Many metallic transition-metal oxides turn insulating when grown as films that are only a few unit-cells thick. The microscopic origins of these thickness induced metal-to-insulator transitions however remain under dispute. Here, we simulate the extreme case of a monolayer of an inconspicuous correlated metal -- the strontium vanadate SrVO$_3$ -- deposited on a SrTiO$_3$ substrate. Crucially, our system can have a termination to vacuum consisting of either a SrO or a VO$_2$ top layer. While we find that both lead to Mott insulating behavior at nominal stoichiometry, the phase diagram emerging upon doping -- chemically or through an applied gate voltage -- is qualitatively different. Indeed, our many-body calculations reveal a cornucopia of nonlocal fluctuations associated with (in)commensurate antiferromagnetic, ferromagnetic, as well as stripe and checkerboard orbital ordering instabilities. Identifying that the two geometries yield crystal-field splittings of opposite signs, we elucidate the ensuing phases through the lens of the orbital degrees of freedom. Quite generally, our work highlights that interface and surface reconstruction and the deformation or severing of coordination polyhedra in ultra-thin films drive rich properties that are radically different from the material's bulk physics.
Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO$_3$ as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which persist even in an ultrahigh vacuum environment, are shown to severe…
The ferroelectric (FE) control of electronic transport is one of the emerging technologies in oxide heterostructures. Many previous studies in FE tunnel junctions (FTJs) exploited solely the differences in the electrostatic potential across the FTJs that are induced by changes in the FE polarization direction. Here, we show that in practice the junction current ratios between the two polarization states can be further enhanced by the electrostatic modification in the correlated electron oxide electrodes, and that FTJs with nanometer thin layers can effectively produce a considerably large elec…
Oxide heterointerfaces constitute a rich platform for realizing novel functionalities in condensed matter. A key aspect is the strong link between structural and electronic properties, which can be modified by interfacing materials with distinct lattice symmetries. Here we determine the effect of the cubic-tetragonal distortion of $\text{SrTiO}_3$ on the electronic properties of thin films of $\text{SrIrO}_3$, a topological crystalline metal hosting a delicate interplay between spin-orbit coupling and electronic correlations. We demonstrate that below the transition temperature at 105 K, $\tex…
The electrical transport properties of ultrathin YBCO films have been modified using an electric double layer transistor configuration employing an ionic liquid. The films were grown on SrTiO3 substrates using high pressure oxygen sputtering. A clear evolution from superconductor to insulator was observed in nominally 7 unit cell thick films. Using a finite size scaling analysis, curves of resistance versus temperature, R(T), over the temperature range from 6K to 22K were found to collapse onto a single scaling function, which suggests the the presence of a quantum critical point. However the …
In this paper, we report the electrical and structural properties of the oxide-based metal/ferroelectric/metal (MFM) junctions. The heterostructures are composed of ultrathin layers of La0.7Ca0.3MnO3 (LCMO) as a metallic layer and, BaTiO3 (BTO) as a ferroelectric layer. Junction based devices, having the dimensions of 400 x 200 micom2, have been fabricated upon LCMO/BTO/LCMO heterostructures by photolithography and Ar-ion milling technique. The DC current-voltage (I-V) characteristics of the MFM junctions were carried out. At 300 K, the devices showed the linear (I-V) characteristics, whereas …
Experimental efforts to stabilize ferromagnetism in ultrathin films of transition metal oxides have so far failed, despite expectations based on density functional theory (DFT) and DFT+U. Here, we investigate one of the most promising materials, SrRuO$_3$, and include correlation effects beyond DFT by means of dynamical mean field theory. In agreement with experiment we find an intrinsic thickness limitation for metallic ferromagnetism in SrRuO$_3$ thin films. Indeed, we demonstrate that the realization of ultrathin ferromagnetic films is out of reach of standard thin-film techniques. Proposin…
We report on the emergent magnetic state of (111)-oriented CoCr2O4 ultrathin films sandwiched by Al2O3 in the quantum confined geometry. At the two-dimensional crossover, polarized neutron reflectometry reveals an anomalous enhancement of the total magnetization compared to the bulk value. Synchrotron x-ray magnetic circular dichroism (XMCD) demonstrates the appearance of long-range ferromagnetic ordering of spins on both Co and Cr sublattices. Brillouin function analyses further corroborates that the observed phenomena are due to the strongly altered magnetic frustration, manifested by the on…
We report on the synthesis of ultrathin films of highly distorted EuNiO3 (ENO) grown by interrupted pulse laser epitaxy on YAlO3 (YAO) substrates. Through mapping the phase space of nickelate thin film epitaxy, the optimal growth temperatures were found to scale linearly with the Goldschmidt tolerance factor. Considering the gibbs energy of the expanding film, this empirical trend is discussed in terms of epitaxial stabilization and the escalation of the lattice energy due to lattice distortions and decreasing symmetry. These findings are fundamental to other complex oxide perovskites, and pro…
Metallic oxide SrVO3 represents a prototype system for the study of the mechanism behind thickness-induced metal-to-insulator transition (MIT) or crossover in thin films due to its simple cubic symmetry with one electron in the 3d state in the bulk. Here we report a deviation of chemical composition and distortion of lattice structure existing in the initial 3 unit cells of SrVO3 films grown on SrTiO3 (001) from its bulk form, which shows a direct correlation to the thickness-dependent MIT. In-situ photoemission and scanning tunneling spectroscopy indicate a MIT at the critical thickness of ~3…
The tetragonal phase of chromium (III) oxide, although unstable in the bulk, can be synthesized in epitaxial heterostructures. The theoretical investigation by density functional theory predicts an antiferromagnetic ground state for this compound. We demonstrate experimentally antiferromagnetism up to 40 K in ultrathin films of t-Cr2O3 by electrical measurements exploiting interface effect within a neighboring ultrathin Pt layer. We show that magnetotransport in Pt is affected by both spin-Hall magnetoresistance and magnetic proximity effect while we exclude any role of magnetism for the low-t…
A central issue in the physics of high temperature superconductors is to understand superconductivity within a single copper-oxide layer or bilayer, the fundamental structural unit in the cuprates, and how it is lost with underdoping. As mobile holes are removed from the CuO_2 planes, the transition temperature T_C and superfluid density n_S decrease in a surprisingly correlated fashion in crystals and thick films. We seek to elucidate the intrinsic physics of bilayers in the strongly underdoped regime, near the critical doping level where superconductivity disappears. We report measurements o…
We observed a hump-like feature in Hall effects of SrRuO$_3$ ultrathin films, and systematically investigated it with controlling thicknesses, temperatures and magnetic fields. The hump-like feature is extremely stable, even surviving as a magnetic field is tilted by as much as 85$^\circ$. Based on the atomic-level structural analysis of a SrRuO$_3$ ultrathin film with a theoretical calculation, we reveal that atomic rumplings at the thin-film surface enhance Dzyaloshinskii-Moriya interaction, which can generate stable chiral spin textures and a hump-like Hall effect. Moreover, temperature dep…
Insulator-to-Metal Transition via Magnetic Reconstruction at Oxide Interfaces
CAS Key Laboratory of Magnetic Materials and Devices, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences（中国科学院磁性材料与器件重点实验室，宁波材料技术与工程研究所）；Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences（浙江省磁性材料与应用技术重点实验室，宁波材料技术与工程研究所）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Eastern Institute of Technology（东方理工学院）；International Research Centre Magtop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所磁顶国际研究中心）；CNR-SPIN, UOS Salerno（意大利国家研究委员会自旋中心萨莱诺联合实验室）；Photon Science Division, Paul Scherrer Institut（保罗谢尔研究所光子科学部）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学材料科学与光电工程技术中心）
We report on a systematic study of the temperature-dependent Hall coefficient and thermoelectric power in ultra-thin metallic LaNiO$_3$ films that reveal a strain-induced, self-doping carrier transition that is inaccessible in the bulk. As the film strain varies from compressive to tensile at fixed composition and stoichiometry, the transport coefficients evolve in a manner strikingly similar to those of bulk hole-doped superconducting cuprates with varying doping level. Density functional calculations reveal that the strain-induced changes in the transport properties are due to self-doping in…
Observation of mirror-odd and mirror-even spin texture in ultrathin epitaxially strained RuO2 films
University of Minnesota-Twin Cities（明尼苏达大学双城分校）；Kyung Hee University（庆熙大学）；Rice University（莱斯大学）；Paul Scherrer Institute（保罗谢勒研究所）；Gwangju Institute of Science and Technology (GIST)（光州科学技术院）
Motivated by the goal of realizing topological phases in thin films and heterostructures of correlated oxides, we propose here a quantum anomalous Hall insulator (QAHI) in ultrathin films of double perovskites based on mixed 3d-5d or 3d-4d transition metal ions, grown along the [111] direction. Considering the specific case of ultrathin Ba2FeReO6, we present a theoretical analysis of an effective Hamiltonian derived from first-principles. We establish that a strong spin-orbit coupling at Re site, t2g symmetry of the low-energy d-bands, polarity of its [111] orientation of perovskite structure,…
Magnetism and spin-orbit coupling (SOC) are two quintessential ingredients underlying novel topological transport phenomena in itinerant ferromagnets. When spin-polarized bands support nodal points/lines with band degeneracy that can be lifted by SOC, the nodal structures become a source of Berry curvature; this leads to a large anomalous Hall effect (AHE). Contrary to three-dimensional systems that naturally host nodal points/lines, two-dimensional (2D) systems can possess stable nodal structures only when proper crystalline symmetry exists. Here we show that 2D spin-polarized band structures…
Divergent density of states (DOS) can induce extraordinary phenomena such as significant enhancement of superconductivity and unexpected phase transitions. Moreover, van Hove singularities (VHSs) are known to lead to divergent DOS in two-dimensional (2D) systems. Despite the recent interest in VHSs, only a few controllable cases have been reported to date. In this work, we investigate the electronic band structures of a 2D VHS with angle-resolved photoemission spectroscopy and control transport properties by utilizing an atomically ultrathin SrRuO$_3$ film. By applying electric fields with alk…
The electronic structure of transition metal oxides featuring correlated electrons can be rationalized within the Zaanen-Sawatzky-Allen framework. Following a brief description of the present paradigms of electronic behavior, we focus on the physics of rare earth nickelates as an archetype of complexity emerging within the charge transfer regime. The intriguing prospect of realizing the physics of high $T_c$ cuprates through heterostructuring resulted in a massive endeavor to epitaxially stabilize these materials in ultra-thin form. A plethora of new phenomena unfolded in such artificial struc…
In response to Lu et al, (arXiv:1506.02787v1), here we present a detailed writeup concerning the questions raised in their comment on our eprint (arXiv:1505.07451). The key question raised by Lu et al was if the bulk-like charge ordered state becomes indetectable with resonant scattering due to ultrathin film thickness. In this reply, we first detail the relation of our work to past work on the same compound by Staub et al to demonstrate that the presented data are indeed sufficient to support our claims of no charge order on ultra thin films of NdNiO3 (NNO) on NdGaO3 (NGO). Further, we demons…
Atomically sharp oxide heterostructures often exhibit unusual physical properties that are absent in the constituent bulk materials. The interplay between electrostatic boundary conditions, strain and dimensionality in ultrathin epitaxial films can result in monolayer-scale transitions in electronic or magnetic properties. Here we report an atomically sharp antiferromagnetic-to-ferromagnetic phase transition when atomically growing polar antiferromagnetic LaMnO3 (001) films on SrTiO3 substrates. For a thickness of five unit cells or less, the films are antiferromagnetic, but for six unit cells…
For heterostructures of ultrathin, strongly correlated copper-oxide films and dielectric perovskite layers, we predict inhomogeneous electronic interface states. Our study is based on an extended Hubbard model for the cuprate film. The interface is implemented by a coupling to the electron and phonon degrees of freedom of the dielectric oxide layer. We find that electronic ordering in the film is associated with a strongly inhomogeneous polaron effect. We propose to consider the interfacial tuning as a powerful mechanism to control the charge ordering in correlated electronic systems.
The 5$d$ transition metal oxides, in particular iridates, host novel electronic and magnetic phases due to the interplay between onsite Coulomb repulsion ($U$) and spin-orbit coupling (SOC). The reduced dimensionality brings another degree of freedom to increase the functionality of these systems. By taking the example of ultrathin films of SrIrO$_3$,theoretically, we demonstrate that confinement led localization can introduce large magnetic anisotropy energy (MAE) in the range 2-7 meV/Ir which is one to two orders higher than that of the traditional MAE compounds formed out of transition meta…
Unique superconductivity at surfaces/interfaces, as exemplified by LaAlO3/SrTiO3 interfaces, and the high transition temperature in ultrathin FeSe films, have triggered intense debates on how superconductivity is affected in atomic and electronic reconstructions. The surface of superconducting cubic spinel oxide LiTi2O4 is another interesting system because its inherent surface electronic and atomic reconstructions add complexity to superconducting properties. Investigations of such surfaces are hampered by the lack of single crystals or high-quality thin films. Here, using low-temperature sca…
Dimensionality reduction induced metal-insulator transitions in oxide heterostructures are usually coupled with structural and magnetic phase transitions, which complicate the interpretation of the underlying physics. Therefore, achieving isostructural MIT is of great importance for fundamental physics and even more for applications. Here, we report an isostructural metal-insulator transition driven by dimensional-crossover in spin-orbital coupled SrIrO3 films. By using in-situ pulsed laser deposition and angle-resolved photoemission spectroscopy, we synthesized and investigated the electronic…
