Measurement of second order susceptibilities of GaN and AlGaN

Abstract

Rotational Maker fringes, scaled with respect to χ11(2) of crystalline quartz, were used to determine the second order susceptibilities χ31(2) and χ33(2) for samples of thin AlxGa1−xN films, a thicker GaN film, and a free-standing GaN platelets. The pump wavelength was 1064nm. The AlxGa1−xN samples, ranging in thickness from roughly 0.5to4.4μm, were grown by metalorganic chemical vapor deposition (MOCVD) and hydride vapor-phase epitaxy (HVPE) on (0001) sapphire substrates. The Al mole fractions x were 0, 0.419, 0.507, 0.618, 0.660, and 0.666, for the MOCVD-grown samples, and x=0, 0.279, 0.363, and 0.593 for the HVPE-grown samples. An additional HVPE-grown GaN sample ∼70μm thick was also examined. The free-standing bulk GaN platelets consisted of an HVPE grown film ∼226μm thick removed from its growth substrate, and a crystal ∼160μm thick grown by high-pressure techniques. For the AlxGa1−xN samples, the magnitudes of χ31(2) and χ33(2) decrease roughly linearly with increasing x and extrapolate to ∼0 for x=1. Furthermore, the constraint expected for a perfect wurtzite structure, namely χ33(2)=−2χ31(2), was seldom observed, and the samples with x=0.660 and x=0.666 showed χ31(2) and χ33(2) having the same sign. These results are consistent with the theoretical studies of nonlinear susceptibilities for AlN and GaN performed by Chen et al. [Appl. Phys. Lett. 66, 1129 (1995)]. The thicker bulk GaN samples displayed a complex superposition of high- and low-frequency Maker fringes due to the multiple-pass interference of the pump and second-harmonic generation beams, and the nonlinear coefficients were approximately consistent with those measured for the thin-film GaN sample.