This dissertation reports on the development of a nonlinear surface spectroscopy and the observation of nonlinear optical phenomena using sputtered zinc oxide waveguides. The first is known as Surface Coherent Raman Spectroscopy, or SCRS, and is capable of monolayer sensitivity. The second, discovered during the development of SCRS, is optical limiting and a previously unobserved form of optical switching based on an absorptive nonlinear coupling mechanism.; Overviews of the theories of waveguiding, linear coupling, and SCRS are given. Experiments showing that the spectrum of a monolayer coverage of molecules on the surface of a metal oxide waveguide can be obtained using SCRS are reported. For this purpose ZnO waveguides were fabricated using rf magnetron sputtering; the details of which are presented. The results of the characterization of these films, using an optical loss technique, Rutherford backscattering, and X-ray diffraction, are also presented.; Experiments are described and data are presented to show the existence of optical limiting and optical switching phenomena in ZnO waveguides. The experimental dependence of these phenomena on input pulse energy, wavelength, temporal pulse width, and type of distributed coupling mechanism is described. Existing nonlinear distributed coupler theory is extended to include the effect of an absorptive nonlinearity and the results of this theory are used to explain some of the characteristic features of the experimental results. A value of n(,2) (TURNEQ) 2 x 10('-16) m('2)/W for the nonlinear coefficient of sputtered ZnO films is obtained.
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