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Jeon, Seokmin,Bosco, Jeffrey P.,Wilson, Samantha S.,Rozeveld, Steve J.,Kim, Hyungjun,Atwater, Harry A. American Chemical Society 2014 The Journal of Physical Chemistry Part C Vol.118 No.24
<P>The growth of epitaxial Zn<SUB>3</SUB>P<SUB>2</SUB> 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 Zn<SUB>3</SUB>P<SUB>2</SUB> 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 P<SUB>4</SUB> 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 Zn<SUB>3</SUB>P<SUB>2</SUB> crystalline phase is precipitated. These features were corroborated by transmission electron micrographs of the Zn<SUB>3</SUB>P<SUB>2</SUB>/GaAs interface as well as density functional theory calculations of P reactions with the GaAs surface. Finally, the valence-band offset between the crystalline Zn<SUB>3</SUB>P<SUB>2</SUB> epilayer and the GaAs substrate was determined to be Δ<I>E</I><SUB>V</SUB> = 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.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpccck/2014/jpccck.2014.118.issue-24/jp4127804/production/images/medium/jp-2013-127804_0010.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/jp4127804'>ACS Electronic Supporting Info</A></P>