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Register a new userDefect engineering in oxide heterostructures by enhanced oxygen surface exchange
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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.
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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.
Interface engineering is an extremely useful tool for systematically investigating materials and the various ways materials interact with each other. We describe different interface engineering strategies designed to reveal the origin of the electric and magnetic dead-layer at La0.67Sr0.33MnO3 interfaces. La0.67Sr0.33MnO3 is a key example of a strongly correlated peroskite oxide material in which a subtle balance of competing interactions gives rise to a ferromagnetic metallic groundstate. This balance, however, is easily disrupted at interfaces. We systematically vary the dopant profile, the disorder and the oxygen octahedra rotations at the interface to investigate which mechanism is responsible for the dead layer. We find that the magnetic dead layer can be completely eliminated by compositional interface engineering such that the polar discontinuity at the interface is removed. This, however, leaves the electrical dead-layer largely intact. We find that deformations in the oxygen octahedra network at the interface are the dominant cause for the electrical dead layer.
The electronic transport through Au-(Cu$_{2}$O)$_n$-Au junctions is investigated using first-principles calculations and the nonequilibrium Greens function method. The effect of varying the thickness (i.e., $n$) is studied as well as that of point defects and anion substitution. For all Cu$_{2}$O thicknesses the conductance is more enhanced by bulk-like (in contrast to near-interface) defects, with the exception of O vacancies and Cl substitutional defects. A similar transmission behavior results from Cu deficiency and N substitution, as well as from Cl substitution and N interstitials for thick Cu$_{2}$O junctions. In agreement with recent experimental observations, it is found that N and Cl doping enhances the conductance. A Frenkel defect, i.e., a superposition of an O interstitial and O substitutional defect, leads to a remarkably high conductance. From the analysis of the defect formation energies, Cu vacancies are found to be particularly stable, in agreement with earlier experimental and theoretical work.
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.
Ferroelectric field-effect doping has emerged as a powerful approach to manipulate the ground state of correlated oxides, opening the door to a new class of field-effect devices. However, this potential is not fully exploited so far, since the size of the field-effect doping is generally much smaller than expected. Here we study the limiting factors through magneto-transport, scanning transmission electron and piezo-response force microscopy in ferroelectric/superconductor (YBa2Cu3O7-{delta} /BiFeO3) heterostructures, a model system showing very strong field-effects. Still, we find that they are limited in the first place by an incomplete ferroelectric switching. This can be explained by the existence of a preferential polarization direction set by the atomic terminations at the interface. More importantly, we also find that the field-effect carrier doping is accompanied by a strong modulation of the carrier mobility. Besides making quantification of field-effects via Hall measurements not straightforward, this finding suggests that ferroelectric poling produces structural changes (e.g. charged defects or structural distortions) in the correlated oxide channel. Those findings have important consequences for the understanding of ferroelectric field-effects and for the strategies to further enhance them.
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