High-order stimulated Raman scattering in a highly transient regime driven by a pair of ultrashort pulses.

We demonstrate efficient generation of high-order anti-Stokes Raman sidebands in a highly transient regime, using a pair of approximately 100-fs laser pulses tuned to Raman resonance with vibrational transitions in methane or hydrogen. The use of this technique looks promising for efficient subfemtosecond pulse generation.