Single-Crystalline Thin Films for Studying Intrinsic Properties of BiFeO3–SrTiO3 Solid Solution Photoelectrodes in Solar Energy Conversion

Solid solutions have been widely investigated for solar energy conversion because of the ease to control properties (e.g., band edge positions, charge carrier transport, and chemical stability). In this study, we introduce a new method to investigate intrinsic solar energy conversion properties of solid solutions through fabricating high-quality single-crystalline solid solution films by pulsed laser deposition. This method rules out external factors, such as morphology, crystalline grain size, orientation, density and distribution, surface area, and particle–particle or particle–conducting layer connection, that have plagued previous studies on solid solution photoelectrodes. Perovskite BiFeO3 (BFO) and SrTiO3 (STO) were chosen as "end" members of the solid solutions (i.e., (BFO)x(STO)1–x (0 ≤ x ≤ 1)). Optical and photoelectrochemical (PEC) properties of the solid solutions significantly varied with changing compositions. Among the six studied compositions, BFO:STO (3:1 molar ratio) exhibited the highest photocurrent density with the photovoltage of 1.08 V. The photoelectrode also produced stable photocurrent for 12 h. Faradaic efficiencies of H2 and O2 formation close to 100% were measured.