Single-phase epitaxial films of the monoclinic polymorph of BiVO4 were synthesized by reactive molecular-beam epitaxy under adsorption-controlled conditions. The BiVO4 films were grown on (001) yttria-stabilized cubic zirconia (YSZ) substrates. Four-circle x-ray diffraction, scanning transmission electron microscopy (STEM), and Raman spectroscopy confirm the epitaxial growth of monoclinic BiVO4 with an atomically abrupt interface and orientation relationship (001)BiVO4 ∥ (001)YSZ with [100]BiVO4 ∥ [100]YSZ. Spectroscopic ellipsometry, STEM electron energy loss spectroscopy (STEM-EELS), and x-ray absorption spectroscopy indicate that the films have a direct band gap of 2.5 ± 0.1 eV.
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