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The below bandgap optical transitions of an aluminum nitride (AlN) crystal grown on a tungsten (W) substrate by physical vapor transport (PVT) are investigated by below-bandgap-excited photoluminescence (PL) spectroscopy and first-principles calculations. Oxygen (O) is the only impurity in the AlN-on-W crystal grown by PVT. By analyzing the excitation-power-, excitation-photon-energy-, and temperature-dependence of the PL spectra, the emission peaks of defect complexes involving aluminum vacancy (VAl) and substitutional oxygen (ON) with different spatial and atomic configurations, i.e., VAl–ON and VAl–2ON with ON featuring axial or basal configurations, are identified. It is revealed that two different charging states coexist in thermal equilibrium for each configuration of VAl–ON complexes. The optical transitions between the conduction band and (VAl–ON)2− and/or (VAl–2ON)1− contribute the UV emissions and those between the valence band and (VAl–ON)1− or (VAl–2ON)0 contribute the red emissions.