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S. S. A. Seo

Publications and source records attributed to S. S. A. Seo.

At least 19 recordsLinked to original sources

Engineering One-Dimensional Quantum Stripes from Superlattices of Two-Dimensional Layered Materials

One-dimensional (1D) quantum systems, which are predicted to exhibit novel states of matter in theory, have been elusive in experiment. Here we report a superlattice method of creating artificial 1D quantum stripes, which offers dimensional tunability from two- to one-dimensions. As a model system, we have fabricated 1D iridium (Ir) stripes using a-axis oriented superlattices of a relativistic Mott insulator Sr2IrO4 and a wide bandgap insulator LaSrGaO4, both of which are crystals with layered structure. In addition to the successful formation of 1D Ir-stripe structure, we have observed 1D quantum-confined electronic states from optical spectroscopy and resonant inelastic x-ray scattering. Since this 1D superlattice approach can be applied to a wide range of layered materials, it opens a new era of 1D science.

cond-mat.mtrl-sci↗

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 (Sr_{n+1}Ir_{n}O_{3n+1}), conventional PLD methods often result in mixed phases of Sr2IrO4 (n = 1), Sr3Ir2O7 (n = 2), and SrIrO3 (n = infinity). 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-teminated 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.

cond-mat.str-el↗

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 (T_C), 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 T_C 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 for improved device applications.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

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.

cond-mat.mtrl-sci↗

Domain wall conductivity in semiconducting hexagonal ferroelectric TbMnO$_3$ thin films

Although enhanced conductivity at ferroelectric domain boundaries has been found in BiFeO$_3$ films, Pb(Zr,Ti)O$_3$ films, and hexagonal rare-earth manganite single crystals, the mechanism of the domain wall conductivity is still under debate. Using conductive atomic force microscopy, we observe enhanced conductance at the electrically-neutral domain walls in semiconducting hexagonal ferroelectric TbMnO$_3$ thin films where the structure and polarization direction are strongly constrained along the c-axis. This result indicates that domain wall conductivity in ferroelectric rare-earth manganites is not limited to charged domain walls. We show that the observed conductivity in the TbMnO$_3$ films is governed by a single conduction mechanism, namely, the back-to-back Schottky diodes model tuned by the segregation of defects.

cond-mat.mtrl-sci↗

Alleviating polarity-conflict at the heterointerfaces of KTaO$_3$/GdScO$_3$ polar complex-oxides

We have synthesized and investigated the heterointerfaces of KTaO$_3$ (KTO) and GdScO$_3$ (GSO), which are both polar complex-oxides along the pseudo-cubic [001] direction. Since their layers have the same, conflicting net charges at interfaces, i.e. KO(-1)/ScO$_2$(-1) or TaO$_2$(+1)/GdO(+1), forming the heterointerface of KTO/GSO should be forbidden due to strong Coulomb repulsion, the so-called $\textit{polarity conflict}$. However, we have discovered that atomic reconstruction occurs at the heterointerfaces between KTO thin-films and GSO substrates, which effectively alleviates the polarity conflict without destroying the hetero-epitaxy. Our result demonstrates one of the important ways to create artificial heterostructures from polar complex-oxides.

cond-mat.mtrl-sci↗

Compressive strain-induced metal-insulator transition in orthorhombic SrIrO3 thin films

We have investigated the electronic properties of epitaxial orthorhombic SrIrO3 thin-films under compressive strain. The metastable, orthorhombic SrIrO3 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 (\r{ho}) of the thin films increases by a few orders of magnitude, and the d\r{ho}/dT 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 magneto-resistance 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 SrIrO3 thin-films.

cond-mat.str-el↗

Tuning Magnetic Coupling in Sr$_2$IrO$_4$ Thin Films with Epitaxial Strain

We report x-ray resonant magnetic scattering (XRMS) and resonant inelastic x-ray scattering (RIXS) studies of epitaxially-strained $\mathrm{Sr_2IrO_4}$ thin films. The films were grown on $\mathrm{SrTiO_3}$ and $\mathrm{(LaAlO_3)_{0.3}(Sr_2AlTaO_6)_{0.7}}$ substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk $\mathrm{Sr_2IrO_4}$, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature $\mathrm{T_N}$, while raising (lowering) the energy of the zone boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced change in bond lengths.

cond-mat.str-el↗

Epitaxial Ba2IrO4 thin-films grown on SrTiO3 substrates by pulsed laser deposition

We have synthesized epitaxial Ba2IrO4 (BIO) thin-films on SrTiO3 (001) substrates by pulsed laser deposition and studied their electronic structure by dc-transport and optical spectroscopic experiments. We have observed that BIO thin-films are insulating but close to the metalinsulator transition boundary with significantly smaller transport and optical gap energies than its sister compound, Sr2IrO4. Moreover, BIO thin-films have both an enhanced electronic bandwidth and electronic-correlation energy. Our results suggest that BIO thin-films have great potential for realizing the interesting physical properties predicted in layered iridates.

cond-mat.str-el↗

Anisotropic electronic properties of a-axis-oriented Sr2IrO4 epitaxial thin-films

We have investigated the transport and optical properties along the c-axis of a-axis-oriented Sr2IrO4 epitaxial thin-films grown on LaSrGaO4 (100) substrates. The c-axis resistivity is approximately one order of magnitude larger than that of the ab-plane. Optical absorption spectra with E//b polarization show both Ir 5d intersite transitions and charge-transfer transitions (O 2p to Ir 5d), while E//c spectra show only the latter. The structural anisotropy created by biaxial strain in a-axis-oriented thin-films also changes the electronic structure and gap energy. These a-axis-oriented, epitaxial thin-films provide a powerful tool to investigate the highly anisotropic electronic properties of Sr2IrO4.

cond-mat.str-el↗

Tuning electronic structures via epitaxial strain in Sr2IrO4 thin films

We have synthesized epitaxial Sr2IrO4 thin-films on various substrates and studied their electronic structures as a function of lattice-strains. Under tensile (compressive) strains, increased (decreased) Ir-O-Ir bond-angles are expected to result in increased (decreased) electronic bandwidths. However, we have observed that the two optical absorption peaks near 0.5 eV and 1.0 eV are shifted to higher (lower) energies under tensile (compressive) strains, indicating that the electronic-correlation energy is also affected by in-plane lattice-strains. The effective tuning of electronic structures under lattice-modification provides an important insight into the physics driven by the coexisting strong spin-orbit coupling and electronic correlation.

cond-mat.str-el↗

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 (PLD) 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 LaMnO3+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.

cond-mat.mtrl-sci↗

Preparation of atomically-flat SrTiO3 surfaces using a deionized-water etching and thermal annealing procedure

We report that a deionized water etching and thermal annealing technique can be effective for preparing atomically-flat and singly-terminated surfaces of single crystalline SrTiO3 substrates. After a two-step thermal-annealing and deionized-water etching procedure, topography measured by atomic force microscopy shows the evolution of substrates from a rough to step-terraced surface structure. Lateral force microscopy confirms that the atomically-flat surfaces are singly-terminated. Moreover, this technique can be used to remove excessive strontium oxide or hydroxide composites segregated on the SrTiO3 surface. This acid-etchant-free technique facilitates the preparation of atomically-aligned SrTiO3 substrates, which promotes studies on two-dimensional physics of complex oxide interfaces.

cond-mat.mtrl-sci↗

Charge states and magnetic ordering in LaMnO3/SrTiO3 superlattices

We investigated the magnetic and optical properties of [(LaMnO3)n/(SrTiO3)8]20 (n = 1, 2, and 8) superlattices grown by pulsed laser deposition. We found a weak ferromagnetic and semiconducting state developed in all superlattices. An analysis of the optical conductivity showed that the LaMnO3 layers in the superlattices were slightly doped. The amount of doping was almost identical regardless of the LaMnO3 layer thickness up to eight unit cells, suggesting that the effect is not limited to the interface. On the other hand, the magnetic ordering became less stable as the LaMnO3 layer thickness decreased, probably due to a dimensional effect.

cond-mat.str-el↗

Electronic structure and anomalous band-edge absorption feature in multiferroic MnWO4: An optical spectroscopic study

We investigated the electronic structure and lattice dynamics of multiferroic MnWO4 by optical spectroscopy. With variation of polarization, temperature, and magnetic field, we obtained optical responses over a wide range of photon energies. The electronic structure of MnWO4 near to the Fermi level was examined, with inter-band transitions identified in optical conductivity spectra above a band-gap of 2.5 eV. As for the lattice dynamics, we identified all the infrared transverse optical phonon modes available according to the group-theory analysis. Although we did not observe much change in global electronic structure across the phase transition temperatures, an optical absorption at around 2.2 eV showed an evident change depending upon the spin configuration and magnetic field. The behavior of this band-edge absorption indicates that spin-orbit coupling plays an important role in multiferroic MnWO4.

cond-mat.str-el↗

Nonlinear Hall effect and multichannel conduction in LaTiO3/SrTiO3 superlattices

We report magneto-transport properties of heterointerfaces between the Mott insulator LaTiO3 and the band insulator SrTiO3 in a delta-doping geometry. At low temperatures, we have found a strong nonlinearity in the magnetic field dependence of the Hall resistivity, which can be effectively controlled by varying the temperature and the electric field. We attribute this effect to multichannel conduction of interfacial charges generated by an electronic reconstruction. In particular, the formation of a highly mobile conduction channel revealed by our data is explained by the greatly increased dielectric permeability of SrTiO3 at low temperatures, and its electric-field dependence reflects the spatial distribution of the quasi-two-dimensional electron gas.

cond-mat.str-el↗

Two-Dimensional Confinement of 3d1 Electrons in LaTiO3/LaAlO3 Multilayers

We report spectroscopic ellipsometry measurements of the anisotropy of the interband transitions parallel and perpendicular to the planes of (LaTiO3)n(LaAlO3)5 multilayers with n = 1-3. These provide direct information about the electronic structure of the two-dimensional (2D) 3d^1 state of the Ti ions. In combination with LDA+U calculations, we suggest that 2D confinement in the TiO2 slabs lifts the degeneracy of the t_{2g} states leaving only the planar d_xy orbitals occupied. We outline that these multilayers can serve as a model system for the study of the t_{2g} 2D Hubbard model.

cond-mat.str-el↗