Novel electronic structure induced by a highly strained oxide interface with incommensurate crystal fields
H. W. Ou, J. F. Zhao, Y. Zhang, B. P. Xie, D. W. Shen, Y. Zhu, Z. Q. Yang, J. G. Che, X. G. Luo, X. H. Chen, M. Arita, K. Shimada, H. Namatame, M. Taniguchi, C.… 展开作者
H. W. Ou, J. F. Zhao, Y. Zhang, B. P. Xie, D. W. Shen, Y. Zhu, Z. Q. Yang, J. G. Che, X. G. Luo, X. H. Chen, M. Arita, K. Shimada, H. Namatame, M. Taniguchi, C. M. Cheng, K. D. Tsuei, D. L. Feng
The misfit oxide, Bi$_{2}$Ba$_{1.3}$K$_{0.6}$Co$_{2.1}$O$_{y}$, made of alternating rocksalt-structured [BiO/BaO] layers and hexagonal CoO$_{2}$ layers, was studied by angle-resolved photoemission spectroscopy. Detailed electronic structure of such a highly strained oxide interfaces is revealed for the first time. We found that under the two incommensurate crystal fields, electrons are confined within individual sides of the interface, and scattered by umklapp scattering of the crystal field from the other side. In addition, the high strain on the rocksalt layer raises its chemical potential and induces large charge transfer to the CoO$_{2}$ layer. Furthermore, a novel interface effects, the interfacial enhancement of electron-phonon interactions, is discovered. Our findings of these electronic properties lay a foundation for designing future functional oxide interfaces.
Epitaxial strain is a proven route to enhancing the properties of complex oxides, however, the details of how the atomic structure accommodates strain are poorly understood due to the difficulty of measuring the oxygen positions in thin films. We present a general methodology for determining the atomic structure of strained oxide films via x-ray diffraction, which we demonstrate using LaNiO3 films. The oxygen octahedral rotations and distortions have been quantified by comparing the intensities of half-order Bragg peaks, arising from the two unit cell periodicity of the octahedral rotations, w…
Manipulating the strain induced poly-domains and phase transition in correlated oxide material are important for high performance devices fabrication. Though the electronic transport in the strained oxide film at macroscopic scales can be directly measured, the anisotropic electronic state and the controllable phase separation cross the insulator-to-metal transition within nanoscale size are still elusive. Here, we selected VO2 crystal film as a prototypical oxide and achieved the manipulation of anisotropy electronic phase separation via injecting He+ nanobeam into VO2 film at room temperatur…
Manipulating the orbital occupation of valence electrons via epitaxial strain in an effort to induce new functional properties requires considerations of how changes in the local bonding environment affect the band structure at the Fermi level. Using synchrotron radiation to measure the x-ray linear dichroism of epitaxially strained films of the correlated oxide CaFeO3, we demonstrate that the orbital polarization of the Fe valence electrons is opposite from conventional understanding. Although the energetic ordering of the Fe 3d orbitals is confirmed by multiplet ligand field theory analysis …
Neutron diffraction has been used to determine the magnetic structure of Na$_8$Cu$_5$O$_{10}$, a stoichiometric compound containing chains based on edge-sharing CuO$_4$ plaquettes. The chains are doped with 2/5 hole per Cu site and exhibit long-range commensurate charge order with an onset well above room temperature. Below $T_N = 23$ K, the neutron data indicate long-range collinear magnetic order with a spin density modulation whose propagation vector is commensurate along and incommensurate perpendicular to the chains. Competing interchain exchange interactions are discussed as a possible o…
We studied the nano-scale structure of the short-range incommensurate magnetic order in La1.5Sr0.5CoO4 by elastic neutron scattering. We find that magnetic diffuse scattering is isotropic in the a-b plane, in contrast with the naive expectation based on the popular stripe model. Indeed, charge segregation into lines favoring certain lattice direction(s) would facilitate linear stacking faults in an otherwise robust antiferromagnetism of un-doped material, leading to anisotropic disorder, with a characteristic symmetry pattern present in the neutron scattering data.
Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the h…
While it is known that the double-layer Bi$_2$Sr$_2$CaCu$_2$O$_{8+y}$ (BSCCO) cuprate superconductor exhibits a one-dimensional (1D) incommensurate superlattice (IS), the effect of IS on the electronic structure remains elusive. Following the recent shift of the interest from underdoped to optimum and overdoped phase in BSCCO by increasing the hole doping $x$, controlled by the oxygen interstitials concentration $y$, here we focus on the multiple splitting of the density of states (DOS) peaks and emergence of higher order van Hove singularities (VHS) due to the 1D incommensurate superlattice. …
First-principles carrier mobility and optical absorption of strained ZnO with self-consistent Hubbard interactions
Korea Institute for Advanced Study（韩国高等研究院）；Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin（德克萨斯大学奥斯汀分校奥登计算工程与科学学院）；Department of Physics, The University of Texas at Austin（德克萨斯大学奥斯汀分校物理系）
Dedicated control of oxygen vacancies is an important route to functionalizing complex oxide films. It is well-known that tensile strain significantly lowers the oxygen vacancy formation energy, whereas compressive strain plays a minor role. Thus, atomically reconstruction by extracting oxygen from a compressive-strained film is challenging. Here we report an unexpected LaCoO2.5 phase with a zigzag-like oxygen vacancy ordering through annealing a compressive-strained LaCoO3 in vacuum. The synergetic tilt and distortion of CoO5 square pyramids with large La and Co shifts are quantified using sc…
Epitaxial strain provides important pathways to control the magnetic and electronic states in transition metal oxides. However, the large strain is usually accompanied by a strong reduction of the oxygen vacancy formation energy, which hinders the direct manipulation of their intrinsic properties. Here using a post-deposition ozone annealing method, we obtained a series of oxygen stoichiometric SrCoO3 thin films with the tensile strain up to 3.0%. We observed a robust ferromagnetic ground state in all strained thin films, while interestingly the tensile strain triggers a distinct metal to insu…
Lattice structure can dictate electronic and magnetic properties of a material. Especially, reconstruction at a surface or heterointerface can create properties that are fundamentally different from those of the corresponding bulk material. We have investigated the lattice structure on the surface and in the thin films of epitaxial SrRuO3 with the film thickness up to 22 pseudo-cubic unit cells (u.c.), using the combination of surface sensitive low energy electron diffraction and bulk sensitive scanning transmission electron microscopy. Our analysis indicates that, in contrast to many perovski…
We observe quasi-static incommensurate magnetic peaks in neutron scattering experiments on layered cobalt oxides La2-xSrxCoO4 with high Co oxidation states that have been reported to be paramagnetic. This enables us to measure the magnetic excitations in this highly hole-doped incommensurate regime and compare our results with those found in the low-doped incommensurate regime that exhibit hourglass magnetic spectra. The hourglass shape of magnetic excitations completely disappears given a high Sr doping. Moreover, broad low-energy excitations are found, which are not centered at the incommens…
Single-crystal neutron diffraction has been used to determine the incommensurate magnetic structure of NaCu2O2, a compound built up of chains of edge-sharing CuO4 plaquettes. Magnetic structures compatible with the lattice symmetry were identified by a group-theoretical analysis, and their magnetic structure factors were compared to the experimentally observed Bragg intensities. In conjunction with other experimental data, this analysis yields an elliptical helix structure in which both the helicity and the polarization plane alternate among copper-oxide chains. This magnetic ground state is d…
We report an inelastic-neutron-scattering and muon-spin-relaxation study of the effect of 2% spinless (Zn) impurities on the magnetic order and dynamics of YBa$_2$Cu$_3$O$_{6.6}$, an underdoped high-temperature superconductor that exhibits a prominent spin-pseudogap in its normal state. Zn substitution induces static magnetic order at low temperatures and triggers a large-scale spectral-weight redistribution from the magnetic resonant mode at 38 meV into uniaxial, incommensurate spin excitations with energies well below the spin-pseudogap. These observations indicate a competition between inco…
A slave rotor-Hartree Fock formalism is presented for studying the properties of the p-d model describing perovskite transition metal oxides, and a flexible and efficient numerical formalism is developed for its solution. The methodology is shown to yield, within an unified formulation, the significant aspects of the rare earth nickelate phase diagram, including the paramagnetic metal state observed for the LaNiO3 and the correct ground-state magnetic order of insulating compounds. It is then used to elucidate ground state changes occurring as morphology is varied from bulk to strained and un-…
The insulating ternary oxide YbFe$_2$O$_4$ displays an unusual frustration-driven incommensurate charge-ordering (CO) transition, linked to possible ferroelectricity. Based on high-resolution synchrotron data, we report a detailed structural model showing that the CO phase is an incommensurate charge-density wave and cannot be ferroelectric, since the electrical dipole moments are also incommensurately modulated. The change between continuous and "spotty" helices of scattering at the CO transition is attributed to three-dimensional fluctuations of the direction of the ordering wavevector.
Signatures of symmetry-stabilized Dirac fermions in correlated oxide CaNbO3 thin films
Oak Ridge National Laboratory（橡树岭国家实验室）；Kyung Hee University（庆熙大学）；Pusan National University（釜山国立大学）；Florida State University（佛罗里达州立大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Argonne National Laboratory（阿贡国家实验室）；Gachon University（嘉泉大学）
I show that a nonequilibrium paraelectric to ferroelectric transition can be induced using midinfrared pulses. This relies on a quartic $lQ_{\textrm{l$_z$}}^2Q_{\textrm{h$_x$}}^2$ coupling between the lowest ($Q_{\textrm{l$_z$}}$) and highest ($Q_{\textrm{h$_x$}}$) frequency infrared-active phonon modes of a paraelectric material. Density functional calculations show that the coupling constant $l$ is negative, which causes a softening of the $Q_{\textrm{l$_z$}}$ mode when the $Q_{\textrm{h$_x$}}$ mode is externally pumped. A rectification along the $Q_{\textrm{l$_z$}}$ coordinate that stabiliz…
We show through both theoretical arguments and numerical calculations that graphene discerns an unconventional sequence of quantized Hall conductivity, when subject to both magnetic fields (B) and strain. The latter produces time-reversal symmetric pseudo/axial magnetic fields (b). The single-electron spectrum is composed of two interpenetrating sets of Landau levels (LLs), located at $\pm \sqrt{2 n |b \pm B|}$, $n=0, 1, 2, \cdots$. For $b>B$, these two sets of LLs have opposite \emph{chiralities}, resulting in {\em oscillating} Hall conductivity between 0 and $\mp 2 e^2/h$ in electron and hol…
Moiré engineering has recently emerged as a capable approach to control quantum phenomena in condensed matter systems. In van der Waals heterostructures, moiré patterns can be formed by lattice misorientation between adjacent atomic layers, creating long range electronic order. To date, moiré engineering has been executed solely in stacked van der Waals multilayers. Herein, we describe our discovery of electronic moiré patterns in films of a prototypical magnetoresistive oxide La0.67Sr0.33MnO3 (LSMO) epitaxially grown on LaAlO3 (LAO) substrates. Using scanning probe nano-imaging, we observe mi…
We found a new cobalt oxide (CaOH)1.14CoO2 by utilizing the high-pressure technique. X-ray and electron diffraction studies revealed that the compound has layer structure which consists of CdI2-type CoO2 layers and rock-salt-type double CaOH atomic layers. The two subcells have incommensurate periodicity along the a-axis, resulting in modulated crystal structure due to the inter-subcell interaction. The structural modulation affects carrier conduction through the potential randomness. We found that the two-dimensional (2-D) variable-range hopping (VRH) regime with hole conduction is dominant a…
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）
We report on atomic-scale visualization of the structure of infinite-layer cuprate SrCuO2 thin films grown on Nb-doped SrTiO3 substrates by molecular beam epitaxy. In-situ scanning tunneling microscopy study reveals stoichiometric copper oxide (CuO2) plane with a 2 x 2 surface reconstruction, prompted by preferential clustering of four adjacent CuO2 plaquettes. By imaging the subsurface Sr atoms, intra-unit-cell rotational symmetry breaking is observed, which, together with the adjacent CuO2 clustering, can be well accounted for by a periodic up-down buckling of oxygen ions on the CuO2 plane. …
At a temperature of roughly 1\,K, \ce{Sr2RuO4} undergoes a transition from a normal Fermi liquid to a superconducting phase. Even while the former is relatively simple and well understood, the superconducting state is not even after 25 years of study. More recently it has been found that critical temperatures can be enhanced by application of uniaxial strain, up to a critical strain, after which it falls off. In this work, we take an `instability' approach and seek for divergences in susceptibilities. This provides an unbiased way to distinguish tendencies to competing ground states. We show t…
We report an experimental study of \nco, a Mott insulator containing chains of edge-sharing CuO$_4$ plaquettes, by polarized x-ray absorption spectroscopy (XAS), resonant magnetic x-ray scattering (RMXS), magnetic susceptibility, and pyroelectric current measurements. The XAS data show that the valence holes reside exclusively on the Cu$^{2+}$ sites within the copper-oxide spin chains and populate a $d$-orbital polarized within the CuO$_4$ plaquettes. The RMXS measurements confirm the presence of incommensurate magnetic order below a Néel temperature of $T_N = 11.5$ K, which was previously inf…
Epitaxial strain imposed in complex oxide thin films by heteroepitaxy is recognized as a powerful tool for identifying new properties and exploring the vast potential of materials performance. A particular example is LaCoO3, a zero spin, nonmagnetic material in the bulk, whose strong ferromagnetism in a thin film remains enigmatic despite a decade of intense research. Here, we use scanning transmission electron microscopy complemented by X-ray and optical spectroscopy to study LaCoO3 epitaxial thin films under different strain states. We observed an unconventional strain relaxation behavior re…
We studied the ferroelectricity of magnetic oxides in which its emergence coincides with the onset of a second incommensurate magnetic order. We solved for the wave function of e_{g} electrons in the presence of magnetic orders. The coupling between the magnetic and electric orders is provided by the spin-orbit interaction. It was found that the net electric dipole moment of the system came from the bond between the transition metal and oxygen atoms. The anisotropy of d-orbitals also played an important role. Finally, the form of the coupling leads us to the conclusion that it is an improper f…
The electronic properties of excitonic insulators have been examined precisely in recent years. Pictures of exciton condensation may be applied to the spin-state transition observed in perovskite cobalt oxides. We examine the crystal-field and magnetic-field dependences of spatial spin structures on the basis of the density matrix renormalization group method using an effective model for the one-dimensional two-orbital Hubbard model in strong-coupling limit. We find an excitonic insulating (EI) phase and a spin-state ordering (SSO) phase in the intermediate region between low-spin and high-spi…
Using x-ray and neutron scattering, we have studied the structural and magnetic properties of the single-layer manganite La{1-x}Sr{1+x}MnO4 (0 < x < 0.7). Single crystals were grown by the traveling-solvent floating-zone method at 18 La/Sr concentrations. The low-temperature phase diagram can be understood by considering the strong coupling of the magnetic and orbital degrees of freedom, and it can be divided into three distinct regions: low (x < 0.12), intermediate (0.12< x < 0.45), and high (x > 0.45) doping. LaSrMnO_4 (x=0) is an antiferromagnetic Mott insulator,and its spin-wave spectrum i…
We present neutron scattering studies of the inter-planar correlations in the high-temperature superconductor La1.88Sr0.12CuO4 (T_c=27 K). The correlations are studied both in a magnetic field applied perpendicular to the CuO2 planes, and in zero field under different cooling conditions. We find that the effect of the magnetic field is to increase the magnetic scattering signal at all values of the out-of-plane wave vector L, indicating an overall increase of the magnetic moments. In addition, weak correlations between the copper oxide planes develop in the presence of a magnetic field. This e…
Electronic phases with symmetry properties matching those of conventional liquid crystals have recently been discovered in transport experiments on semiconductor heterostructures and metal oxides at milli-Kelvin temperatures. We report the spontaneous onset of a onedimensional, incommensurate modulation of the spin system in the high-temperature superconductor YBa2Cu3O6.45 upon cooling below ~150 K, while static magnetic order is absent above 2 K. The evolution of this modulation with temperature and doping parallels that of the in-plane anisotropy of the resistivity, indicating an electronic …
