Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics

We report on the selective fabrication of high-quality Sr${}_2$IrO${}_4$ and SrIrO${}_3$ epitaxial thin films from a single polycrystalline Sr${}_2$IrO${}_4$ target by pulsed laser deposition. Using a combination of X-ray diffraction and photoemission spectroscopy characterizations, we discover that within a relatively narrow range of substrate temperature, the oxygen partial pressure plays a critical role in the cation stoichiometric ratio of the films, and triggers the stabilization of different Ruddlesden-Popper (RP) phases. Resonant X-ray absorption spectroscopy measurements taken at the Ir $L$-edge and the O $K$-edge demonstrate the presence of strong spin-orbit coupling, and reveal the electronic and orbital structures of both compounds. These results suggest that in addition to the conventional thermodynamics consideration, higher members of the Sr${}_{n+1}$Ir${}_n$O${}_{3n+1}$ series can possibly be achieved by kinetic control away from the thermodynamic limit. These findings offer a new approach to the synthesis of ultra-thin films of the RP series of iridates and can be extended to other complex oxides with layered structure.