from a general expression of the modulated signal are in good agreement with the experimental results. Using the theoretical expression of the signal, we analyze the resolving power and the sensitivity of our Raman spectrometer. We show that a second harmonic detection in high-frequency transfer modulation generates a lineshape without modulation broadening. A 2.6-kHz-wide resonance has been obtained with iodine, mainly limited by both the transit time and collisions.