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.
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