Properties Of Oxide Heterostructures Research Articles

Asymmetric Interfacial Intermixing Associated Magnetic Coupling in LaMnO3/LaFeO3 Heterostructures

The structural and magnetic properties of LaMnO3/LaFeO3 (LMO/LFO) heterostructures are characterized using a combination of scanning transmission electron microscopy, electron energy-loss spectroscopy, bulk magnetometry, and resonant x-ray reflectivity. Unlike the relatively abrupt interface when LMO is deposited on top of LFO, the interface with reversed growth order shows significant cation intermixing of Mn3+ and Fe3+, spreading ∼8 unit cells across the interface. The asymmetric interfacial chemical profiles result in distinct magnetic properties. The bilayer with abrupt interface shows a single magnetic hysteresis loop with strongly enhanced coercivity, as compared to the LMO plain film. However, the bilayer with intermixed interface shows a step-like hysteresis loop, associated with the separate switching of the “clean” and intermixed LMO sublayers. Our study illustrates the key role of interfacial chemical profile in determining the functional properties of oxide heterostructures.

Depth-Resolved Modulation of Metal-Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces.

Interface-induced modifications of the electronic, magnetic, and lattice degrees of freedom drive an array of novel physical properties in oxide heterostructures. Here, large changes in metal-oxygen band hybridization, as measured in the oxygen ligand hole density, are induced as a result of interfacing two isovalent correlated oxides. Using resonant X-ray reflectivity, a superlattice of SrFeO3 and CaFeO3 is shown to exhibit an electronic character that spatially evolves from strongly O-like in SrFeO3 to strongly Fe-like in CaFeO3 . This alternating degree of Fe electronic character is correlated with a modulation of an Fe 3d orbital polarization, giving rise to an orbital superstructure. At the SrFeO3 /CaFeO3 interfaces, the ligand hole density and orbital polarization reconstruct in a single unit cell of CaFeO3 , demonstrating how the mismatch in these electronic parameters is accommodated at the interface. These results provide new insight into how the orbital character of electrons is altered by correlated oxide interfaces and lays out a broadly applicable approach for depth-resolving band hybridization.

Strain Engineering of Epitaxial Oxide Heterostructures Beyond Substrate Limitations

Epitaxial strain, imparted by an underlying substrate, is a powerful pathway to drive phase transitions and dramatically alter properties in oxide heterostructures, enabling the emergence of new ground states and the enhancement of ferroelectricity, piezoelectricity, superconductivity and ferromagnetism. However, the limitation of commercially available single-crystal substrates and the lack of continuous strain tunability preclude the ability to take full advantage of strain engineering for further exploring novel properties and exhaustively studying fundamental physics in complex oxides. Here we report an approach for imposing continuously tunable, large epitaxial strain in oxide heterostructures beyond substrate limitations by inserting an interface layer through tailoring its gradual strain relaxation. Taking BiFeO3 as a model system, we demonstrate that the introduction of an ultrathin interface layer allows the creation of a desired strain that can induce phase transition and stabilize a new metastable super-tetragonal phase as well as morphotropic phase boundaries overcoming substrate limitations. Furthermore, continuously tunable strain from tension to compression can be generated by precisely adjusting the thickness of the interface layer, leading to the first achievement of continuous O-R-T phase transition in BiFeO3 on a single substrate. This proposed route could be extended to other oxide heterostructures, providing a platform for creating exotic phases and emergent phenomena.

Evidence for exchange bias coupling at the perovskite/brownmillerite interface in spontaneously stabilized SrCoO3−δ/SrCoO2.5 bilayers

Interface effect in complex oxide thin film heterostructures lies at the vanguard of current research to design technologically relevant functionality and explore emergent physical phenomena. While most of the previous works focus on the perovskite/perovskite heterostructures, the study on perovskite/brownmillerite interfaces remain at its infancy. Here, we investigate spontaneously stabilized perovskite-ferromagnet (SrCoO3-{\delta})/brownmillertite-antiferromagnet (SrCoO2.5) bi-layer with TN > TC and discover an unconventional interfacial magnetic exchange bias effect. From magnetometry investigations, it is rationalized that the observed effect stems from the interfacial ferromagnet/antiferromagnet coupling. The possibility for coupled ferromagnet/spinglass interface engendering such effect is ruled out. Strikingly, a finite coercive field persists in the paramagnetic state of SrCoO3-{\delta} whereas the exchange bias field vanishes at TC. We conjecture the observed effect to be due to the effective external quenched staggered field provided by the antiferromagtic layer for the ferromagnetic spins at the interface. Our results not only unveil a new paradigm to tailor the interfacial magnetic properties in oxide heterostructures without altering the cations at the interface, but also provide a purview to delve into the fundamental aspects of exchange bias in such unusual systems paving a big step forward in thin film magnetism.

Role of polar compensation in interfacial ferromagnetism of LaNiO3/CaMnO3 superlattices

Polar compensation can play an important role in the determination of interfacial electronic and magnetic properties in oxide heterostructures. Using x-ray absorption spectroscopy, x-ray magnetic circular dichroism, bulk magnetometry, and transport measurements, we find that interfacial charge redistribution via polar compensation is essential for explaining the evolution of interfacial ferromagnetism in LaNiO$_3$/CaMnO$_3$ superlattices as a function of LaNiO$_3$ layer thickness. In insulating superlattices (4 unit cells or less of LaNiO$_3$), magnetism is dominated by Ni-Mn superexchange, while itinerant electron-based Mn-Mn double-exchange plays a role in thicker metallic superlattices. X-ray magnetic circular dichroism and resonant x-ray scattering show that Ni-Mn superexchange contributes to the magnetization even in metallic superlattices. This Ni-Mn superexchange interaction can be explained in terms of polar compensation at the LaNiO$_3$-CaMnO$_3$ interface. These results highlight the different mechanisms responsible for interfacial ferromagnetism and the importance of understanding compensation due to polar mismatch at oxide-based interfaces when engineering magnetic properties.

Thickness Dependent Properties in Oxide Heterostructures Driven by Structurally Induced Metal–Oxygen Hybridization Variations

Thickness‐driven electronic phase transitions are broadly observed in different types of functional perovskite heterostructures. However, uncertainty remains whether these effects are solely due to spatial confinement, broken symmetry, or rather to a change of structure with varying film thickness. Here, this study presents direct evidence for the relaxation of oxygen‐2p and Mn‐3d orbital (p–d) hybridization coupled to the layer‐dependent octahedral tilts within a La2/3Sr1/3MnO3 film driven by interfacial octahedral coupling. An enhanced Curie temperature is achieved by reducing the octahedral tilting via interface structure engineering. Atomically resolved lattice, electronic, and magnetic structures together with X‐ray absorption spectroscopy demonstrate the central role of thickness‐dependent p–d hybridization in the widely observed dimensionality effects present in correlated oxide heterostructures.

Research Update: Interface-engineered oxygen octahedral tilts in perovskite oxide heterostructures

Interface engineering of structural distortions is a key for exploring the functional properties of oxide heterostructures and superlattices. In this paper, we report on our comprehensive investigations of oxygen octahedral distortions at the heterointerface between perovskite oxides SrRuO3 and BaTiO3 on GdScO3 substrates and of the influences of the interfacially engineered distortions on the magneto-transport properties of the SrRuO3 layer. Our state-of-the-art annular bright-field imaging in aberration-corrected scanning transmission electron microscopy revealed that the RuO6 octahedral distortions in the SrRuO3 layer have strong dependence on the stacking order of the SrRuO3 and BaTiO3 layers on the substrate. This can be attributed to the difference in the interfacial octahedral connections. We also found that the stacking order of the oxide layers has a strong impact on the magneto-transport properties, allowing for control of the magnetic anisotropy of the SrRuO3 layer through interface engineering. Our results demonstrate the significance of the interface engineering of the octahedral distortions on the structural and physical properties of perovskite oxides.

(Invited) Properties of Oxide Heterostructures

We present theoretical and experimental studies of three oxide heterostructures: LaAlO3/EuO heterojunction, Fe/BaTiO3/Pt superlattice and epitaxial LaCoO3 on (100)-oriented silicon. We use density functional theory (DFT) to predict the physical properties of the heterostucture and molecular beam epitaxy (MBE) to realize it in practice. We predict spin polarized two dimensional electron gas at the LaAlO3/EuO interface, linear magnetoelectric effect in a Fe/BaTiO3/Pt superlattice, and predict and demonstrate experimentally strain stabilized ferromagnetism in LaCoO3 on silicon.

Defects and transport in complex oxide thin films

Epitaxial oxide thin films are at the heart of new “oxide electronic” applications, such as excitonic ultraviolet light-emitting diodes and resistive switching memories. Complex oxide films are often grown by pulsed laser deposition (PLD) because the technique is believed to be material agnostic. Here, we show that one of the fundamental premises used to justify the use of PLD, that material is transferred from an ablation target to the film without stoichiometry deviations, is incorrect even when no volatile elements are involved. Even more importantly, the commonly used solution of increasing the laser energy density above a material-specific threshold value to obtain stoichiometric films cannot be used in the case of low carrier density systems such as SrTiO3, where even minute 1018 cm−3 order cation nonstoichiometry can have a dramatic effect on transport. Lattice parameter deviations in oxide films, which are often incorrectly ascribed to oxygen loss, correlate very well with cation nonstoichiometry. We show that proper simultaneous choice of ablation laser fluence and ablation area is essential and often more important than the growth temperature and oxygen pressure for obtaining bulklike properties in oxide heterostructures.