Structural basis for the conducting interface between LaAlO3 and SrTiO3

The complete atomic structure of a five-monolayer film of LaAlO3 on SrTiO3 has been determined for the first time by surface x-ray diffraction in conjunction with the coherent Bragg rod analysis phase-retrieval method and further structural refinement. Cationic mixing at the interface results in dilatory distortions and the formation of metallic La(1-x)SrxTiO3. By invoking electrostatic potential minimization, the ratio of Ti{4+}/Ti{3+} across the interface was determined, from which the lattice dilation could be quantitatively explained using ionic radii considerations. The correctness of this model is supported by density functional theory calculations. Thus, the formation of a quasi-two-dimensional electron gas in this system is explained, based on structural considerations.     

Electrolyte gate-controlled Kondo effect in SrTiO3

We report low-temperature, high-field magnetotransport measurements of SrTiO(3) gated by an ionic gel electrolyte. A saturating resistance upturn and negative magnetoresistance that signal the emergence of the Kondo effect appear for higher applied gate voltages. This observation, enabled by the wide tunability of the ionic gel-applied electric field, promotes the interpretation of the electric field-effect-induced 2D electron system in SrTiO(3) as an admixture of magnetic Ti(3+) ions, i.e., localized and unpaired electrons, and delocalized electrons that partially fill the Ti 3d conduction band.     

Atomic-scale analysis of the oxygen configuration at a SrTiO3 dislocation core

The atomic structure of a SrTiO3 dislocation is revealed directly by phase-retrieval electron microscopy. In particular, atomic columns of light oxygen are observed simultaneously with the columns of considerably heavier Sr and Ti. A distinct structural modification of the oxygen octahedra at the dislocation core as well as a significant nonstoichiometry, including a deficiency of oxygen, are observed. Deviations from the bulk chemical concentration are quantified column by column by means of structure modeling and quantum-mechanical simulations of the electron scattering process.     

Practical spatial resolution of electron energy loss spectroscopy in aberration corrected scanning transmission electron microscopy

The resolution of electron energy loss spectroscopy (EELS) is limited by delocalization of inelastic electron scattering rather than probe size in an aberration corrected scanning transmission electron microscope (STEM). In this study, we present an experimental quantification of EELS spatial resolution using chemically modulated 2×(LaMnO(3))/2×(SrTiO(3)) and 2×(SrVO(3))/2×(SrTiO(3)) superlattices by measuring the full width at half maxima (FWHM) of integrated Ti M(2,3), Ti L(2,3), V L(2,3), Mn L(2,3), La N(4,5), La N(2,3) La M(4,5) and Sr L(3) edges over the superlattices. The EELS signals recorded using large collection angles are peaked at atomic columns. The FWHM of the EELS profile, obtained by curve-fitting, reveals a systematic trend with the energy loss for the Ti, V, and Mn edges. However, the experimental FWHM of the Sr and La edges deviates significantly from the observed experimental tendency.     

Direct 3D imaging of Al70.4Pd21Mn8.6 quasicrystal local atomic structure by X-ray holography

Inverse x-ray fluorescence holography was used to explore the local atomic order of a nearly perfect quasicrystal with composition Al70. 4Pd21Mn8.6. We have demonstrated the possibility of direct 3D imaging of the atomic decoration in a quasicrystal. We have obtained the average 3D environment of selected coordination shells around the Mn atoms. These results open the way to obtaining further and more complete information about the various coordination shells in complex materials by measuring multiple energy x-ray holograms at different sites.     

Electronic and magnetic reconstructions in La0.7Sr0.3MnO3/SrTiO3 heterostructures: a case of enhanced interlayer coupling controlled by the interface

We report on the magnetic coupling of La0.7Sr0.3MnO3 layers through SrTiO3 spacers in La0.7Sr0.3MnO3/SrTiO3 epitaxial heterostructures. Combined aberration-corrected microscopy and electron-energy-loss spectroscopy evidence charge transfer to the empty conduction band of the titanate. Ti d electrons interact via superexchange with Mn, giving rise to a Ti magnetic moment as demonstrated by x-ray magnetic circular dichroism. This induced magnetic moment in the SrTiO3 controls the bulk magnetic and transport properties of the superlattices when the titanate layer thickness is below 1 nm.     

应力作用下铁电超晶格BaTiO3/SrTiO3的结构和极化的第一性原理研究

通过第一性原理计算，研究了在不同应力作用下铁电超晶格BaTiO₃/SrTiO₃的结构以及自发极化的变化.结果显示，在应力作用下，晶格发生变形，并且沿着c轴在Ti原子和O原子之间电荷发生传输.随着应力的增加，超晶格中各类原子沿着c轴的位移都会有不同程度上的增加，造成了铁电超晶格的自发极化不断提高.此外，在该模型中，通过变化所施加的应力，可以控制超晶格的极化性质.     

具有原子分辨率的x射线荧光全息术的数值模拟研究

根据x射线荧光全息术的成像原理，对体心立方晶系的Fe单晶进行了数值模拟（包括荧光全 息图及其重构像），在各个晶面（001，010，100）上得到Fe原子的像，与Fe的晶格模型的 原子位置一致，表明运用这种x射线荧光全息术，能够在原子水平上得到单晶或准晶体的内 部结构图像. 关键词： x射线荧光全息术 同步辐射 晶体结构 傅里叶变换     

Structural comparison of n-type and p-type LaAlO3/SrTiO3 interfaces

Using a surface x-ray diffraction technique, we investigated the atomic structure of two types of interfaces between LaAlO3 and SrTiO3, that is, p-type (SrO/AlO2) and n-type (TiO2/LaO) interfaces. Our results demonstrate that the SrTiO3 in the sample with the n-type interface has a large polarized region, while that with the p-type interface has a limited polarized region. In addition, atomic intermixing was observed to extend deeper into the SrTiO3 substrate at the n-type interface compared to the p type. These differences result in distinct degrees of band bending, which likely contributes to the striking contrast in electrical conductivity between the two types of interfaces.     

Multienergy anomalous diffuse scattering

A new approach to local structure determination is presented. A three-dimensional region of the reciprocal space of a SrTiO(3) single crystal was mapped by measuring x-ray diffuse scattering patterns at different sample orientations in order to reconstruct the local atomic structure. The phase problem was solved by means of anomalous scattering from strontium atoms at photon energies near their K absorption edge. Real-space reconstruction provides the average short-range order atomic arrangement in the vicinity of anomalous scatterers up to a distance of several unit cells.     

Reversible transition between thermodynamically stable phases with low density of oxygen vacancies on the SrTiO3(110) surface

The surface reconstruction of SrTiO3(110) is studied with scanning tunneling microscopy and density functional theory (DFT) calculations. The reversible phase transition between (4×1) and (5×1) is controlled by adjusting the surface metal concentration [Sr] or [Ti]. Resolving the atomic structures of the surface, DFT calculations verify that the phase stability changes upon the chemical potential of Sr or Ti. In particular, the density of oxygen vacancies is low on the thermodynamically stabilized SrTiO3(110) surface.     

Resonant soft x-ray scattering from stepped surfaces of SrTiO3

We studied the resonant diffraction signal from stepped surfaces of SrTiO(3) at the Ti 2p → 3d (L(2,3)) resonance in comparison with x-ray absorption (XAS) and specular reflectivity data. The steps on the surface form an artificial superstructure suitable as a model system for resonant soft x-ray diffraction. A small step density on the surface is sufficient to produce a well defined diffraction peak. We determined the optical parameters of the sample across the resonance and found that the differences between the energy dependence of the x-ray absorption signal, the specular reflectivity and the step-related peak reflect the different quantities probed in these signals. When recorded at low incidence or detection angles, XAS and specular reflectivity spectra are strongly distorted by the changes of the angle of total reflection with energy. The resonant diffraction spectrum is less affected and can be used as a spectroscopic probe even in less favorable geometries.     

Spontaneous 2-dimensional carrier confinement at the n-type SrTiO3/LaAlO3 interface

We describe the intrinsic mechanism of 2-dimensional electron confinement at the n-type SrTiO3/LaAlO3 interface as a function of the sheet carrier density n(s) via advanced first-principles calculations. Electrons localize spontaneously in Ti 3d(xy) levels within a thin (?2 nm) interface-adjacent SrTiO3 region for n(s) lower than a threshold value n(c)～10(14) cm(-2). For n(s)>n(c) a portion of charge flows into Ti 3d(xz)-d(yz) levels extending farther from the interface. This intrinsic confinement can be attributed to the interface-induced symmetry breaking and localized nature of Ti 3d t(2g) states. The sheet carrier density directly controls the binding energy and the spatial extension of the conductive region. A direct, quantitative relation of these quantities with n(s) is provided.     

Surface and defect structure of oxide nanowires on SrTiO3

Processing the SrTiO(3)(001) surface results in the self-assembly of reduced titanate nanowires whose widths are approximately 1 nm. We have imaged these nanowires and their defects at elevated temperatures by atomic resolution scanning tunneling microscopy. The nanowire structure is modeled with density functional theory, and defects observed in the center of the nanowire are determined to be Ti(4)O(3) vacancy clusters. The activation energy for Ti(4)O(3) vacancy cluster diffusion is explicitly measured as 4.98±0.17 eV with an exponential prefactor of μ=6.57×10(29) (s(-1).     

Structure of SrTiO3 films on Si

The epitaxial deposition of oxides on silicon opens the possibility of incorporating their diverse properties into silicon-device technology. Deposition of SrTiO(3) on silicon was first reported over a decade ago, but growing the coherent, lattice-matched films that are critical for many applications has been difficult for thicknesses beyond 5 unit cells. Using a combination of density functional calculations and x-ray diffraction measurements, we determine the atomic structure of coherent SrTiO(3) films on silicon, finding that the Sr concentration at the interface varies with the film thickness. The structures with the lowest computed energies best match the x-ray diffraction. During growth, Sr diffuses from the interface to the surface of the film; the increasing difficulty of Sr diffusion with film thickness may cause the disorder seen in thicker films. The identification of this unique thickness-dependent interfacial structure opens the possibility of modifying the interface to improve the thickness and quality of metal oxide films on silicon.     

X-ray linear dichroism dependence on ferroelectric polarization

X-ray absorption spectroscopy and photoemission electron microscopy are techniques commonly used to determine the magnetic properties of thin films, crystals, and heterostructures. Recently, these methods have been used in the study of magnetoelectrics and multiferroics. The analysis of such materials has been compromised by the presence of multiple order parameters and the lack of information on how to separate these coupled properties. In this work, we shed light on the manifestation of dichroism from ferroelectric polarization and atomic structure using photoemission electron microscopy and x-ray absorption spectroscopy. Linear dichroism arising from the ferroelectric order in the PbZr0:2Ti0:8O3 thin films was studied as a function of incident x-ray polarization and geometry to unambiguously determine the angular dependence of the ferroelectric contribution to the dichroism. These measurements allow us to examine the contribution of surface charges and ferroelectric polarization as potential mechanisms for linear dichroism. The x-ray linear dichroism from ferroelectric order revealed an angular dependence based on the angle between the ferroelectric polarization direction and the x-ray polarization axis, allowing a formula for linear dichroism in ferroelectric samples to be defined.     

Atomic structures by direct transform of diffraction patterns

We propose all the diffraction patterns can be directly transformed to provide three-dimensional atomic structures for the system studied. Depending on the scattering process, either the holography or Patterson transform scheme is used. For diffraction patterns which are generated from a localized emitter source or dominated by an inelastic-scattering feature like core-level photoelectron or low-energy Kikuchi electron, holography transform is needed. On the other hand, for diffraction patterns which were dominated by elastic-scattering, like grazing-incidence X-ray diffraction, electron correlated thermal diffuse scattering or low-energy electron diffraction curves, Patterson transform is needed. To prove our point, high-fidelity and artifact-free three-dimensional atomic structures obtained by transform of low-energy Kikuchi electron patterns and low-energy electron diffraction curves are presented. The future of these direct methods by transforming diffraction patterns will be discussed.     

Hard X ray holographic diffraction imaging

We determine the absolute electron density of a lithographically grown nanostructure with 25 nm resolution by combining hard x-ray Fourier transform holography with iterative phase retrieval methods. While holography immediately reveals an unambiguous image of the object, we deploy in addition iterative phase retrieval algorithms for pushing the resolution close to the diffraction limit. The use of hard (8 keV) x rays eliminates practically all constraints on sample environment and enables a destruction-free investigation of relatively thick or buried samples, making holographic diffraction imaging a very attractive tool for materials science. We note that the technique is ideally suited for subpicosecond imaging that will become possible with the emerging hard x-ray free-electron lasers.     

钛酸锶晶体的光致介电常数激增以及超顺电大极化子理论

钙钛矿类化合物钛酸锶具有明显的光致介电增长的性质,这是由于被光激发至Ti⁴⁺的3d能带上的电子具有良好的巡游特性,为了进一步揭示光致介电增长的微观机理,这里假设巡游电子同时与两类声子发生耦合作用,一方面,电子与A_1g模式的晶格呼吸子发生强相互作用,另一方面,电子还与T_1u模式的非简谐声子具有相对较弱的耦合.通过变分法计算可得,这种复杂的电声耦合作用在晶体中形成两种极化子:自陷极化子和超顺电大极化子.正是由于超顺电大极化子的形成,导致了光致介电激增的现象.     

Photoemission from buried interfaces in SrTiO3/LaTiO3 superlattices

We have measured photoemission spectra of SrTiO3/LaTiO3 superlattices with a topmost SrTiO3 layer of variable thickness. A finite coherent spectral weight with a clear Fermi cutoff was observed at chemically abrupt SrTiO3/LaTiO3 interfaces, indicating that an "electronic reconstruction" occurs at the interface between the Mott insulator LaTiO3 and the band insulator SrTiO3. For SrTiO3/LaTiO3 interfaces annealed at high temperatures (approximately 1000 degrees C), which leads to Sr/La atomic interdiffusion and hence to the formation of La(1-x)Sr(x)TiO3-like material, the intensity of the incoherent part was found to be dramatically reduced whereas the coherent part with a sharp Fermi cutoff was enhanced due to the spread of charge. These important experimental features are well reproduced by layer dynamical-mean-field-theory calculation.