Iron oxide (α-Fe2O3, hematite), aka rust, is one of few materials meeting these criteria, but its poor transport properties and fast charge recombination present challenges for efficient charge carrier generation, separation and collection. We explore innovative solutions to these challenges using ultrathin (20-30 nm) films on specular back reflectors. This simple optical cavity design effectively traps the light in otherwise nearly translucent ultrathin films, amplifying the intensity close to the surface wherein photogenerated charge carriers can reach the surface and split water before recombination takes place. This is the enabling key towards the development of high-efficiency iron oxide photoelectrodes whose structure and properties can be tailored by design. However, the design rules for these devices remain elusive because iron oxide behaves differently than conventional semiconductors such as silicon, probably due to the strong correlation between the electrons that give rise to the current and the ions that form the crystalline lattice.
Our first goal is to discover the physico-chemical processes that limit the performance of iron oxide photoelectrode and devise design principles that enable overcoming these limitations through material design at the nanoscale that combines iron oxide together with selective underlayers and overlayers that separate positive and negative charge carriers, thereby reducing recombination losses and increasing efficiency. The second goal is to apply these design principles to construct high-efficiency solar water splitting devices. The third and final goal is to invent new device architectures and operation schemes that enable affordable solar hydrogen production in large-scale applications, closing the gap between basic research on lab-scale devices and a new solar energy technology that provides stable power on demand.