Four-wave mixing and the study of optical nonlinearities in semiconductors and semiconductor quantum dots

Abstract

This dissertation describes the study of various nonlinear optical effects in both bulk and quantum-confined semiconductors. Transverse effects in increasing absorption optical bistability are considered in bulk CdS for both single beam and wave mixing geometries. Measurement of the temporal response of BiI₃ quantum dots is described using degenerate four-wave mixing and explained theoretically. Finally, the experimental techniques developed to measure the one- and two-photon absorption coefficients of CdS quantum dots in glass are described along with the latest theoretical description and interpretation of the experimental spectra. The basic theory of increasing absorption optical bistability is presented along with experimental observation of this effect in CdS at low temperature. Transverse effects in increasing absorption optical bistability were observed in single beam experiments with CdS at low temperatures. The ring structures observed experimentally are explained theoretically. Degenerate four-wave mixing performed with this nonlinearity is theoretically shown to produce new scattering orders compared with a standard Kerr analysis. Experimental observation of these new scattering orders is presented. The temporal response of the nonlinearity in a solution of BiI₃ quantum dots in acetonitrile is determined using degenerate four-wave mixing. The independent contributions to the phase-conjugate signal are determined for both of the spatial gratings induced in the solution. The observed temporal responses indicated that a thermal mechanism was responsible for the nonlinearity. A theoretical analysis based on a thermal nonlinearity is presented which provides good agreement with the observed responses. The experimental techniques necessary to measure the one- and two-photon absorption coefficients of CdS quantum dots are described. The resultant measurements of quantum dot samples with microcrystallites ranging from 3.6 to 10.8 nm in diameter indicate no splitting of the energy levels associated with the hole. Theoretical spectra indicate this can be partially explained by the inclusion of Coulombic effects of the charged electron-hole pair.