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Magnetoelectric coupling in artificial multiferroic interfaces can be drastically affected by the switching of oxygen vacancies and by the inversion of the ferroelectric polarization. Disentangling both effects is of major importance toward exploiting these effects in practical spintronic or spinorbitronic devices. We report on the independent control of ferroelectric and oxygen vacancy switching in multiferroic tunnel junctions with a La0.7Sr0.3MnO3 bottom electrode, a BaTiO3 ferroelectric barrier, and a Ni top electrode. We show that the concurrence of interface oxidation and ferroelectric switching allows for the controlled inversion of the interface spin polarization. Moreover, we show the possibility of a spin-memristor where the controlled oxidation of the interface allows for a continuum of memresistance states in the tunneling magnetoresistance. These results signal interesting new avenues toward neuromorphic devices where, as in practical neurons, the electronic response is controlled by electrochemical degrees of freedom.

Controlling magnetic anisotropy is an important objective towards engineering novel magnetic device concepts in oxide electronics. In thin film manganites, magnetic anisotropy is weak and it is primarily determined by the substrate, through induced structural distortions resulting from epitaxial mismatch strain. On the other hand, in cobaltites, with a stronger spin orbit interaction, magnetic anisotropy is typically much stronger. In this paper, we show that interfacing La0.7Sr0.3MnO3 (LSMO) with an ultrathin LaCoO3 (LCO) layer drastically modifies the magnetic anisotropy of the manganite, making it independent of the substrate and closer to the magnetic isotropy characterizing its rhombohedral structure. Ferromagnetic resonance measurements evidence a tendency of manganite magnetic moments to point out-of-plane suggesting non collinear magnetic interactions at the interface. These results may be of interest for the design of oxide interfaces with tailored magnetic structures for new oxide devices.

The persistence of ferroelectricity in ultrathin layers relies critically on screening or compensation of polarization charges which otherwise destabilize the ferroelectric state. At surfaces, charged defects play a crucial role in the screening mechanism triggering novel mixed electrochemical-ferroelectric states. At interfaces, however, the coupling between ferroelectric and electrochemical states has remained unexplored. Here, we make use of the dynamic formation of the oxygen vacancy profile in the nanometer-thick barrier of a ferroelectric tunnel junction to demonstrate the interplay between electrochemical and ferroelectric degrees of freedom at an oxide interface. We fabricate ferroelectric tunnel junctions with a La_{0.7}Sr_{0.3}MnO_{3} bottom electrode and BaTiO_{3} ferroelectric barrier. We use poling strategies to promote the generation and transport of oxygen vacancies at the metallic top electrode. Generated oxygen vacancies control the stability of the ferroelectric polarization and modify its coercive fields. The ferroelectric polarization, in turn, controls the ionization of oxygen vacancies well above the limits of thermodynamic equilibrium, triggering the build up of a Schottky barrier at the interface which can be turned on and off with ferroelectric switching. This interplay between electronic and electrochemical degrees of freedom yields very large values of the electroresistance (more than 10^{6}% at low temperatures) and enables a controlled switching between clockwise and counterclockwise switching modes in the same junction (and consequently, a change of the sign of the electroresistance). The strong coupling found between electrochemical and electronic degrees of freedom sheds light on the growing debate between resistive and ferroelectric switching in ferroelectric tunnel junctions, and moreover, can be the source of novel concepts in memory devices and neuromorphic computing.

The electronic reconstruction occurring at oxide interfaces may be the source of interesting device concepts for future oxide electronics. Among oxide devices, multiferroic tunnel junctions are being actively investigated as they offer the possibility to modulate the junction current by independently controlling the switching of the magnetization of the electrodes and of the ferroelectric polarization of the barrier. In this Letter, we show that the spin reconstruction at the interfaces of a La_{0.7}Sr_{0.3}MnO_{3}/BaTiO_{3}/La_{0.7}Sr_{0.3}MnO_{3} multiferroic tunnel junction is the origin of a spin filtering functionality that can be turned on and off by reversing the ferroelectric polarization. The ferroelectrically controlled interface spin filter enables a giant electrical modulation of the tunneling magnetoresistance between values of 10% and 1000%, which could inspire device concepts in oxides-based low dissipation spintronics.

The peculiar features of domain walls observed in ferroelectrics make them promising active elements for next-generation non-volatile memories, logic gates and energy-harvesting devices. Although extensive research activity has been devoted recently to making full use of this technological potential, concrete realizations of working nanodevices exploiting these functional properties are yet to be demonstrated. Here, we fabricate a multiferroic tunnel junction based on ferromagnetic La 0.7 Sr 0.3 MnO 3 electrodes separated by an ultrathin ferroelectric BaTiO 3 tunnel barrier, where a head-to-head domain wall is constrained. An electron gas stabilized by oxygen vacancies is confined within the domain wall, displaying discrete quantum-well energy levels. These states assist resonant electron tunnelling processes across the barrier, leading to strong quantum oscillations of the electrical conductance.

At interfaces between complex oxides, electronic, orbital and magnetic reconstructions may produce states of matter absent from the materials involved, offering novel possibilities for electronic and spintronic devices. Here we show that magnetic reconstruction has a strong influence on the interfacial spin selectivity, a key parameter controlling spin transport in magnetic tunnel junctions. In epitaxial heterostructures combining layers of antiferromagnetic LaFeO(3) (LFO) and ferromagnetic La(0.7)Sr(0.3)MnO(3) (LSMO), we find that a net magnetic moment is induced in the first few unit planes of LFO near the interface with LSMO. Using X-ray photoemission electron microscopy, we show that the ferromagnetic domain structure of the manganite electrodes is imprinted into the antiferromagnetic tunnel barrier, endowing it with spin selectivity. Finally, we find that the spin arrangement resulting from coexisting ferromagnetic and antiferromagnetic interactions strongly influences the tunnel magnetoresistance of LSMO/LFO/LSMO junctions through competing spin-polarization and spin-filtering effects.

The magnetoresistance of La0.7Sr0.3MnO3/SrTiO3 superlattices with magnetic field rotating out-of-plane shows unexpected peaks for in-plane fields. Resistivity calculations with spin-orbit coupling reveal that orbital reconstruction at the manganite interface leads to a 2D ferromagnetic electron gas coupled antiparallel to the manganite "bulk". These orbital and magnetic reconstructions are supported by X-ray linear dichroism and ab initio calculations., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Electric-field control of magnetism has remained a major challenge which would greatly impact data storage technology. Although progress in this direction has been recently achieved, reversible magnetization switching by an electric field requires the assistance of a bias magnetic field. Here we take advantage of the novel electronic phenomena emerging at interfaces between correlated oxides and demonstrate reversible, voltage-driven magnetization switching without magnetic field. Sandwiching a non-superconducting cuprate between two manganese oxide layers, we find a novel form of magnetoelectric coupling arising from the orbital reconstruction at the interface between interfacial Mn spins and localized states in the CuO2 planes. This results in a ferromagnetic coupling between the manganite layers that can be controlled by a voltage. Consequently, magnetic tunnel junctions can be electrically toggled between two magnetization states, and the corresponding spin-dependent resistance states, in the absence of a magnetic field.

We report a strong effect of interface-induced magnetization on the transport properties of magnetic tunnel junctions consisting of ferromagnetic manganite La0.7Ca0.3MnO3 and insulating cuprate PrBa2Cu3O7. Contrary to the typically observed steady increase of the tunnel magnetoresistance with decreasing temperature, this system exhibits a sudden anomalous decrease at low temperatures. Interestingly, this anomalous behavior can be attributed to the competition between the positive spin polarization of the manganite contacts and the negative spin-filter effect from the interface-induced Cu magnetization.

Reducing the operation temperature of solid oxide fuel cells is a major challenge towards their widespread use for power generation. This has triggered an intense materials research effort involving the search for novel electrolytes with higher ionic conductivity near room temperature. Two main directions are being currently followed: the use of doping strategies for the synthesis of new bulk materials and the implementation of nanotechnology routes for the fabrication of artificial nanostructures with improved properties. In this paper, we review our recent work on solid oxide fuel cell electrolyte materials in these two directions, with special emphasis on the importance of disorder and reduced dimensionality in determining ion conductivity. Substitution of Ti for Zr in the A(2)Zr(2-) (y)Ti(y)O(7) (A = Y, Dy, and Gd) series, directly related to yttria stabilized zirconia (a common fuel cell electrolyte), allows controlling ion mobility over wide ranges. In the second scenario we describe the strong enhancement of the conductivity occurring at the interfaces of superlattices made by alternating strontium titanate and yttria stabilized zirconia ultrathin films. We conclude that cooperative effects in oxygen dynamics play a primary role in determining ion mobility of bulk and artificially nanolayered materials and should be considered in the design of new electrolytes with enhanced conductivity.

The search for electrolyte materials with high oxygen conductivities is a key step toward reducing the operation temperature of fuel cells, which is currently above 700 degrees C. We report a high lateral ionic conductivity, showing up to eight orders of magnitude enhancement near room temperature, in yttria-stabilized zirconia (YSZ)/strontium titanate epitaxial heterostructures. The enhancement of the conductivity is observed, along with a YSZ layer thickness-independent conductance, showing that it is an interface process. We propose that the atomic reconstruction at the interface between highly dissimilar structures (such as fluorite and perovskite) provides both a large number of carriers and a high-mobility plane, yielding colossal values of the ionic conductivity.

We show magnetoresistance in excess of 1000% in trilayers containing highly spin-polarized La0.7Ca0.3MnO3 and high-Tc superconducting YBa2Cu3O7. This large magnetoresistance is reminiscent of the giant magnetoresistance (GMR) in metallic superlattices but with much larger values, and originates at spin imbalance due to the injection of spin-polarized carriers. Furthermore, in contrast to ordinary GMR, the magnetoresistance is intimately related to the superconductivity in the YBa2Cu3O7 layer and vanishes in the normal state. This result, aside from its fundamental importance, may be of interest for the design of novel spintronic devices based on ferromagnet/superconductor structures.

Charge neutrality and stoichiometry impose severe restrictions on the mechanisms of epitaxial growth of complex oxides. The fundamental question arises of what is the minimum growth unit when sample thickness is reduced beyond the size of the unit cell. We have investigated the growth mechanism of YBa2Cu3O7 cuprate superconductor, using a consistent approach based on the growth of noninteger numbers of YBa2Cu3O7 layers in YBa(2)Cu(3)O(7)/PrBa(2)Cu3O7 superlattices. Ex situ chemical and structural analysis evidence a 2D block-by-block mechanism in which the minimum growth units are complete unit cell blocks, growing coherently over large lateral distances.