A spin-orbit playground: surfaces and interfaces of transition metal oxides.

Within the last twenty years, the status of the spin-orbit interaction has evolved from that of a simple atomic contribution to a key effect that modifies the electronic band structure of materials. It is regarded as one of the basic ingredients for spintronics, locking together charge and spin degrees of freedom and recently it is instrumental in promoting a new class of compounds, the topological insulators. In this review, we present the current status of the research on the spin-orbit coupling in transition metal oxides, discussing the case of two semiconducting compounds, [Formula: see text] and [Formula: see text], and the properties of surface and interfaces based on these. We conclude with the investigation of topological effects predicted to occur in different complex oxides.

Rare-earth nickelates RNiO3: thin films and heterostructures.

This review stands in the larger framework of functional materials by focussing on heterostructures of rare-earth nickelates, described by the chemical formula RNiO3 where R is a trivalent rare-earth R = La, Pr, Nd, Sm, …, Lu. Nickelates are characterized by a rich phase diagram of structural and physical properties and serve as a benchmark for the physics of phase transitions in correlated oxides where electron-lattice coupling plays a key role. Much of the recent interest in nickelates concerns heterostructures, that is single layers of thin film, multilayers or superlattices, with the general objective of modulating their physical properties through strain control, confinement or interface effects. We will discuss the extensive studies on nickelate heterostructures as well as outline different approaches to tuning and controlling their physical properties and, finally, review application concepts for future devices.

Multiple Supersonic Phase Fronts Launched at a Complex-Oxide Heterointerface.

Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We measure the dynamics of the lattice and that of the charge disproportionation in NdNiO_{3}, when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO_{3} substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the NdNiO_{3} film, followed by a sonic lattice wave. When combined with measurements of magnetic disordering and of the metal-insulator transition, these results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces.

Striped nanoscale phase separation at the metal-insulator transition of heteroepitaxial nickelates.

Nucleation processes of mixed-phase states are an intrinsic characteristic of first-order phase transitions, typically related to local symmetry breaking. Direct observation of emerging mixed-phase regions in materials showing a first-order metal-insulator transition (MIT) offers unique opportunities to uncover their driving mechanism. Using photoemission electron microscopy, we image the nanoscale formation and growth of insulating domains across the temperature-driven MIT in NdNiO3 epitaxial thin films. Heteroepitaxy is found to strongly determine the nanoscale nature of the phase transition, inducing preferential formation of striped domains along the terraces of atomically flat stepped surfaces. We show that the distribution of transition temperatures is a local property, set by surface morphology and stable across multiple temperature cycles. Our data provide new insights into the MIT of heteroepitaxial nickelates and point to a rich, nanoscale phenomenology in this strongly correlated material.

Interlayer coupling through a dimensionality-induced magnetic state.

Dimensionality is known to play an important role in many compounds for which ultrathin layers can behave very differently from the bulk. This is especially true for the paramagnetic metal LaNiO3, which can become insulating and magnetic when only a few monolayers thick. We show here that an induced antiferromagnetic order can be stabilized in the [111] direction by interfacial coupling to the insulating ferromagnet LaMnO3, and used to generate interlayer magnetic coupling of a nature that depends on the exact number of LaNiO3 monolayers. For 7-monolayer-thick LaNiO3/LaMnO3 superlattices, negative and positive exchange bias, as well as antiferromagnetic interlayer coupling are observed in different temperature windows. All three behaviours are explained based on the emergence of a (»,»,»)-wavevector antiferromagnetic structure in LaNiO3 and the presence of interface asymmetry with LaMnO3. This dimensionality-induced magnetic order can be used to tailor a broad range of magnetic properties in well-designed superlattice-based devices.

Interfacial Control of Magnetic Properties at LaMnO3/LaNiO3 Interfaces.

The functional properties of oxide heterostructures ultimately rely on how the electronic and structural mismatches occurring at interfaces are accommodated by the chosen materials combination. We discuss here LaMnO3/LaNiO3 heterostructures, which display an intrinsic interface structural asymmetry depending on the growth sequence. Using a variety of synchrotron-based techniques, we show that the degree of intermixing at the monolayer scale allows interface-driven properties such as charge transfer and the induced magnetic moment in the nickelate layer to be controlled. Further, our results demonstrate that the magnetic state of strained LaMnO3 thin films dramatically depends on interface reconstructions.

Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface.

Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion. Light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.

Electron confinement at the LaAlO3/SrTiO3 interface.

Physical and structural phenomena originating from polar discontinuities have generated enormous activity. In the last ten years, the oxide interface between polar LaAlO(3) and non-polar SrTiO(3), both band insulators, has attracted particular interest, as it hosts an electron liquid with remarkable properties: it superconducts, has a sizeable spin-orbit interaction and its properties are tunable by an electric field. The profile of the carrier density at the interface and the exact band structure are properties strongly linked and still objects of debate. Here we review the experimental findings on the origin and the extension of the electron liquid and discuss the theoretical models developed to describe the charge profile and the band structure. We also introduce a model to account for the effect of interface disorder which could modify the charge distribution.

Interface Fermi states of LaAlO3/SrTiO3 and related heterostructures.

The interfaces of LaAlO3/SrTiO3 and (LaAlO3)(x)(SrTiO3)(1-x)/SrTiO3 heterostructures have been investigated by soft x-ray photoelectron spectroscopy for different layer thicknesses across the insulator-to-metal interface transition. The valence band and Fermi edge were probed using resonant photoemission across the Ti L(2,3) absorption edge. The presence of a Fermi-edge signal originating from the partially filled Ti 3d orbitals is only found in the conducting samples. No Fermi-edge signal could be detected for insulating samples below the critical thickness. Furthermore, the angular dependence of the Fermi intensity allows the determination of the spatial extent of the conducting electron density perpendicular to the interface.

Tunable conductivity threshold at polar oxide interfaces.

The physical mechanisms responsible for the formation of a two-dimensional electron gas at the interface between insulating SrTiO(3) and LaAlO(3) have remained a contentious subject since its discovery in 2004. Opinion is divided between an intrinsic mechanism involving the build-up of an internal electric potential due to the polar discontinuity at the interface between SrTiO(3) and LaAlO(3), and extrinsic mechanisms attributed to structural imperfections. Here we show that interface conductivity is also exhibited when the LaAlO(3) layer is diluted with SrTiO(3), and that the threshold thickness required to show conductivity scales inversely with the fraction of LaAlO(3) in this solid solution, and thereby also with the layer's formal polarization. These results can be best described in terms of the intrinsic polar-catastrophe model, hence providing the most compelling evidence, to date, in favour of this mechanism.

Ultrafast strain engineering in complex oxide heterostructures.

We report on ultrafast optical experiments in which femtosecond midinfrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO(3) epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates.

Electrostatic coupling and local structural distortions at interfaces in ferroelectric/paraelectric superlattices.

The performance of ferroelectric devices is intimately entwined with the structure and dynamics of ferroelectric domains. In ultrathin ferroelectrics, ordered nanodomains arise naturally in response to the presence of a depolarizing field and give rise to highly inhomogeneous polarization and structural profiles. Ferroelectric superlattices offer a unique way of engineering the desired nanodomain structure by modifying the strength of the electrostatic interactions between different ferroelectric layers. Through a combination of X-ray diffraction, transmission electron microscopy, and first-principles calculations, the electrostatic coupling between ferroelectric layers is studied, revealing the existence of interfacial layers of reduced tetragonality attributed to inhomogeneous strain and polarization profiles associated with the domain structure.

Electrostriction at the LaAlO3/SrTiO3 interface.

We present a direct comparison between experimental data and ab initio calculations for the electrostrictive effect in the polar LaAlO(3) layer grown on SrTiO(3) substrates. From the structural data, a complete screening of the LaAlO(3) dipole field is observed for film thicknesses between 6 and 20 uc. For thinner films, an expansion of the c axis of 2% matching the theoretical predictions for an electrostrictive effect is observed experimentally.

Metal-insulator transition in ultrathin LaNiO3 films.

Transport in ultrathin films of LaNiO(3) evolves from a metallic to a strongly localized character as the film's thickness is reduced and the sheet resistance reaches a value close to h/e(2), the quantum of resistance in two dimensions. In the intermediate regime, quantum corrections to the Drude low-temperature conductivity are observed; they are accurately described by weak localization theory. Remarkably, the negative magnetoresistance in this regime is isotropic, which points to magnetic scattering associated with the proximity of the system to either a spin-glass state or the charge ordered antiferromagnetic state observed in other rare earth nickelates.

X-ray diffraction studies of 180 degrees ferroelectric domains in PbTiO3/SrTiO3 superlattices under an applied electric field.

The dielectric response of PbTiO(3)/SrTiO(3) superlattices is studied using electrical and structural measurements. While the dielectric response of paraelectric superlattices is well accounted for by the lattice contribution, superlattices with ferroelectric compositions exhibit an enhanced permittivity. X-ray diffraction allowed the presence of ordered nanodomains in ferroelectric superlattices to be established and their displacement under an applied bias to be directly probed, demonstrating that the enhanced permittivity in these artificial materials is due to domain wall motion.

Tunable Rashba spin-orbit interaction at oxide interfaces.

The quasi-two-dimensional electron gas found at the LaAlO{3}/SrTiO{3} interface offers exciting new functionalities, such as tunable superconductivity, and has been proposed as a new nanoelectronics fabrication platform. Here we lay out a new example of an electronic property arising from the interfacial breaking of inversion symmetry, namely, a large Rashba spin-orbit interaction, whose magnitude can be modulated by the application of an external electric field. By means of magnetotransport experiments we explore the evolution of the spin-orbit coupling across the phase diagram of the system. We uncover a steep rise in Rashba interaction occurring around the doping level where a quantum critical point separates the insulating and superconducting ground states of the system.

Two-dimensional quantum oscillations of the conductance at LaAlO3/SrTiO3 interfaces.

We report on a study of magnetotransport in LaAlO3 /SrTiO3 interfaces characterized by mobilities of the order of several thousands cm2/V s. We observe Shubnikov-de Haas oscillations whose period depends only on the perpendicular component of the magnetic field. This observation directly indicates the formation of a two-dimensional electron gas originating from quantum confinement at the interface. From the temperature dependence of the oscillation amplitude we extract an effective carrier mass m* ≃ 1.45 m(e). An electric field applied in the back-gate geometry increases the mobility, the carrier density, and the oscillation frequency.

Electron scattering at dislocations in LaAlO3/SrTiO3 interfaces.

We report experimental investigations of the effects of microstructural defects and of disorder on the properties of 2D electron gases at oxide interfaces. The cross section for scattering of electrons at dislocations in LaAlO(3)/SrTiO(3) interfaces has been measured and found to equal approximately 5 nm. Our experiments reveal that the transport properties of these electron gases are strongly influenced by scattering at dislocation cores.

Superconductivity at the LaAlO(3)/SrTiO(3) interface.

We report on the structural characterization of LaAlO(3)/SrTiO(3) interfaces and on their transport properties. LaAlO(3) films were prepared using pulsed laser deposition onto TiO(2) terminated (001) SrTiO(3) substrates inducing a metallic conduction at the interface. Resistance and Hall effect measurements reveal a sheet carrier density between 0.4 and 1.2 × 10(14) electrons cm(-2) at room temperature and a mobility of ∼300 cm(2) V(-1) s(-1) at low temperatures. A transition to a superconducting state is observed at a temperature of ∼200 mK. The superconducting characteristics display signatures of 2D superconductivity.

Electric field control of the LaAlO3/SrTiO3 interface ground state.

Interfaces between complex oxides are emerging as one of the most interesting systems in condensed matter physics. In this special setting, in which translational symmetry is artificially broken, a variety of new and unusual electronic phases can be promoted. Theoretical studies predict complex phase diagrams and suggest the key role of the charge carrier density in determining the systems' ground states. A particularly fascinating system is the conducting interface between the band insulators LaAlO(3) and SrTiO(3) (ref. 3). Recently two possible ground states have been experimentally identified: a magnetic state and a two-dimensional superconducting condensate. Here we use the electric field effect to explore the phase diagram of the system. The electrostatic tuning of the carrier density allows an on/off switching of superconductivity and drives a quantum phase transition between a two-dimensional superconducting state and an insulating state. Analyses of the magnetotransport properties in the insulating state are consistent with weak localization and do not provide evidence for magnetism. The electric field control of superconductivity demonstrated here opens the way to the development of new mesoscopic superconducting circuits.