Subfemtosecond pulse generation and multiplicative increase of pulse spacing in high-order stimulated Raman scattering

We demonstrate a technique for multiplicatively increasing the pulse spacing of subfemtosecond pulse trains generated by high-order stimulated Raman scattering, which uses pairs of off-resonant two-photon excitation of a molecular Raman mode to establish strong molecular modulation in the medium. Every laser pair has two single-mode laser beams tuned slightly off two-photon resonance, and the laser pairs have their corresponding carrier frequencies shifted from each other by one half, one third, or one fourth of the selected molecular Raman mode frequency. Theoretical analyses and calculations based on the fundamental vibrational transition of solid hydrogen show that the pulse spacing of the subfemtosecond pulse trains thus generated can readily be doubled, tripled, or even quadrupled.