Scanning gradiometry with a single spin quantum magnetometer.

Quantum sensors based on spin defects in diamond have recently enabled detailed imaging of nanoscale magnetic patterns, such as chiral spin textures, two-dimensional ferromagnets, or superconducting vortices, based on a measurement of the static magnetic stray field. Here, we demonstrate a gradiometry technique that significantly enhances the measurement sensitivity of such static fields, leading to new opportunities in the imaging of weakly magnetic systems. Our method relies on the mechanical oscillation of a single nitrogen-vacancy center at the tip of a scanning diamond probe, which up-converts the local spatial gradients into ac magnetic fields enabling the use of sensitive ac quantum protocols. We show that gradiometry provides important advantages over static field imaging: (i) an order-of-magnitude better sensitivity, (ii) a more localized and sharper image, and (iii) a strong suppression of field drifts. We demonstrate the capabilities of gradiometry by imaging the nanotesla fields appearing above topographic defects and atomic steps in an antiferromagnet, direct currents in a graphene device, and para- and diamagnetic metals.

Bulk-like dielectric and magnetic properties of sub 100 nm thick single crystal Cr2O3 films on an epitaxial oxide electrode.

The manipulation of antiferromagnetic order in magnetoelectric Cr2O3 using electric field has been of great interest due to its potential in low-power electronics. The substantial leakage and low dielectric breakdown observed in twinned Cr2O3 thin films, however, hinders its development in energy efficient spintronics. To compensate, large film thicknesses (250 nm or greater) have been employed at the expense of device scalability. Recently, epitaxial V2O3 thin film electrodes have been used to eliminate twin boundaries and significantly reduce the leakage of 300 nm thick single crystal films. Here we report the electrical endurance and magnetic properties of thin (less than 100 nm) single crystal Cr2O3 films on epitaxial V2O3 buffered Al2O3 (0001) single crystal substrates. The growth of Cr2O3 on isostructural V2O3 thin film electrodes helps eliminate the existence of twin domains in Cr2O3 films, therefore significantly reducing leakage current and increasing dielectric breakdown. 60 nm thick Cr2O3 films show bulk-like resistivity (~ 1012 Ω cm) with a breakdown voltage in the range of 150-300 MV/m. Exchange bias measurements of 30 nm thick Cr2O3 display a blocking temperature of ~ 285 K while room temperature optical second harmonic generation measurements possess the symmetry consistent with bulk magnetic order.

The ultrathin limit of improper ferroelectricity.

The secondary nature of polarization in improper ferroelectrics promotes functional properties beyond those of conventional ferroelectrics. In technologically relevant ultrathin films, however, the improper ferroelectric behavior remains largely unexplored. Here, we probe the emergence of the coupled improper polarization and primary distortive order parameter in thin films of hexagonal YMnO3. Combining state-of-the-art in situ characterization techniques separately addressing the improper ferroelectric state and its distortive driving force, we reveal a pronounced thickness dependence of the improper polarization, which we show to originate from the strong modification of the primary order at epitaxial interfaces. Nanoscale confinement effects on the primary order parameter reduce the temperature of the phase transition, which we exploit to visualize its order-disorder character with atomic resolution. Our results advance the understanding of the evolution of improper ferroelectricity within the confinement of ultrathin films, which is essential for their successful implementation in nanoscale applications.

Depolarizing-Field Effects in Epitaxial Capacitor Heterostructures.

We identify a transient enhancement of the depolarizing field, leading to an unexpected quench of net polarization, during the growth of a prototypical metal-ferroelectric-metal epitaxial system made of BaTiO_{3} and SrRuO_{3}. Reduced conductivity and, hence, charge screening efficiency in the early growth stage of the SrRuO_{3} top electrode promotes a breakdown of ferroelectric BaTiO_{3} into domains. We demonstrate how a thermal annealing procedure can recover the single-domain state. By tracking the polarization state in situ, using optical second harmonic generation, we bring new understanding to interface-related electrostatic effects in ferroelectric capacitors.

Metastable monoclinic [110] layered perovskite Dy2Ti2O7 thin films for ferroelectric applications.

Using the Combinatorial Substrate Epitaxy (CSE) approach, we report the stabilization of Dy2Ti2O7 epitaxial monoclinic, layered-perovskite phase Dy2Ti2O7 thin films. To achieve this, the films are deposited on high density, polished La2Ti2O7 polycrystalline ceramic substrates, which are stable as monoclinic layered-perovskites, and were prepared by conventional sintering. Microstructural analysis using electron backscatter diffraction (EBSD), electron diffraction (ED), and high-resolution transmission electron microscopy (HRTEM) support this observation. Further, they reveal that the cubic pyrochlore phase is observed far from the interface as films are grown thicker (100 nm), confirming the importance of substrate-induced phase and space group selection. This works reinforces the vast potential of CSE to promote the stabilization of metastable phases, thus giving access to new functional oxide materials, across a range of novel material systems including ferroelectrics.

Deterministic switching of ferromagnetism at room temperature using an electric field.

The technological appeal of multiferroics is the ability to control magnetism with electric field. For devices to be useful, such control must be achieved at room temperature. The only single-phase multiferroic material exhibiting unambiguous magnetoelectric coupling at room temperature is BiFeO3 (refs 4 and 5). Its weak ferromagnetism arises from the canting of the antiferromagnetically aligned spins by the Dzyaloshinskii-Moriya (DM) interaction. Prior theory considered the symmetry of the thermodynamic ground state and concluded that direct 180-degree switching of the DM vector by the ferroelectric polarization was forbidden. Instead, we examined the kinetics of the switching process, something not considered previously in theoretical work. Here we show a deterministic reversal of the DM vector and canted moment using an electric field at room temperature. First-principles calculations reveal that the switching kinetics favours a two-step switching process. In each step the DM vector and polarization are coupled and 180-degree deterministic switching of magnetization hence becomes possible, in agreement with experimental observation. We exploit this switching to demonstrate energy-efficient control of a spin-valve device at room temperature. The energy per unit area required is approximately an order of magnitude less than that needed for spin-transfer torque switching. Given that the DM interaction is fundamental to single-phase multiferroics and magnetoelectrics, our results suggest ways to engineer magnetoelectric switching and tailor technologically pertinent functionality for nanometre-scale, low-energy-consumption, non-volatile magnetoelectronics.

Functional ferroic heterostructures with tunable integral symmetry.

The relation between symmetry and functionality was pinpointed by Pierre Curie who stated that it is the symmetry breaking that creates physical properties. This fundamental principle is nowadays used for engineering heterostructures whose integral symmetry leads to exotic phenomena such as one-way transparency. For switching devices, however, such symmetry-related functionalities cannot be used because the symmetry in conventional heterostructures is immutable once the material has been synthesized. Here we demonstrate a concept for post-growth symmetry control in PbZr0.2Ti0.8O3 and BiFeO3-based heterostructures. A conducting oxide is sandwiched between two ferroelectric layers, and inversion symmetry is reversibly switched on or off by layer-selective electric-field poling. The generalization of our approach to other materials and symmetries is discussed. We thus establish ferroic trilayer structures as device components with reversibly tunable symmetry and demonstrate their use as light emitters that can be activated and deactivated by applying moderate electric voltages.

Electric-field-induced magnetization reversal in a ferromagnet-multiferroic heterostructure.

A reversal of magnetization requiring only the application of an electric field can lead to low-power spintronic devices by eliminating conventional magnetic switching methods. Here we show a nonvolatile, room temperature magnetization reversal determined by an electric field in a ferromagnet-multiferroic system. The effect is reversible and mediated by an interfacial magnetic coupling dictated by the multiferroic. Such electric-field control of a magnetoelectric device demonstrates an avenue for next-generation, low-energy consumption spintronics.

Microscopic origin of the giant ferroelectric polarization in tetragonal-like BiFeO(3).

We report direct experimental evidence for a room-temperature, ∼130 µC/cm(2) ferroelectric polarization from the tetragonal-like BiFeO(3) phase. The physical origin of this remarkable enhancement of ferroelectric polarization has been investigated by a combination of x-ray absorption spectroscopy, scanning transmission electron microscopy, and first principles calculations. A large strain-induced Fe-ion displacement relative to the oxygen octahedra, combined with the contribution of Bi 6s lone pair electrons, is the mechanism driving the large ferroelectric polarization in this tetragonal-like phase.

How to obtain a magnetic hard-soft architecture by pulsed laser deposition.

In spin valve type systems, one ferromagnetic electrode must be magnetically hard to act as a reference layer while the other electrode must be magnetically soft to act as a sensor or storage layer. This magnetic hard-soft architecture can usually be obtained by four different methods: the use of two ferromagnets with different coercive fields (here CoFe(2) and Ni(80)Fe(20)), the use of an underlayer enhancing the coercive field of one of the two ferromagnets (here Ta and Ru), the use of a ferromagnet coupled to a ferrimagnet or antiferromagnet (here NiO/CoFe(2) and CoFe(2)O(4)/CoFe(2)), or the use of an artificial antiferromagnet (here CoFe(2)/Ru/CoFe(2)). We show that at least the first and the third methods seem to work with pulsed laser deposition in the thermodynamic conditions used.