Effect of Two-Photon Stark Shift on the Multi-Frequency Raman Spectra

High order Raman generation has received considerable attention as a possible method for generating ultrashort pulses. A large number of Raman orders can be generated when the Raman-active medium is pumped by two laser pulses that have a frequency separation equal to the Raman transition frequency. High order Raman generation has been studied in the different temporal regimes, namely: adiabatic, where the pump pulses are much longer than the coherence time of the transition; transient, where the pulse duration is comparable to the coherence time; and impulsive, where the bandwidth of the ultrashort pulse is wider than the transition frequency. To date, almost all of the work has been concerned with generating as broad a spectrum as possible, but we are interested in studying the spectra of the individual orders when pumped in the transient regime. We concentrate on looking at extra peaks that are generated when the Raman medium is pumped with linearly chirped pulses. The extra peaks are generated on the low frequency side of the Raman orders. We discuss how linear Raman scattering from two-photon dressed states can lead to the generation of these extra peaks