Cross-correlation frequency-resolved optical gating coherent anti-Stokes Raman scattering with frequency-converting...

Photonic-crystal fibers provide a high efficiency of frequency upconversion of regeneratively amplified femtosecond pulses of a Cr: forsterite laser, permitting the generation of subpicosecond anti-Stokes pulses with a smooth temporal envelope and a linear positive chirp, ideally suited for femtosecond coherent nonlinear spectroscopy. These pulses from a photonic-crystal fiber were cross correlated in our experiments with the femtosecond second-harmonic output of the Cr: forsterite laser in toluene solution, used as a test object, in boxcars geometry to measure the spectra of coherent anti-Stokes Raman scattering (CARS) of toluene molecules (XFROG CARS).