We studied, for the first time to our knowledge, transient stimulated Raman
scattering in H-2-D-2 and H-2-CH4 gas mixtures excited with 200-fs and 2-p
s, 390-nm pulses. Depending on the composition and partial pressure, of tho
se gases, we observed similar to 40 output lines simultaneously. Under opti
mum conditions a conversion efficiency of as much as 8% in the combination
Raman line at 556 nm was obtained in the H-2-CH4 gas mixtures. The differen
ce between picosecond and femtosecond pumping is due to self-phase modulati
on and to generation of a spectral continuum in the latter. Our calculation
of the ratio of the partial pressures is in a good agreement with the expe
rimental results. A new method for measuring the unknown Raman scattering c
ross section of gas molecules is suggested. (C) 1999 Optical Society of Ame
rica.