Titanium and Magnesium Co-Alloyed Hematite Thin Films for Photoelectrochemical Water Splitting

Using a combination of density functional theory calculation and materials synthesis and characterization we examine the properties of charge-compensated Ti and Mg co-alloyed hematite thin films for the application of photoelectrochemical (PEC) water splitting. We find that the charge-compensated co-alloying results in the following effects: (1) It enhances the solubility of Mg and Ti, which leads to reduced electron effective mass and therefore increased electron mobility; (2) It tunes the carrier density and therefore allows the optimization of electrical conductivity; and (3) It reduces the density of charged defects and therefore reduces carrier recombination. As a result, the Ti and Mg co-alloyed hematite thin films exhibit improved water oxidation photocurrent magnitudes as compared to pure hematite thin films. Our results suggest that charge-compensated co-alloying is a plausible approach for engineering hematite for the application of PEC water splitting.