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The properties of magnetic nanoparticles tend to be depressed by the unavoidable presence of a magnetically inactive surface layer. However, outstanding magnetic properties with a room-temperature magnetization near the bulk value can be produced by high-temperature synthesis methods involving capping with organic acid. The capping molecules are not magnetic, so the origin of the enhanced magnetization remains elusive. In this work, we present a real-space characterization on the subnanometer scale of the magnetic, chemical, and structural properties of iron-oxide nanoparticles via aberration-corrected scanning transmission electron microscopy. For the first time, electron magnetic chiral dichroism is used to map the magnetization of nanoparticles in real space with subnanometer spatial resolution. We find that the surface of the nanoparticles is magnetically ordered. Combining the results with density functional calculations, we establish how magnetization is restored in the surface layer. The bonding with the acid's O atoms results in O-Fe atomic configuration and distances close to bulk values. We conclude that the nature and number of molecules in the capping layer is an essential ingredient in the fabrication of nanoparticles with optimal magnetic properties.

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 CuO 2 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.

Complex oxides displaying ferroelectric and/or multiferroic behavior are of high fundamental and applied interest. In this work, we show that it is possible to achieve polar order in a superlattice made up of two nonpolar oxides by means of oxygen vacancy ordering. Using scanning transmission electron microscopy imaging, we show the polar displacement of magnetic Fe ions in a superlattice of (LaFeO3)2/(SrFeO3) grown on a SrTiO3 substrate. Using density functional theory calculations, we systematically study the effect of epitaxial strain, octahedral rotations, and surface terminations in the superlattice and find them to have a negligible effect on the antipolar displacements of the Fe ions lying in between SrO and LaO layers of the superlattice (i.e., within La0.5Sr0.5FeO3 unit cells). The introduction of oxygen vacancies, on the other hand, triggers a polar displacement of the Fe ions. We confirm this important result using electron energy loss spectroscopy, which shows partial oxygen vacancy ordering in the region where polar displacements are observed and an absence of vacancy ordering outside of that area.

Defects in ceramic materials are generally seen as detrimental to their functionality and applicability. Yet, in some complex oxides, defects present an opportunity to enhance some of their properties or even lead to the discovery of exciting physics, particularly in the presence of strong correlations. A paradigmatic case is the high‐temperature superconductor YBa2Cu3O7‐δ (Y123), in which nanoscale defects play an important role as they can immobilize quantized magnetic flux vortices. Here previously unforeseen point defects buried in Y123 thin films that lead to the formation of ferromagnetic clusters embedded within the superconductor are unveiled. Aberration‐corrected scanning transmission microscopy has been used for exploring, on a single unit‐cell level, the structure and chemistry resulting from these complex point defects, along with density functional theory calculations, for providing new insights about their nature including an unexpected defect‐driven ferromagnetism, and X‐ray magnetic circular dichroism for bearing evidence of Cu magnetic moments that align ferromagnetically even below the superconducting critical temperature to form a dilute system of magnetic clusters associated with the point defects.

The proximity effect in a model manganite-cuprate system is investigated theoretically. We consider a situation in which spin-polarized electrons in manganite layers antiferromagnetically couple with electrons in cuprate layers as observed experimentally. The effect of the interfacial magnetic coupling is found to be much stronger than the injection of spin-polarized electrons into the cuprate region. As a result, the superconducting transition temperature depends on the thickness of the cuprate layer significantly. Since the magnetic coupling creates negative polarization, an applied magnetic field and the negative polarization compete, resulting in the inverse spin-switch behavior where the superconducting transition temperature is increased by applying a magnetic field.