Cancellation of laser phase fluctuations in Stokes and anti - Stokes generation

In the coherent anti-Stokes Raman scattering process, the spectrum of the generated optical phonon depends on the degree of temporal correlation between the pump laser field and the Stokes field. When the two fields are strongly correlated, such as when the Stokes field is generated with stimulated Raman scattering (SRS), the spectral shape of the optical phonon is found experimentally and theoretically to be the same as the gain-narrowed Raman line shape because the laser phase fluctuations cancel out totally, leaving only the collisional noise in the SRS process. When the two fields are uncorrelated, the shape of the optical-phonon spectrum is found to be the same as the Raman line shape without gain narrowing. When two fields are partially correlated, then the two spectral components appear together. We provide a method to measure the degree of correlation between two optical fields that have different central frequencies. The theory developed to interpret the experimental results is an extension of the quantum theory of SRS to include anti-Stokes scattering. We show that only in the high-gain limit can the quantum fluctuations be thought of as arising from a classical noise process.