A-axis oriented Zn_0.72Mg_0.28O epitaxial thin films with large second-order nonlinear susceptibility

Abstract Large nonlinear susceptibility that originates from strong electronic polarization enables ultrafast nonlinear optical devices. This work discovers that Mg incorporation has important contribution for enhancing second-order nonlinear susceptibility (χ (2)) and laser-induced surface-damage threshold of wurtzite ZnO epitaxial thin films deposited by radio-frequency magnetron sputtering method. Second-harmonic generation measurements derive that as-deposited Zn0.72Mg0.28O shows a gain of 48%, 77% and 33% in χ 33, χ 31 and χ 15 with respect to as-deposited ZnO. Specially, the annealed Zn0.72Mg0.28O has a χ 33 value of −57.0 ± 1.8 pm V−1, which gets comparable to that of LiNbO3 crystals. Triple-axis x-ray diffraction measurements conclude that the Mg incorporation should increase the χ (2) under optical frequency electric field by strengthening electronic polarization rather than increasing the residual strain in the film. Furthermore, the annealed Zn0.72Mg0.28O exhibits an increase of 48% in laser-induced surface-damage threshold relative to [11–20] ZnO crystals. These findings open the way of the Zn0.72Mg0.28O thin films to ultrafast nonlinear optical devices.