Supercontinuum-based three-color three-pulse time-resolved coherent anti-Stokes Raman scattering.

We demonstrate the use of a photonic crystal fiber (PCF) as a compact three-color fs laser system operating at 76 MHz, limited only by the repetition rate of the pump laser. The system is suitable for background-free time-resolved four-wave mixing measurements, which arguably reach fundamental limits in signal detectivity. We give a detailed characterization of the near transform-limited multi-color pulses that are extracted from the PCF, and prove the system through time-resolved coherent anti-Stokes Raman scattering measurements in bipyridyl ethylene and styrene.