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Different nonlinear optical interactions in a novel SRS‐active non‐centrosymmetric tetragonal crystal Ca2ZnSi2O7 were investigated at room and cryogenic (≈9 K) temperature under picosecond laser pumping. In addition to measuring octave‐spanning Stokes and anti‐Stokes combs we observed several cascaded and cross‐cascaded χ(3) ↔ χ(3) effects involving several SRS‐active phonons. All recorded Raman‐induced...
Nonlinear optical interactions based on χ(2) and χ(3) effects were investigated in the tetragonal, non‐centrosymmetric melilite‐type crystal Sr2ZnGe2O7. Among them are Stokes and anti‐Stokes lasing comb generation, SHG, THG, SFG, and cascaded χ(3) ↔ χ(2) self‐frequency conversion, arising from onemicron picosecond pumping. All lasing components were identified and attributed to a single SRS‐promoting...
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