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Register a new userThickness dependent properties in oxide heterostructures driven by structurally induced metal-oxygen hybridization variations
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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, we present 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.
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The synthesis of materials with well-controlled composition and structure improves our understanding of their intrinsic electrical transport properties. Recent developments in atomically controlled growth have been shown to be crucial in enabling the study of new physical phenomena in epitaxial oxide heterostructures. Nevertheless, these phenomena can be influenced by the presence of defects that act as extrinsic sources of both doping and impurity scattering. Control over the nature and density of such defects is therefore necessary, are we to fully understand the intrinsic materials properties and exploit them in future device technologies. Here, we show that incorporation of a strontium copper oxide nano-layer strongly reduces the impurity scattering at conducting interfaces in oxide LaAlO3-SrTiO3(001) heterostructures, opening the door to high carrier mobility materials. We propose that this remote cuprate layer facilitates enhanced suppression of oxygen defects by reducing the kinetic barrier for oxygen exchange in the hetero-interfacial film system. This design concept of controlled defect engineering can be of significant importance in applications in which enhanced oxygen surface exchange plays a crucial role.
The self-polarization of PbZr0.52Ti0.48O3 thin film is switched by changing film thickness through the competition between the strain relaxation-induced flexoelectric fields and the interfacial effects. Without an applied electric field, this reversal of self-polarization is exploited to control the magnetic properties of La0.67Sr0.33MnO3 by the competition/cooperation between the charge-mediated and the strain-mediated effects. Scanning transmission electron microscopy, polarized near edge x-ray absorption spectroscopy, and half-integer diffraction measurements are employed to decode this intrinsic magnetoelectric effects in La0.67Sr0.33MnO3/PbZr0.52Ti0.48O3 heterostructures. With PbZr0.52Ti0.48O3 films < 48 nm, the self-polarization-driven carrier density modulation around La0.67Sr0.33MnO3/PbZr0.52Ti0.48O3 interface and the strain-mediated Mn 3d orbital occupancy work together to enhance magnetism of 14 unit cells La0.67Sr0.33MnO3 film; with PbZr0.52Ti0.48O3 layers > 48 nm, the strain-induced the change of bond length/angle of MnO6 accompanied with a modified spin configuration are responsible for the decrease in Curie temperature and magnetization of 14 unit cells La0.67Sr0.33MnO3 film.
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 electroresistance ratio at room temperature. To understand these surprising results, we employed an additional control parameter, which is related to the crossing of electronic and magnetic phase boundaries of the correlated electron oxide. The FE-induced phase modulation at the heterointerface ultimately results in an enhanced electroresistance effect. Our study highlights that the strong coupling between degrees of freedom across heterointerfaces could yield versatile and novel applications in oxide electronics.
Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking $mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni $3d$ orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O $K$-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena.
The use of the spin Hall effect and its inverse to electrically detect and manipulate dynamic spin currents generated via ferromagnetic resonance (FMR) driven spin pumping has enabled the investigation of these dynamically injected currents across a wide variety of ferromagnetic materials. However, while this approach has proven to be an invaluable diagnostic for exploring the spin pumping process it requires strong spin-orbit coupling, thus substantially limiting the materials basis available for the detector/channel material (primarily Pt, W and Ta). Here, we report FMR driven spin pumping into a weak spin-orbit channel through the measurement of a spin accumulation voltage in a Si-based metal-oxide-semiconductor (MOS) heterostructure. This alternate experimental approach enables the investigation of dynamic spin pumping in a broad class of materials with weak spin-orbit coupling and long spin lifetime while providing additional information regarding the phase evolution of the injected spin ensemble via Hanle-based measurements of the effective spin lifetime.
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