Roles of Al-vacancy complexes on the luminescence spectra of low dislocation density Si-doped AlN grown by halide vapor phase epitaxy

Abstract

Roles of Al-vacancy (VAl) complexes on the cathodoluminescence (CL) spectra of Si-doped AlN grown by halide vapor phase epitaxy (HVPE) on a physical-vapor-transported (0001) AlN substrate are described, making a connection with the results of positron annihilation measurements. A combination of HVPE and AlN substrate enabled decreasing deleterious carbon concentration and dislocation density, respectively, thus accentuating the influences of VAl-complexes on the luminescence processes. A low-temperature CL spectrum of unintentionally doped AlN exhibited predominant excitonic emissions at around 6 eV and a marginal deep-state emission band at around 3.7 eV that originates from residual carbon (<1016 cm−3) on nitrogen sites (CN). However, the sample was revealed to contain a considerable amount (∼1017 cm−3) of vacancy clusters, most likely comprising a VAl and nitrogen-vacancies (VN), namely, VAlVN1−2, which act as nonradiative recombination centers that decrease overall CL intensity at elevated temperatures. With increasing Si-doping concentration ([Si]), major vacancy species progressively changed from VAlVN1−2 to VAlON1−2, where ON is oxygen on N sites, which exhibit other deep-state emission bands ranging from 3.2 to 3.5 eV. Further increase in [Si] gave rise to the formation of donor-compensating defects comprising VAl and Si on the second-nearest-neighbor Al sites (SiAl), abbreviated by VAl−SiAln, which exhibit emission shoulders at around 2.9–3.0 eV. When [Si] exceeded 5 × 1018 cm−3, an emission band at around 4.5 eV emerged, which had been ascribed to originate from the nearest-neighbor SiAlCN complexes. Because VAl-complexes, including those containing impurities, are thermally stable, incorporation of vacancies should be blocked at the growth stage.