John H. Gruenewald

Compressive strain-induced metal–insulator transition in orthorhombic SrIrO 3 thin films

Orthorhombic SrIrO 3 is a correlated metal whose electronic properties are highly susceptible to external perturbations due to the comparable interactions of spin–orbit interaction and electronic correlation. We have investigated the electronic properties of epitaxial orthorhombic SrIrO 3 thin-films under compressive strain using transport measurements, optical absorption spectra, and magnetoresistance. The metastable, orthorhombic SrIrO 3 thin-films are synthesized on various substrates using an epi-stabilization technique. We have observed that as in-plane lattice compression is increased, the dc-resistivity (ρ) of the thin films increases by a few orders of magnitude, and the dρ/d T changes from positive to negative values. However, optical absorption spectra show Drude-like, metallic responses without an optical gap opening for all compressively strained thin films. Transport measurements under magnetic fields show negative magnetoresistance at low temperature for compressively strained thin-films. Our results suggest that weak localization is responsible for the strain-induced metal–insulator transition for the orthorhombic SrIrO 3 thin-films.

Pulsed laser deposition with simultaneous in situ real-time monitoring of optical spectroscopic ellipsometry and reflection high-energy electron diffraction

We present a pulsed laser deposition system that can monitor growth by simultaneously using in situ optical spectroscopic ellipsometry (SE) and reflection high-energy electron diffraction (RHEED). The RHEED precisely monitors the number of thin-film layers and surface structure during the deposition, and the SE measures the optical spectra of the samples simultaneously. The thin-film thickness information obtained from RHEED facilitates the SE modeling process, which allows extracting the in situ optical spectra, i.e., the dielectric functions of thin-films during growth. The in situ dielectric functions contain indispensable information about the electronic structure of thin-films. We demonstrate the performance of this system by growing LaMnO(3+δ) (LMO) thin-films on SrTiO3 (001) substrates. By using in situ SE and RHEED simultaneously, we show that real-time thickness and dielectric functions of the LMO thin-films can be effectively extracted. The simultaneous monitoring of both optical SE and RHEED offers important clues to understand the growth mechanism of atomic-scale thin-films.

Selective growth of epitaxial Sr2IrO4 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.

Engineering 1D Quantum Stripes from Superlattices of 2D Layered Materials.

Dimensional tunability from two dimensions to one dimension is demonstrated for the first time using an artificial superlattice method in synthesizing 1D stripes from 2D layered materials. The 1D confinement of layered Sr2 IrO4 induces distinct 1D quantum-confined electronic states, as observed from optical spectroscopy and resonant inelastic X-ray scattering. This 1D superlattice approach is generalizable to a wide range of layered materials.

Enhanced metallic properties of SrRuO3 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...

Investigations of metastable Ca2IrO4 epitaxial thin-films: systematic comparison with Sr2IrO4 and Ba2IrO4

We have synthesized thermodynamically metastable Ca2IrO4 thin-films on YAlO3 (110) substrates by pulsed laser deposition. The epitaxial Ca2IrO4 thin-films are of K2NiF4-type tetragonal structure. Transport and optical spectroscopy measurements indicate that the electronic structure of the Ca2IrO4 thin-films is similar to that of Jeff = 1/2 spin-orbit-coupled Mott insulator Sr2IrO4 and Ba2IrO4, with the exception of an increased gap energy. The gap increase is to be expected in Ca2IrO4 due to its increased octahedral rotation and tilting, which results in enhanced electron-correlation, U/W. Our results suggest that the epitaxial stabilization growth of metastable-phase thin-films can be used effectively for investigating layered iridates and various complex-oxide systems.

Optical Signatures of Spin-Orbit Exciton in Bandwidth-Controlled Sr 2 IrO 4 Epitaxial Films via High-Concentration Ca and Ba Doping

We have investigated the electronic and optical properties of (Sr

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

_{1-x}

Electronic and optical properties of La-doped Sr3Ir2O7 epitaxial thin films

Ca

Unconventional anomalous Hall effect from antiferromagnetic domain walls of Nd2Ir2O7 thin films

_{x}