Layered oxides have been intensively studied due to their high designability for various electronic functions. Here we synthesize a new oxide as epitaxial thin film form by pulsed laser deposition. Film characterizations including cross-section and plan-view transmission electron microscopy confirm that the film is composed of twisted stack of triangular-lattice Rh and Bi layers. We foresee that the concept of twisted oxide layers will open up a new route to design further functional layered oxides.
Synthesizing metastable phase often opens new functions in materials but is a challenging topic. Thin film techniques have advantages to form materials which do not exist in nature since nonequilibrium processes are frequently utilized. In this study, we successfully synthesize epitaxially stabilized new compound of perovskite Eu2+Mo4+O3 as a thin film form by a pulsed laser deposition. Analogous perovskite SrMoO3 is a highly conducting paramagnetic material, but Eu2+ and Mo4+ are not compatible in equilibrium and previous study found more stable pyrochlore Eu23+Mo24+O7 prefers to form. By usi…
Single-crystalline thin film of an iridium dioxide polymorph Ir2O4 has been fabricated by the pulsed laser deposition of LixIr2O4 precursor and the subsequent Li-deintercalation using soft chemistry. Ir2O4 crystallizes in a spinel (AB2O4) without A cations in the tetrahedral site, which is isostructural to lambda-MnO2. Ir ions form a pyrochlore sublattice, which is known to give rise to a strong geometrical frustration. This Ir spinel was found to be a narrow gap insulator, in remarkable contrast to the metallic ground state of rutile-type IrO2. We argue that an interplay of strong spin-orbit …
We report the formation and observation of an electron liquid in Sr$_{2-x}$La$_{x}$TiO$_4$, the quasi-two-dimensional counterpart of SrTiO$_3$, through reactive molecular-beam epitaxy and {\it in situ} angle-resolved photoemission spectroscopy. The lowest lying states are found to be comprised of Ti 3$d_{xy}$ orbitals, analogous to the LaAlO$_3$/SrTiO$_3$ interface and exhibit unusually broad features characterized by quantized energy levels and a reduced Luttinger volume. Using model calculations, we explain these characteristics through an interplay of disorder and electron-phonon coupling a…
We report on the synthesis and transport properties of perovskite (Pv) CaIrO3 thin films. The Pv phase of CaIrO3 was stabilized by epitaxial growth on SrTiO3, (LaAlO3)0.3(Sr2AlTaO6)0.7, and LaAlO3 substrates with strong tensile, weak tensile, and compressive strains, respectively. The resistivity of these films showed a poorly metallic behavior. The Hall resistivity exhibited a sign change as a function of temperature and a nonlinear magnetic-field dependence, which clearly indicated the coexistence of electrons and holes and hence supported that Pv CaIrO3 films are semimetallic. The observed …
EuIn2Sb2: epitaxially stabilized axion insulator candidate with strong spin-orbit coupling
Institute of Science Tokyo（东京科学大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所 新兴物质科学中心）；Toyota Physical and Chemical Research Institute（丰田物理化学研究所）
We have studied the atomic ordering of B-site transition metals and magnetic properties in the pulsed-laser deposited films of La2CrFeO6 (LCFO) and La2VMnO6 (LVMO), whose bulk materials are known to be single perovskites with random distribution of the B-site cations. Despite similar ionic characters of constituent transition metals in each compound, the maximum B-site order attained was surprisingly high, ~90% for LCFO and ~80% for LVMO, suggesting a significant role of epitaxial stabilization in the spontaneous ordering process. Magnetization and valence state characterizations revealed that…
Gilbert Damping Parameters of Epitaxially-Stabilized Iron Gallium Thin Films from Ferromagnetic Resonance
The Ferroelectronics Laboratory, University of Michigan（密歇根大学铁电实验室）；Imec（imec研究所）；Department of Materials Science and Engineering, University of Wisconsin-Madison（威斯康星大学麦迪逊分校材料科学与工程系）
We fabricated epitaxial thin films of hexagonal DyMnO3, which otherwise form in a bulk perovskite structure, via deposition on Pt(111)//Al2O3 (0001) and YSZ(111) substrates: each of which has in-plane hexagonal symmetry. The polarization hysteresis loop demonstrated the existence of ferroelectricity in our hexagonal DyMnO3 films at least below 70 K. The observed 2.2 uC/cm^2 remnant polarization at 25 K corresponded to a polarization enhancement by a factor of 10 compared to that of the bulk orthorhombic DyMnO3. Interestingly, this system showed an antiferroelectric-like feature in its hysteres…
Fast, reversible redox reactions in solids at low temperatures without thermomechanical degradation are a promising strategy for enhancing the overall performance and lifetime of many energy materials and devices. However, the robust nature of the cation's oxidation state and the high thermodynamic barrier have hindered the realization of fast catalysis and bulk diffusion at low temperatures. Here, we report a significant lowering of the redox temperature by epitaxial stabilization of strontium cobaltites (SrCoOx) grown directly as one of two distinct crystalline phases, either the perovskite …
La2/3Ca1/3MnO3 thin films have been grown on yttria-stabilized zirconia (YSZ) buffered silicon-on-insulator (SOI) substrate by the pulsed laser deposition technique. While full cube-on-cube epitaxy was achieved for the YSZ layer, the top manganite layer was multi-domain-oriented, with a coexistence of cube-on-cube and cube-on-diagonal epitaxy. Due to a combined influence from the magnetocrystalline anisotropy and the magnetoelastic anisotropy, in zero field the local spin orientation varies across the twin boundaries. As a result, a quite large low-field magnetoresistance (LFMR) based on spin-…
Pressure-induced superconductivity in epitaxially-stabilized Pr$_3$Ni$_2$O$_7$ films
The University of Tokyo（东京大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所新兴物质科学中心）；Institute for Materials Research (IMR), Tohoku University（东北大学物质材料研究机构）；Advanced Institute for Materials Research (WPI-AIMR), Tohoku University（东北大学先进物质材料研究机构）；Tokyo College, The University of Tokyo（东京大学东京学院）
The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in two-dimensional materials. We report a novel $\sqrt{19}\times\sqrt{19}$ charge order in few-layer thick 1T-TaTe$_2$ transition metal dichalcogenide films grown by molecular beam epitaxy, which has not been realized. Our photoemission and scanning probe measurements demonstrate that monolayer 1T-TaTe$_2$ exhibits a variety of metastable charge density wave orders, including the $\sqrt{19}\times\sqrt{19}$ superstructure, which can be selectively stabili…
The low temperature properties of double exchange model in triangular lattice are investigated via truncated polynomial expansion method (TPEM), which reduces the computational complexity and enables parallel computation. We found that for the half-filling case a stable 120-degree spin configuration phase occurs owing to the frustration of triangular lattice and is further stabilized by antiferromagnetic (AF) superexchange interaction, while a transition between a stable ferromagnetic (FM) phase and a unique flux phase with small finite-size effect is induced by AF superexchange interaction fo…
We present a combination of thermodynamic and dynamic experimental signatures of a disorder driven dynamic cooperative paramagnet in a 50% site diluted triangular lattice spin-1/2 system, Y$_2$CuTiO$_6$. Magnetic ordering and spin freezing are absent down to 50 mK, far below the Curie Weiss scale of ~-134 K. We observe scaling collapses of the magnetic field- and temperature-dependent magnetic heat capacity and magnetisation data, respectively, in conformity with expectations from the random singlet physics. Our experiments establish the suppression of any freezing scale, if at all present, by…
A triangular lattice selenide series of rare earth (RE), CsRESe2, were synthesized as large single crystals using a flux growth method. This series stabilized in either trigonal (R-3m) or hexagonal (P63/mmc) crystal systems. Physical properties of CsRESe2 were explored by magnetic susceptibility and heat capacity measurements down to 0.4 K. Antiferromagnetic interaction was observed in all magnetic compounds, while no long-range magnetic order was found, indicating the frustrated magnetism. CsDySe2 presents spin freezing at 0.7 K, revealing a spin-glass state. CsCeSe2 and CsYbSe2 present broad…
The spin-1/2 triangular lattice antiferromagnet YbMgGaO$_{4}$ has attracted recent attention as a quantum spin-liquid candidate with the possible presence of off-diagonal anisotropic exchange interactions induced by spin-orbit coupling. Whether a quantum spin-liquid is stabilized or not depends on the interplay of various exchange interactions with chemical disorder that is inherent to the layered structure of the compound. We combine time-domain terahertz spectroscopy and inelastic neutron scattering measurements in the field polarized state of YbMgGaO$_{4}$ to obtain better microscopic insig…
5d iridates have shown vast emergent phenomena due to a strong interplay among its lattice, charge and spin degrees of freedom, because of which the potential in spintronic application of the thin-film form is highly leveraged. Here we have epitaxially stabilized perovskite SrIr$_{0.8}$Sn$_{0.2}$O$_3$ on [001] SrTiO$_3$ substrates through pulsed laser deposition and systematically characterized the structural, electronic and magnetic properties. Physical properties measurements unravel an insulating ground state with a weak ferromagnetism in the compressively strained epitaxial film. The octah…
BiFeO3 thin films with various thicknesses were grown epitaxially on (001) LaSrAlO4 single crystal substrates using pulsed laser deposition. High resolution x-ray diffraction measurements revealed that a tetragonal-like phase with c-lattice constant ~4.65 Å is stabilized by a large misfit strain. Besides, a rhombohedral-like phase with c-lattice constant ~3.99 Å was also detected at film thickness of ~50 nm and above to relieve large misfit strains. In-plane piezoelectric force microscopy studies showed clear signals and self-assembled nanoscale stripe domain structure for the tetragonal-like …
The electronic and magnetic properties in ABO3 perovskite oxides are extremely sensitive to lattice structure but also the dimensionality, such as the thickness in thin film form. Here, we report the thickness-dependent electro-magnetic properties of ultrathin epitaxially stabilized Sr1-xBaxRuO3 (x = 0.08, 0.2) thin films on SrTiO3 (001) substrate. The results reveal that the Ba-doping (0.08 < x < 0.20) reduces RuO6 orthorhombic distortions existing in SrRuO3 and induces a tetragonal distortion as evidenced by out-of-plane lattice expansion. A metal-to-insulator transition, accompanied by a fe…
Dielectric and magnetic phenomena in spin and charge frustrated system RFe2O4 (R is a rare-earth metal ion) are studied. An electronic model for charge, spin and orbital degrees in a pair of triangular-lattice planes is derived. We analyze this model by utilizing the mean-field approximation and the Monte-Carlo simulation in a finite size cluster. A three fold-type charge ordered structure with charge imbalance between the planes is stabilized in finite temperatures. This polar charge order is reinforced by spin ordering of Fe ions. This novel magneto-dielectric phenomenon is caused by spin fr…
A variety of nickel oxide compounds have long been studied for their manifestation of various correlated electron phenomena. Recently, superconductivity was observed in nanoscale infinite layer nickelate thin films of Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, epitaxially stabilized on SrTiO$_3$ substrates via topotactic reduction from the perovskite precursor phase. Here we present the synthesis and properties of PrNiO$_2$ thin films on SrTiO$_3$. Upon doping in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$, we observe superconductivity with a transition temperature of 7-12 K, and robust critical current density at 2 K of 3…
While pyrochlore iridate thin films are theoretically predicted to possess a variety of emergent topological properties, experimental verification of these predictions can be obstructed by the challenge in thin film growth. Here we report on the pulsed laser deposition and characterization of thin films of a representative pyrochlore compound Bi2Ir2O7. The films were epitaxially grown on yttria-stabilized zirconia substrates and have lattice constants that are a few percent larger than that of the bulk single crystals. The film composition shows a strong dependence on the oxygen partial pressu…
The Johns Hopkins University（约翰斯·霍普金斯大学）；Institute for Quantum Matter, William H. Miller III Department of Physics and Astronomy（量子物质研究所，威廉·H·米勒三世物理与天文系）；Quantum Matter Institute, University of British Columbia（不列颠哥伦比亚大学量子物质研究所）；Neutron Scattering Division, Oak Ridge National Laboratory（橡树岭国家实验室中子散射部）；Department of Physics & Astronomy, University of British Columbia（不列颠哥伦比亚大学物理与天文系）；Centre for Molecular and Materials Science, TRIUMF（TRIUMF分子与材料科学中心）
Here we demonstrate a new monoclinic iron oxide phase (μ-Fe$_{2}$O$_{3}$), epitaxially stabilized by growth on (010) β-Ga$_{2}$O$_{3}$. Density functional theory (DFT) calculations find that the lattice parameters of freestanding μ-Fe$_{2}$O$_{3}$ are within ~1% of those of β-Ga$_{2}$O$_{3}$ and that its energy of formation is comparable to that of naturally abundant Fe$_{2}$O$_{3}$ polytypes. A superlattice of μ-Fe$_{2}$O$_{3}$/β-Ga$_{2}$O$_{3}$ is grown by plasma assisted molecular beam epitaxy, with resulting high-resolution x-ray diffraction (XRD) measurements indicating that the μ-Fe$_{2}…
