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The surface electronic properties of bulk-grown β-Ga2O3 (2¯01) single crystals are investigated. The band gap is found using optical transmission to be 4.68 eV. High-resolution x-ray photoemission coupled with hybrid density functional theory calculation of the valence band density of states provides insights into the surface band bending. Importantly, the standard linear extrapolation method for determining the surface valence band maximum (VBM) binding energy is found to underestimate the separation from the Fermi level by ∼0.5 eV. According to our interpretation, most reports of surface electron depletion and upward band bending based on photoemission spectroscopy actually provide evidence of surface electron accumulation. For uncleaned surfaces, the surface VBM to Fermi level separation is found to be 4.95 ± 0.10 eV, corresponding to downward band bending of ∼0.24 eV and an electron accumulation layer with a sheet density of ∼5 × 1012 cm−2. Uncleaned surfaces possess hydrogen termination which acts as surface donors, creating electron accumulation and downward band bending at the surface. In situ cleaning by thermal annealing removes H from the surface, resulting in a ∼0.5 eV shift of the surface VBM and formation of a surface electron depletion layer with upward band bending of ∼0.26 eV due to native acceptor surface states. These results are discussed in the context of the charge neutrality level, calculated bulk interstitial hydrogen transition levels, and related previous experimental findings.

Transition from electron accumulation to depletion at β-Ga2O3 surfaces: The role of hydrogen and the charge neutrality level