Single-crystalline Zn3N2 thin films have been grown on MgO (100) and YSZ (100) substrates by plasma-assisted molecular beam epitaxy. Depending on growth conditions, the film orientation can be tuned from (100) to (111). For each orientation, x-ray diffraction and reflection high-energy electron diffraction are used to determine the epitaxial relationships and to quantify the structural quality. Using high-temperature x-ray diffraction, the Zn3N2 linear thermal expansion coefficient is measured with an average of (1.5 ± 0.1) × 10−5 K−1 in the range of 300–700 K. The Zn3N2 films are found to be systematically n-type and degenerate, with carrier concentrations of 1019–1021 cm−3 and electron mobilities ranging from 4 to 388 cm2 V−1 s−1. Low-temperature Hall effect measurements show that ionized impurity scattering is the main mechanism limiting the mobility. The large carrier densities lead to measured optical bandgaps in the range of 1.05–1.37 eV due to Moss–Burstein band filling, with an extrapolated value of 0.99 eV for actual bandgap energy.

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