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We report on the generation of higher-order stimulated Raman scattering (SRS) in a saturated aqueous solution of MgSO4, pumped by a 532 nm frequency-doubled Nd:YAG laser operating with multiple longitudinal modes. The first- (∼561.4 nm), second- (∼594 nm), and third-order (∼630 nm) Stokes components of SRS were observed, and were attributed to the symmetric vibrations of the [SO4] tetrahedral structural groups. Two possible physical mechanisms for generating higher-order SRS were analyzed. The results point to an efficient method for generating new laser wavelengths from a liquid blended media system through a higher-order nonlinear SRS process.

Frequency conversion based on stimulated Raman scattering (SRS) is an effective and appealing method for generating new laser wavelengths. We report the generation of SRS derived from [Formula: see text], [Formula: see text], and [Formula: see text] stretching vibrations in three kinds of saturated aqueous solutions of inorganic salts (NaNO3, MgSO4, and K2CO3), pumped by a 532 nm frequency-doubled Nd: YAG laser. The maximal conversion efficiencies of SRS in three kinds of saturated aqueous solutions were measured, which correspond to ∼11%, 7%, and 5.5%, respectively. The 1st–3rd Stokes Raman and total conversion efficiencies were calculated using Raman coupled equations. Also, we analyze and discuss the affecting factors on the conversion efficiency of Stokes Raman. This work will be significant for future applications of SRS in obtaining new laser wavelengths in solutions.