Compression of single-cycle mid-infrared pulses by Raman-active molecular modulators

We show theoretically how high-order stimulated Raman scattering in the impulsive pump-probe regime can be used for generation of single mid-infrared (MIR) single-cycle pulses. The propagation of MIR probe pulses in a hollow waveguide filled with a Raman-excited gaseous medium, with a probe delay in the maximum of the molecular oscillations, results in spectral broadening covering almost 2 octaves. The spectral phases of this broadening can be compensated for by use of an output glass window with anomalous dispersion in the MIR. The spectral and temporal characteristics of the output pulses and the mechanism of pulse compression are studied by use of numerical and analytical solutions, and compression of a 70-fs input pulse at 4 microm to a single-cycle 6.5-fs output pulse is shown.