Highly transient stimulated Raman scattering in SrMoO₄ under ultrafast laser pumping with a controllable chirp

For the first time, to the best of our knowledge, we demonstrate highly transient, multiwavelength, single-pass Raman generation with combined frequency shifts on two Raman modes of an SrMoO₄ crystal with high total Raman conversion efficiency of up to 48% in conditions of competition with self-phase modulation (SPM). A 58-mm-long SrMoO₄ crystal was used as the active medium under pumping by the 1030-nm, 40-µJ laser pulses with controllable dispersive stretching in a range of 0.25-6 ps at negative and positive chirping. The pump pulse chirping was optimized for both high- and low-frequency Raman shifts on the primary (888 cm^-1) and secondary (327 cm^-1) Raman modes of the crystal. At the optimal conditions, four Stokes components of stimulated Raman scattering (SRS) radiation with high- and low-frequency Raman shifts at the wavelengths of 1066, 1134, 1177, and 1261 nm were efficiently generated.