Conducting LaAlO3/SrTiO3 heterointerfaces on atomically flat substrates prepared by deionized-water

We have investigated how the recently-developed water-leaching method for atomically-flat SrTiO3 (STO) substrates affects the transport properties of LaAlO3 (LAO) and STO heterointerfaces. Using pulsed laser deposition at identical growth conditions, we have synthesized epitaxial LAO thin-films on two different STO substrates, which are prepared by water-leaching and buffered hydrofluoric acid (BHF) etching methods. The structural, transport, and optical properties of LAO/STO heterostructures grown on water-leached substrates show the same high-quality as the samples grown on BHF-etched substrates. These results indicate that the water-leaching method can be used to grow complex oxide heterostructures with atomically well-defined heterointerfaces without safety concerns.Comment: 10 pages, 4 figure

Conducting LaAlO\u3csub\u3e3\u3c/sub\u3e/SrTiO\u3csub\u3e3\u3c/sub\u3e Heterointerfaces on Atomically-Flat Substrates Prepared by Deionized-Water

We have investigated how the recently-developed water-leaching method for atomically-flat SrTiO3 (STO) substrates affects the transport properties of LaAlO3 (LAO) and STO heterointerfaces. Using pulsed laser deposition at identical growth conditions, we have synthesized epitaxial LAO thin-films on two different STO substrates, which are prepared by water-leaching and buffered hydrofluoric acid (BHF) etching methods. The structural, transport, and optical properties of LAO/STO heterostructures grown on water-leached substrates show the same high-quality as the samples grown on BHF-etched substrates. These results indicate that the water-leaching method can be used to grow complex oxide heterostructures with atomically well-defined heterointerfaces without safety concerns

Electronic and Optical Properties of La-Doped Sr\u3csub\u3e3\u3c/sub\u3eIr\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e7\u3c/sub\u3e Epitaxial Thin Films

We have investigated structural, transport, and optical properties of tensile strained (Sr1−xLax)3Ir2O7 (x = 0, 0.025, 0.05) epitaxial thin films. While high-Tc superconductivity is predicted theoretically in the system, we have observed that all of the samples remain insulating with finite optical gap energies and Mott variable-range hopping characteristics in transport. Cross-sectional scanning transmission electron microscopy indicates that structural defects such as stacking faults appear in this system. The insulating behavior of the La-doped Sr3Ir2O7 thin films is presumably due to disorder-induced localization and ineffective electron doping of La, which brings to light the intriguing difference between epitaxial thin films and bulk single crystals of the iridates

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

Optical Signatures of Spin-Orbit Exciton in Bandwidth-Controlled Sr\u3csub\u3e2\u3c/sub\u3eIrO\u3csub\u3e4\u3c/sub\u3e Epitaxial Films via High-Concentration Ca and Ba Doping

We have investigated the electronic and optical properties of (Sr1−xCax)2IrO4 (x = 0–0.375) and (Sr1−yBay)2IrO4 (y = 0–0.375) epitaxial thin films, in which the bandwidth is systematically tuned via chemical substitutions of Sr ions by Ca and Ba. Transport measurements indicate that the thin-film series exhibits insulating behavior, similar to the Jeff = 1/2 spin-orbit Mott insulator Sr2IrO4. As the average A-site ionic radius increases from (Sr1−xCax)2IrO4 to (Sr1−yBay)2IrO4, optical conductivity spectra in the near-infrared region shift to lower energies, which cannot be explained by the simple picture of well-separated Jeff = 1/2 and Jeff = 3/2 bands. We suggest that the two-peak-like optical conductivity spectra of the layered iridates originates from the overlap between the optically forbidden spin-orbit exciton and the intersite optical transitions within the Jeff = 1/2 band. Our experimental results are consistent with this interpretation as implemented by a multiorbital Hubbard model calculation: namely, incorporating a strong Fano-like coupling between the spin-orbit exciton and intersite d−d transitions within the Jeff = 1/2 band

Enhanced Metallic Properties of SrRuO\u3csub\u3e3\u3c/sub\u3e Thin Films via Kinetically Controlled Pulsed Laser Epitaxy

Metal electrodes are a universal element of all electronic devices. Conducting SrRuO3 (SRO) epitaxial thin films have been extensively used as electrodes in complex-oxide heterostructures due to good lattice mismatches with perovskite substrates. However, when compared to SRO single crystals, SRO thin films have shown reduced conductivity and Curie temperatures (TC), which can lead to higher Joule heating and energy loss in the devices. Here, we report that high-quality SRO thin films can be synthesized by controlling the plume dynamics and growth rate of pulsed laser epitaxy (PLE) with real-time optical spectroscopic monitoring. The SRO thin films grown under the kinetically controlled conditions, down to ca. 16 nm in thickness, exhibit both enhanced conductivity and TC as compared to bulk values, due to their improved stoichiometry and a strain-mediated increase of the bandwidth of Ru 4d electrons. This result provides a direction for enhancing the physical properties of PLE-grown thin films and paves a way to improved device applications