A method and system (10) are presented for producing exciting radiation (P′) to be used in producing an output coherent anti-stokes Raman scattering (CARS) signal of a medium (12). An input spectral phase coherent optical pulse (P), carrying a pump, a Stokes and a probe photon, is optically processed by adjusting spectral phase and polarization of wavelength components of the input pulse to produce a unitary optical exciting pulse (P′) that carries the pump photon, the Stokes photon and multiple probe photons and is capable of inducing interference between contributions from at least some of vibrational levels in the CARS signal.