Title: Nonlinear optical processes in zinc oxide
Description: ZnO is a technologically interesting material for a variety of blue-VU wavelength optoelectronic applications. For most of these applications, ZnO is excited or pumped with a femtosecond laser source. The nonlinear dynamics and behaviors that result from the interaction between a material and highly intense, ultrashort femtosecond laser pulses is the focus of this dissertation. This dissertation reports on the ultrafast dynamics of ZnO during excitation by intense femtosecond laser pulses. Irradiation of ZnO by femtosecond pulses is known to excite carriers and produce stimulated emission. However, the mechanism of lasing and the resulting changes in optical properties have not yet been precisely determined. We investigate these dynamics by monitoring the response of ZnO using a broadband pump-probe technique that measures the reflectivity and dielectric function from the near-infrared to the near-ultraviolet with a time resolution of about 100 femtoseconds. For excitation densities near the reported lasing thresholds, we determine that the large carrier densities produced by femtosecond laser excitation significantly damps the exciton resonance. This strong damping of the exciton resonance indicates a significant screening of the Coulomb interaction by the excited free carriers. As the resonance recovery occurs over several picoseconds after excitation, we support the model that electron-hole plasma recombination is the primary lasing mechanism in ZnO. In addition to damping of the exciton resonance, we also find that the main resonance for interband electronic transitions in ZnO shifts to lower photon energy after laser excitation. Regardless of the excitation wavelength, we observe broadband changes in the dielectric function of ZnO, ranging from 3.0 to 3.5 eV.

From the dielectric function, many transient material properties, such as the index of refraction and dispersion characteristics of ZnO under excitation, can be determined to optimize ZnO-based optoelectronic devices.