Selective Growth of Epitaxial Sr\u3csub\u3e2\u3c/sub\u3eIrO\u3csub\u3e4\u3c/sub\u3e by Controlling Plume Dimensions in Pulsed Laser Deposition

We report that epitaxial Sr2IrO4 thin-films can be selectively grown using pulsed laser deposition (PLD). Due to the competition between the Ruddlesden-Popper phases of strontium iridates (Srn+1IrnO3n+1), conventional PLD methods often result in mixed phases of Sr2IrO4 (n = 1), Sr3Ir2O7 (n = 2), and SrIrO3 (n = ∞). We have discovered that reduced PLD plume dimensions and slow deposition rates are the key for stabilizing pure Sr2IrO4 phase thin-films, identified by real-time in-situ monitoring of their optical spectra. The slow film deposition results in a thermodynamically stable TiO2\\SrO\IrO2\SrO\SrO configuration at an interface rather than TiO2\\SrO\SrO\IrO2\SrO between a TiO2-terminated SrTiO3 substrate and a Sr2IrO4 thin film, which is consistent with other layered oxides grown by molecular beam epitaxy. Our approach provides an effective method for using PLD to achieve pure phase thin-films of layered materials that are susceptible to several energetically competing phases