Stimulated Raman Scattering in Pb(MoO4)1−x(WO4)x with x = 0, 0.5, 0.8 and 1.0 with Combined Frequency Shifts on High- and Low-Frequency Raman Modes under Synchronous Picosecond Laser Pumping

Comparative characteristics of spontaneous and stimulated Raman scattering in Pb(MoO4)1−x(WO4)x single crystals (x = 0, 0.5, 0.8, and 1.0) including both the high (ν1) and low (ν2) frequency internal anionic group vibrations have been investigated. It was found that among these crystals, Pb(MoO4)0.2(WO4)0.8 is the most suitable for multi-wavelength Raman laser in several Raman modes simultaneously. This is caused by the optimal relative Mo/W content corresponding to the most efficient coherent combination of the (MoO4)2− and (WO4)2− vibrations enhancing the output radiation characteristics of the synchronously pumped Pb(MoO4)0.2(WO4)0.8 Raman laser. Oscillation of up to twelve, closely spaced SRS components in a range of 1128–1360 nm and the strongest pulse shortening down to 1.16 ps in comparison with not only PbMoO4 and PbWO4 but also with all the earlier investigated nominally pure scheelite-like tungstate and molybdate crystals has been achieved.