Abstract
The growth of epitaxial Zn3P2 films on III–V substrates unlocks a promising pathway toward high-efficiency, earth-abundant photovoltaic devices fabricated on reusable, single-crystal templates. The detailed chemical, structural, and electronic properties of the surface and interface of pseudomorphic Zn3P2 epilayers grown on GaAs(001) were investigated using scanning tunneling microscopy/spectroscopy and high-resolution X-ray photoelectron spectroscopy. Two interesting features of the growth process were observed: (1) vapor-phase P4 first reacts with the Ga-rich GaAs surface to form an interfacial GaP layer with a thickness of several monolayers, and (2) a P-rich amorphous overlayer is present during the entire film growth process, beneath which a highly ordered Zn3P2 crystalline phase is precipitated. These features were corroborated by transmission electron micrographs of the Zn3P2/GaAs interface as well as density functional theory calculations of P reactions with the GaAs surface. Finally, the valence-band offset between the crystalline Zn3P2 epilayer and the GaAs substrate was determined to be ΔEV = 1.0 ± 0.1 eV, indicating the formation of a hole-depletion layer at the substrate surface which may inhibit formation of an ohmic contact.
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