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The heteroepitaxial growth of fullerene (C) on single-crystal black phosphorus (BP) has been studied using low-energy electron diffraction, X-ray and ultraviolet photoelectron spectroscopy, and density functional theory simulation. The occupied orbital features from C observed in the photoelectron spectra for C/BP interface are slightly broadened at higher coverages of C and exhibit no direct evidence of hybridization, demonstrating that the C/BP interaction is physisorption. Oxygen exposure of interface leads to obvious oxidation of BP in which C bridges the large electron-transfer barrier from BP to oxygen and plays an important role for the production of O and oxidation of BP. Our findings suggest that C does not form an ideal protection layer as the other n-type semiconductors. With the assistance of density functional theory calculations, the oxidized phosphorus at the interface prevents further charge transfer from BP to C.

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