Yellow luminescence (YL) is probably the longest and most studied defect-related luminescence band in GaN, yet its electronic structure or chemical identity remain unclear. Most of the theoretical work so far has attributed the feature to bulk defects, whereas spectroscopic studies have suggested a surface origin. Here, we apply deep level spectroscopy using sub-bandgap surface photovoltage that provides the energy distribution of the surface charge density. Comparison of surface charge spectra obtained under identical conditions before and after various surface treatments reveals the dynamics of the surface charge density. Further comparison with spectra of the entire state obtained using photoluminescence shows how the charge density stored in YL-related defects is eliminated upon a mild anneal in vacuum. This suggests that the YL-related defect involves a certain molecule adsorbed on the GaN surface, possibly in a complex with an intrinsic surface defect. The observed interaction with air strongly indicates that the YL-related deep level is a surface state.
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