Optimized control of generation of few cycle pulses by molecular modulation

Production of subfemtosecond optical pulses or pulses with predetermined sub-cycle shape of electric field demands a broadband coherent light source of few octaves of bandwidth. Previous work has shown that such a broadband light source can be obtained by the molecular modulation technique. In this article, we review theoretical and experimental improvements in this area: from increasing the efficiency of the generation process by use of hollow waveguides to increasing the number of sidebands generated by the Raman additive technique, or by combined vibrational and rotational Raman generation. We find that stimulated rotational Raman scattering can be either enhanced or suppressed at proper detunings from vibrational Raman resonance in the same molecular ensemble.