Development of a new method for the evaluation of third nonlinear optical properties of powder crystals

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In this work, we developed the equipment based on FWMEW to determine the third optical non-linearity precisely of the powder samples having a large absorption band in the visible range. We measured the chi^<(3)> values of the powder or thin-film samples using this equipment and confirmed the effectiveness of the method. At present, due to the large reflection from the prism surface and the diffraction at the prism-sample interface, the application of FWMEW method is limited to the large chi^<(3)> samples such as VO-Pc or Pt-dimethylglyoxim. Although the THEW method has much higher sensitivity, the FWMEW method has the merit that the measurements under non-resonant conditions are easy. Now, we are improving the SIN on the measurements of FWMEW.In the mean time, we developed the charge-trensfer-complex LB films having optical non-linearity. The preliminary studies on the second order effect by the field modulating spectroscopy were performed. The evaluation of the optical non-linearlity on the power samples of charge transfer compleses such as (TBA)(EtO-C[C(CN)_2]_2and (EtO-TCA) is also started.