Spectral phase shaping for high resolution CARS

By spectral phase shaping of both the pump and probe pulses in coherent anti-Stokes Raman scattering (CARS) spectroscopy we demonstrate the extraction of the frequencies of vibrational lines using an unamplified oscillator. Furthermore we demonstrate chemically selective broadband CARS microscopy on a mixed sample of 4 μm diameter polystyrene (PS) and poly(methyl methacrylate) (PMMA) beads. The CARS signal from either the PS or the PMMA beads is shown to be enhanced or suppressed, depending on the phase profile applied to the broadband spectrum. Using a combination of negative and positive (sloped) π-phase steps in the pump and probe spectrum the purely non-resonant background signal is removed.