Recently theorized hybrid II-IV-N2/III-N heterostructures, based on current commercialized (In,Ga)N devices, are predicted to significantly advance the design space of highly efficient optoelectronics in the visible spectrum, yet there are few epitaxial studies of II-IV-N2 materials. In this work, we present heteroepitaxial ZnGeN2 grown on GaN buffers and AlN templates. We demonstrate that a GaN nucleating surface is crucial for increasing the ZnGeN2 crystallization rate to combat Zn desorption, extending the stoichiometric growth window from 215 °C on AlN to 500 °C on GaN buffers. Structural characterization reveals well-crystallized films with threading dislocations extending from the GaN buffer. These films have a critical thickness for relaxation of 20–25 nm as determined by reflection high energy electron diffraction (RHEED) and cross-sectional scanning electron microscopy (SEM). The films exhibit a cation-disordered wurtzite structure, with lattice constants a = 3.216 ± 0.004 Å and c = 5.215 ± 0.005 Å determined by RHEED and X-ray diffraction (XRD). This work demonstrates a significant step toward the development of hybrid ZnGeN2-GaN integrated devices.
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