Third order nonlinear optical difference frequency generation in KH2PO4, TiO2, LiNbO3, CaCO3, ZnO and CdS

Third-order nonlinear optical susceptibilities of different crystals have been measured relative to LiNbO₃ by observing collinear phase-matched difference frequency generation₁=2₂–₄. The two incident light waves have been produced by a ruby laser (₂,₂=694.3 nm) and by induced Raman scattering (₄,₄=765.8 nm). With noncollinear phase-matching the number of nonlinear processes and the possibilities to determine nonlinear coefficients is much larger than in the collinear case. Therefore the theory of Raman-type third order interactions has been extended to noncollinear propagation of the interacting waves. The theory has been tested experimentally for CdS.