Coherent molecular rotations induced by a femtosecond pulse consisting of two orthogonally polarized pulses

Stimulated Raman scattering induced by a femtosecond pulse formed by two pulses, polarized orthogonally with respect to each other is reported. High-frequency and low-frequency components generated at the center of the pulse through self-phase modulation temporally overlap. The two components induce a coherent molecular rotation through stimulated Raman scattering. The amplitude of this rotation in this way is larger than that of traditional transient stimulated Raman scattering in which linearly, elliptically, and circularly polarized pulses are used.