Generation of high-order rotational lines in hydrogen by four-wave Raman mixing in the femtosecond regime

More than 40 rotational Raman lines are generated using an 800-fs Ti:sapphire laser. The spectral region extends from the near-infrared to the far-ultraviolet with a considerably flat intensity distribution. The effects of laser polarization, pulsewidth, hydrogen pressure, and focusing conditions on the efficiencies of stimulated Raman scattering, four-wave Raman mixing, self-phase modulation, self-focusing, and harmonic generation are investigated. A white light continuum, generated by self-phase modulation, acts as a seed beam for the generation of high-order rotational lines through four-wave Raman mixing. Strong self-phase modulation, however, suppresses the generation of the Raman emission, due to a line broadening of the pump beam. Thus, optimization of experimental conditions is necessary for the efficient generation of high-order rotational lines.