Two-photon absorption and resonant non-phase-matched second-harmonic generation in CdSe

Exciting a hexagonal CdSe crystal with picosecond Nd: glass laser pulses, two-photon absorption and resonant non-phase-matched second-harmonic generation occur simultaneously. Using different crystal orientations, all components of the secondharmonic susceptibility tensor (non-vanishing components ared₃₁,d₃₃ andd₁₅) and some components of the two-photon absorption susceptibility tensor _ijkl⁽³⁾(–_L; _L, _L, –_L) are determined.