Generally, nonlinear optics studies investigate optically-induced changes in refraction or absorption, and their application to spectroscopy or device fabrication. The photorefractive effect is a nonlinear optical effect that occurs in solids, where transport of an optically-induced free-carrier population results in an internal space-charge field, which produces an index change via the linear electrooptic effect. The photorefractive effect has been widely studied for a variety of materials and device applications, mainly because it allows large index changes to be generated with laser beams having only a few milliwatts of average power.Compound semiconductors are important photorefractive materials because they offer a near-infrared optical response, and because their carrier transport properties allow the index change to be generated quickly and efficiently. While many researchers have attempted to measure the fundamental temporal dynamics of the photorefractive effect in semiconductors using continuous-wave, nanosecond- and picosecond-pulsed laser beams, these investigations have been unsuccessful. However, studies with this goal are of clear relevance because they provide information about the fundamental physical processes that produce this effect, as well as the material's speed and efficiency limitations for device applications.In this dissertation, for the first time, we time-resolve the temporal dynamics of the photorefractive nonlinearities in two zincblende semiconductors, semi-insulating GaAs and undoped CdTe. While CdTe offers a lattice-match to the infrared material HgxCd1-xTe, semi-insulating GaAs has been widely used in optoelectronic and high-speed electronic applications. We use a novel transient-grating experimental method that allows picosecond temporal resolution and high sensitivity. Our results provide a clear and detailed picture of the picosecond photorefractive response of both materials, showing nonlinearities due to hot-carrier transport and the Dember space-charge field, and a long-lived nonlinearity that is due to the EL2 midgap species in GaAs. We numerically model our experimental results using a general set of equations that describe nonlinear diffraction and carrier transport, and obtain excellent agreement with the experimental results in both materials, for a wide variety of experimental conditions.
