Self-Assembled Heteroepitaxial Oxide Nanocomposite for Photoelectrochemical Solar Water Oxidation

[Image: see text] We report on spontaneously phase ordered heteroepitaxial SrTiO(3) (STO):ZnFe(2)O(4) (ZFO) nanocomposite films that give rise to strongly enhanced photoelectrochemical solar water oxidation, consistent with enhanced photoinduced charge separation. The STO:ZFO nanocomposite yielded an enhanced photocurrent density of 0.188 mA/cm(2) at 1.23 V vs a reversible hydrogen electrode, which was 7.9- and 2.6-fold higher than that of the plain STO film and ZFO film cases under 1-sun illumination, respectively. The photoelectrode also produced stable photocurrent and Faradaic efficiencies of H(2) and O(2) formation that were more than 90%. Incident-photon-to-current-conversion efficiency measurements, Tauc plots, Mott–Schottky plots, and electrochemical impedance spectroscopy measurements proved that the strongly enhanced photogenerated charge separation resulted from vertically aligned pseudosingle crystalline components, epitaxial heterojunctions, and a staggered band alignment of the components of the nanocomposite films. This study presents a completely new avenue for efficient solar energy conversion applications.