An improved two-wavelength prism coupling method is used to measure the third-order nonlinear optical susceptibility χ(3) of polymer planar waveguide based on the m-line spectroscopy technique. Due to the optical Kerr effect, the index of the waveguide layer is modulated by the strong pump laser which is incident upon the upper base of the prism perpendicularly to guarantee that it is always coupled into the loading force point with the motorized rotary assembly rotate. Measurement of the third-order nonlinear optical susceptibility χ(3) of 1,4-diamino-2,3-diphenoxy-anthraquinone organic dye doped as guests into polymethyl-methacrylate (PMMA) waveguide films is first reported in this paper. A novel method to calculate the third-order nonlinear optical susceptibility χ(3) by the tiny change of the probe beam intensity at a certain synchronous angle of the guided mode is demonstrated and gave the value χ(3)= 3.34x10-11 esu.
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