The author explores absorptive and refractive optical nonlinearities at 1.06 [mu]m in bulk, semi-insulating, undoped GaAs with a particular emphasis on the influence of the native deep-level defect known as EL2. Picosecond pump-probe experimental technique is used to study the speed, magnitude, and origin of the absorptive and refractive optical nonlinearities and to characterize the dynamics of the optical excitation of EL2 in three distinctly different undoped, semi-insulating GaAs samples. Intense optical excitation of these materials leads to the redistribution of charge among the EL2 states resulting in an absorptive nonlinearity due to different cross sections for electron and hole generation through this level. This absorptive nonlinearity is used in conjunction with the linear optical properties of the material and independent information regarding the EL2 concentration to extract the cross section ratio [sigma][sub p]/[sigma][sub e] [approx equal]0.8, where [sigma][sub p](e) is the absorption cross section for hole (electron) generation from EL2[sup +] (EL2[sup 0]). The picosecond pump-probe technique can be used to determine that EL2/EL2[sup +]density ratio in an arbitrary undoped, semi-insulating GaAs sample. The author describes the use of complementary picosecond pump-probe techniques that are designed to isolate and quantify cumulative and instantaneous absorptive and refractive nonlinear processes. Numerical …

Intensive demands have arisen to characterize nonlinear optical properties of materials for applications involving optical limiters, waveguide switches and bistable light switches. The technique of Pulse Delay Modulation is described which can monitor nonlinear changes in transmission with shot noise limited signal-to-noise ratios even in the presence of large background signals. The theoretical foundations of the experiment are presented followed by actual measurements of beam depletion due to second harmonic generation in a LiIO3 crystal and two-photon absorption in the semiconductor ZnSe. Sensitivity to polarization rotation arising from the Kerr Effect in carbon disulfide, saturable absorber relaxation in modelocking dyes and photorefractive effects in ZnSe are demonstrated. The sensitivity of Pulse Delay Modulation is combined with Fabry-Perot enhancement to allow the measurement of two-photon absorption in a 0.46pm thick interference filter spacer layer. Also included is a study of nonlinear optical limiting arising from dielectric breakdown in gases.