Reflective second harmonic generation near resonance in the epitaxial Al-doped ZnO thin film.

The second harmonic (SH) generation from the highly epitaxial Al-doped ZnO film on sapphire was measured, using the femtosecond Ti:Sapphire laser at the near-resonant SH wavelength, in reflection geometry to avoid the sapphire's contribution in the conventional Maker fringes technique. By investigating SH intensities as a function of the azimuthal angle along the film's normal, we found that the sapphire substrate had a negligible contribution to the reflective SH signal and the film had a pure and well-aligned c-domain. We also developed a new method to calculate the component's ratios of the nonlinear susceptibility tensor by analyzing the polarization diagrams of SH intensities under the incidence with two different angles. The ratios indicate that Kleinman's symmetry is broken due to the absorption at SH wavelength and the dominant component of the nonlinear susceptibility tensor is d(33). Calibration using the Z-cut quartz shows a possible overestimate of the nonlinear response by Maker fringes technique.