Determination of ratios between nonlinear-optical coefficients by using subpicosecond optical rectification

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Abstract
We present a qualitative description of subpicosecond optical rectification and a detailed description of its application in, determining the ratios between nonlinear-optical coefficients. We propose the experimental determination of ratios between second-order optical rectification coefficients in all 15 point groups lacking inversion symmetry and having two or more independent nonvanishing nonlinear-optical coefficients in seven crystal structures. We have chosen three common nonlinear-optical crystal structures, cubic, trigonal, and monoclinic, in our experiments. The experimental results on GaAs, LiTaO3, and organic crystals agree with our theoretical calculation and previously reported data and demonstrate the potentiality and feasibility of the novel technique. We believe that this technique will play an important role in the characterization and development of novel nonlinear-optical materials.