Experimental observation of spectral super-broadening of backward stimulated Raman scattering in liquids

The spectral super-broadening of backward stimulated Raman scattering (SRS) in four liquid samples ( C C l 4 , dimethyl sulfoxide, acetone, and C H 2 C l 2 ) have been observed under the pump conditions of using 532-nm and ∼ 11 - n s pulsed laser beams from a frequency-doubled and multilongitudinal mode Pockels Q-switched Nd:YAG laser device. Under the same pump conditions, in acetone the observed maximum broadening range was ≥ 450 c m − 1 for the backward SRS, while it was ≤ 45 c m − 1 for the forward SRS. The physical origin of this observed effect is essentially related to the detailed temporal structure of the 532-nm pump pulse that consists of a series of subpulse of ∼ 50 p s width, owing to the randomly beating effect among a large number of longitudinal modes of the Pockels Q-switched laser source. Each backward SRS subpulse undergoes multiple cross-phase modulation (XPM) by interacting with a certain number of forward pump subpulses, and consequently manifests a super-broadened spectral distribution. In contrast, each forward SRS subpulse interacts only with a single pump subpulse and therefore experiences a much limited XPM influence, resulting in a much smaller spectral broadening. Furthermore, when the 532-nm pump beam was from a single-longitudinal mode-seeded Nd:YAG laser, there was no beating-effect-induced subpulse structure of the pump pulse, and thereby no noticeable spectral broadening for both backward and forward SRS could be observed.