Optimized continuum from a photonic crystal fiber for broadband time-resolved coherent anti-Stokes Raman scattering.

We demonstrate an optimization of continuum generation in a commercially available photonic crystal fiber and show that this continuum can be used to simultaneously measure vibrational dephasing times over an unprecedented frequency range of Raman modes. The dephasing time measurement is based on 2-pulse 3-color coherent anti-Stokes Raman scattering (CARS), and requires a continuum pulse that is coherent over a broad spectral bandwidth. We demonstrate that a continuum with the required characteristics can be generated from a photonic crystal fiber by appropriately conditioning the chirp of the excitation pulse and controlling its pulse energy. We are able to simultaneously measure vibrational dephasing times of multiple Raman modes (covering 500 cm(-1) to 3100 cm(-1)) of acetonitrile and benzonitrile using the optimized continuum with broadband time-resolved CARS.