We have studied third order nonlinearities, including two-photon absorption coeflicient β and nonlinear refractive index n_(2), of GaN in below bandgap ultraviolet (UV) wavelength regime by using UV femtosecond pulses. Two-photon absorption was investigated by demonstrating femtosecond UV pulse-width autocorrelation in a GaN thin film while ferntosecond Z-scan measurements revealed information for both n_(2) and β. The distribution of n_(2) versus wavelength was found to be consistent with a model described by the quadratic Stark effect, which is the dominant factor contributed to the nonlinear refractive index near the bandgap. Large β on the order of 10 cm/GW and large negative n_(2) with a magnitude on the order of several 10~(-12) cm~(2)/W were obtained. The β at near mid-gap infrared (IR) wavelength was also found to be on the order of several cm/GW by using two-photon-type autocorrelations in a GaN thin film. Taking advantage of the large two-photon absorption at mid-gap wavelengths, we have demonstrated excellent image quality on two-photon confocal microscopy, including two-photon-scanning-photoluminescence imaging and two-photon optical-beam-induced current microscopy, on a GaN Hall measurement sample and an InGaN green light emitting diode.
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