Tunable Magnetoelastic Effects in Voltage-Controlled Exchange-Coupled Composite Multiferroic Microstructures.

The magnetoelectric properties of exchange-coupled Ni/CoFeB-based composite multiferroic microstructures are investigated. The strength and sign of the magnetoelastic effect are found to be strongly correlated with the ratio between the thicknesses of two magnetostrictive materials. In cases where the thickness ratio deviates significantly from one, the magnetoelastic behavior of the multiferroic microstructures is dominated by the thicker layer, which contributes more strongly to the observed magnetoelastic effect. More symmetric structures with a thickness ratio equal to one show an emergent interfacial behavior which cannot be accounted for simply by summing up the magnetoelastic effects occurring in the two constituent layers. This aspect is clearly visible in the case of ultrathin bilayers, where the exchange coupling drastically affects the magnetic behavior of the Ni layer, making the Ni/CoFeB bilayer a promising next-generation synthetic magnetic system entirely. This study demonstrates the richness and high tunability of composite multiferroic systems based on coupled magnetic bilayers compared to their single magnetic layer counterparts. Furthermore, because of the compatibility of CoFeB with present magnetic tunnel junction-based spintronic technologies, the reported findings are expected to be of great interest for the development of ultralow-power magnetoelectric memory devices.

Coherent ac spin current transmission across an antiferromagnetic CoO insulator.

The recent discovery of spin current transmission through antiferromagnetic insulating materials opens up vast opportunities for fundamental physics and spintronics applications. The question currently surrounding this topic is: whether and how could THz antiferromagnetic magnons mediate a GHz spin current? This mismatch of frequencies becomes particularly critical for the case of coherent ac spin current, raising the fundamental question of whether a GHz ac spin current can ever keep its coherence inside an antiferromagnetic insulator and so drive the spin precession of another ferromagnet layer coherently? Utilizing element- and time-resolved x-ray pump-probe measurements on Py/Ag/CoO/Ag/Fe75Co25/MgO(001) heterostructures, here we demonstrate that a coherent GHz ac spin current pumped by the Py ferromagnetic resonance can transmit coherently across an antiferromagnetic CoO insulating layer to drive a coherent spin precession of the Fe75Co25 layer. Further measurement results favor thermal magnons rather than evanescent spin waves as the mediator of the coherent ac spin current in CoO.

Observation of room-temperature polar skyrmions.

Complex topological configurations are fertile ground for exploring emergent phenomena and exotic phases in condensed-matter physics. For example, the recent discovery of polarization vortices and their associated complex-phase coexistence and response under applied electric fields in superlattices of (PbTiO3)n/(SrTiO3)n suggests the presence of a complex, multi-dimensional system capable of interesting physical responses, such as chirality, negative capacitance and large piezo-electric responses1-3. Here, by varying epitaxial constraints, we discover room-temperature polar-skyrmion bubbles in a lead titanate layer confined by strontium titanate layers, which are imaged by atomic-resolution scanning transmission electron microscopy. Phase-field modelling and second-principles calculations reveal that the polar-skyrmion bubbles have a skyrmion number of +1, and resonant soft-X-ray diffraction experiments show circular dichroism, confirming chirality. Such nanometre-scale polar-skyrmion bubbles are the electric analogues of magnetic skyrmions, and could contribute to the advancement of ferroelectrics towards functionalities incorporating emergent chirality and electrically controllable negative capacitance.

Anomalous orbital structure in two-dimensional titanium dichalcogenides.

Generally, lattice distortions play a key role in determining the electronic ground states of materials. Although it is well known that trigonal distortions are generic to most two dimensional transition metal dichalcogenides, the impact of this structural distortion on the electronic structure and topological properties has not been understood conclusively. Here, by using a combination of polarization dependent X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) and atomic multiplet cluster calculations, we have investigated the electronic structure of titanium dichalcogenides TiX2 (X = S, Se, Te), where the magnitude of the trigonal distortion increase monotonically from S to Se and Te. Our results reveal the presence of an anomalously large crystal field splitting. This unusual kind of crystal field splitting is likely responsible for the unconventional electronic structure of TiX2 compounds and ultimately controls the degree of the electronic phase protection. Our findings also indicate the drawback of the distorted crystal field picture in explaining the observed electronic ground state and emphasize the key importance of trigonal symmetry, metal-ligand hybridization and electron-electron correlations in defining the electronic structures at the Fermi energy.

Decoupling Carrier Concentration and Electron-Phonon Coupling in Oxide Heterostructures Observed with Resonant Inelastic X-Ray Scattering.

We report the observation of multiple phonon satellite features in ultrathin superlattices of the form nSrIrO_{3}/mSrTiO_{3} using resonant inelastic x-ray scattering (RIXS). As the values of n and m vary, the energy loss spectra show a systematic evolution in the relative intensity of the phonon satellites. Using a closed-form solution for the RIXS cross section, we extract the variation in the electron-phonon coupling strength as a function of n and m. Combined with the negligible carrier doping into the SrTiO_{3} layers, these results indicate that the tuning of the electron-phonon coupling can be effectively decoupled from doping. This work both showcases a feasible method to extract the electron-phonon coupling in superlattices and unveils a potential route for tuning this coupling, which is often associated with superconductivity in SrTiO_{3}-based systems.

Nature of the metal-insulator transition in few-unit-cell-thick LaNiO3 films.

The nature of the metal-insulator transition in thin films and superlattices of LaNiO3 only a few unit cells in thickness remains elusive despite tremendous effort. Quantum confinement and epitaxial strain have been evoked as the mechanisms, although other factors such as growth-induced disorder, cation non-stoichiometry, oxygen vacancies, and substrate-film interface quality may also affect the observable properties of ultrathin films. Here we report results obtained for near-ideal LaNiO3 films with different thicknesses and terminations grown by atomic layer-by-layer laser molecular beam epitaxy on LaAlO3 substrates. We find that the room-temperature metallic behavior persists until the film thickness is reduced to an unprecedentedly small 1.5 unit cells (NiO2 termination). Electronic structure measurements using X-ray absorption spectroscopy and first-principles calculation suggest that oxygen vacancies existing in the films also contribute to the metal-insulator transition.

Effect of (1 1 1)-oriented strain on the structure and magnetic properties of La0.7Sr0.3MnO3 thin films.

Using strain, i.e. subtle changes in lattice constant in a thin film induced by the underlying substrate, opens up intriguing new ways to control material properties. We present a study of the effects of strain on structural and ferromagnetic properties of (1 1 1)pc-oriented La0.7Sr0.3MnO3 epitaxial thin films grown on NdGaO3, SrTiO3, and DyScO3 substrates. (The subscript pc denotes the pseudo-cubic symmetry.) The results show that La0.7Sr0.3MnO3 assumes a monoclinic unit cell on NdGaO3 and DyScO3 and a rhombohedral unit cell on SrTiO3. For La0.7Sr0.3MnO3 on NdGaO3 and DyScO3 a uniaxial magnetic anisotropy is found, while La0.7Sr0.3MnO3 on SrTiO3 is magnetically isotropic. The Néel model is used to explain the anisotropy of the thin films on NdGaO3 and SrTiO3, however, for La0.7Sr0.3MnO3 on DyScO3 the effect of octahedral rotations needs to be included through the single ion model. Through examination of the Curie temperature of the strained films we suggest that (1 1 1)-strain has a different effect on the Jahn-Teller splitting of e g and t 2g electron levels than what is seen in (0 0 1)pc-oriented La0.7Sr0.3MnO3 thin films.

Artificial two-dimensional polar metal at room temperature.

Polar metals, commonly defined by the coexistence of polar crystal structure and metallicity, are thought to be scarce because the long-range electrostatic fields favoring the polar structure are expected to be fully screened by the conduction electrons of a metal. Moreover, reducing from three to two dimensions, it remains an open question whether a polar metal can exist. Here we report on the realization of a room temperature two-dimensional polar metal of the B-site type in tri-color (tri-layer) superlattices BaTiO3/SrTiO3/LaTiO3. A combination of atomic resolution scanning transmission electron microscopy with electron energy-loss spectroscopy, optical second harmonic generation, electrical transport, and first-principles calculations have revealed the microscopic mechanisms of periodic electric polarization, charge distribution, and orbital symmetry. Our results provide a route to creating all-oxide artificial non-centrosymmetric quasi-two-dimensional metals with exotic quantum states including coexisting ferroelectric, ferromagnetic, and superconducting phases.

Electron Accumulation and Emergent Magnetism in LaMnO_{3}/SrTiO_{3} Heterostructures.

Emergent phenomena at polar-nonpolar oxide interfaces have been studied intensely in pursuit of next-generation oxide electronics and spintronics. Here we report the disentanglement of critical thicknesses for electron reconstruction and the emergence of ferromagnetism in polar-mismatched LaMnO_{3}/SrTiO_{3} (001) heterostructures. Using a combination of element-specific x-ray absorption spectroscopy and dichroism, and first-principles calculations, interfacial electron accumulation, and ferromagnetism have been observed within the polar, antiferromagnetic insulator LaMnO_{3}. Our results show that the critical thickness for the onset of electron accumulation is as thin as 2 unit cells (UC), significantly thinner than the observed critical thickness for ferromagnetism of 5 UC. The absence of ferromagnetism below 5 UC is likely induced by electron overaccumulation. In turn, by controlling the doping of the LaMnO_{3}, we are able to neutralize the excessive electrons from the polar mismatch in ultrathin LaMnO_{3} films and thus enable ferromagnetism in films as thin as 3 UC, extending the limits of our ability to synthesize and tailor emergent phenomena at interfaces and demonstrating manipulation of the electronic and magnetic structures of materials at the shortest length scales.

Direct Detection of Pure ac Spin Current by X-Ray Pump-Probe Measurements.

Despite recent progress in spin-current research, the detection of spin current has mostly remained indirect. By synchronizing a microwave waveform with synchrotron x-ray pulses, we use the ferromagnetic resonance of the Py (Ni_{81}Fe_{19}) layer in a Py/Cu/Cu_{75}Mn_{25}/Cu/Co multilayer to pump a pure ac spin current into the Cu_{75}Mn_{25} and Co layers, and then directly probe the spin current within the Cu_{75}Mn_{25} layer and the spin dynamics of the Co layer by x-ray magnetic circular dichroism. This element-resolved pump-probe measurement unambiguously identifies the ac spin current in the Cu_{75}Mn_{25} layer.

Interfacial Symmetry Control of Emergent Ferromagnetism at the Nanoscale.

The emergence of complex new ground states at interfaces has been identified as one of the most promising routes to highly tunable nanoscale materials. Despite recent progress, isolating and controlling the underlying mechanisms behind these emergent properties remains among the most challenging materials physics problems to date. In particular, generating ferromagnetism localized at the interface of two nonferromagnetic materials is of fundamental and technological interest. Moreover, the ability to turn the ferromagnetism on and off would shed light on the origin of such emergent phenomena and is promising for spintronic applications. We demonstrate that ferromagnetism confined within one unit cell at the interface of CaRuO3 and CaMnO3 can be switched on and off by changing the symmetry of the oxygen octahedra connectivity at the boundary. Interfaces that are symmetry-matched across the boundary exhibit interfacial CaMnO3 ferromagnetism while the ferromagnetism at symmetry-mismatched interfaces is suppressed. We attribute the suppression of ferromagnetic order to a reduction in charge transfer at symmetry-mismatched interfaces, where frustrated bonding weakens the orbital overlap. Thus, interfacial symmetry is a new route to control emergent ferromagnetism in materials such as CaMnO3 that exhibit antiferromagnetism in bulk form.

Correlation-Driven Insulator-Metal Transition in Near-Ideal Vanadium Dioxide Films.

We use polarization- and temperature-dependent x-ray absorption spectroscopy, in combination with photoelectron microscopy, x-ray diffraction, and electronic transport measurements, to study the driving force behind the insulator-metal transition in VO_{2}. We show that both the collapse of the insulating gap and the concomitant change in crystal symmetry in homogeneously strained single-crystalline VO_{2} films are preceded by the purely electronic softening of Coulomb correlations within V-V singlet dimers. This process starts 7 K (±0.3 K) below the transition temperature, as conventionally defined by electronic transport and x-ray diffraction measurements, and sets the energy scale for driving the near-room-temperature insulator-metal transition in this technologically promising material.

Observation of a three-dimensional quasi-long-range electronic supermodulation in YBa2Cu3O(7-x)/La0.7Ca0.3MnO3 heterostructures.

Recent developments in high-temperature superconductivity highlight a generic tendency of the cuprates to develop competing electronic (charge) supermodulations. While coupled with the lattice and showing different characteristics in different materials, these supermodulations themselves are generally conceived to be quasi-two-dimensional, residing mainly in individual CuO2 planes, and poorly correlated along the c axis. Here we observed with resonant elastic X-ray scattering a distinct type of electronic supermodulation in YBa2Cu3O(7-x) (YBCO) thin films grown epitaxially on La0.7Ca0.3MnO3 (LCMO). This supermodulation has a periodicity nearly commensurate with four lattice constants in-plane, eight out of plane, with long correlation lengths in three dimensions. It sets in far above the superconducting transition temperature and competes with superconductivity below this temperature for electronic states predominantly in the CuO2 plane. Our finding sheds light on the nature of charge ordering in cuprates as well as a reported long-range proximity effect between superconductivity and ferromagnetism in YBCO/LCMO heterostructures.

Magnetic Interactions at the Nanoscale in Trilayer Titanates.

We report on the phase diagram of competing magnetic interactions at the nanoscale in engineered ultrathin trilayer heterostructures of LaTiO_{3}/SrTiO_{3}/YTiO_{3}, in which the interfacial inversion symmetry is explicitly broken. Combined atomic layer resolved scanning transmission electron microscopy with electron energy loss spectroscopy and electrical transport have confirmed the formation of a spatially separated two-dimensional electron liquid and high density two-dimensional localized magnetic moments at the LaTiO_{3}/SrTiO_{3} and SrTiO_{3}/YTiO_{3} interfaces, respectively. Resonant soft x-ray linear dichroism spectroscopy has demonstrated the presence of orbital polarization of the conductive LaTiO_{3}/SrTiO_{3} and localized SrTiO_{3}/YTiO_{3} electrons. Our results provide a route with prospects for exploring new magnetic interfaces, designing a tunable two-dimensional d-electron Kondo lattice, and potential spin Hall applications.

Observation of polar vortices in oxide superlattices.

The complex interplay of spin, charge, orbital and lattice degrees of freedom provides a plethora of exotic phases and physical phenomena. In recent years, complex spin topologies have emerged as a consequence of the electronic band structure and the interplay between spin and spin-orbit coupling in materials. Here we produce complex topologies of electrical polarization--namely, nanometre-scale vortex-antivortex (that is, clockwise-anticlockwise) arrays that are reminiscent of rotational spin topologies--by making use of the competition between charge, orbital and lattice degrees of freedom in superlattices of alternating lead titanate and strontium titanate layers. Atomic-scale mapping of the polar atomic displacements by scanning transmission electron microscopy reveals the presence of long-range ordered vortex-antivortex arrays that exhibit nearly continuous polarization rotation. Phase-field modelling confirms that the vortex array is the low-energy state for a range of superlattice periods. Within this range, the large gradient energy from the vortex structure is counterbalanced by the corresponding large reduction in overall electrostatic energy (which would otherwise arise from polar discontinuities at the lead titanate/strontium titanate interfaces) and the elastic energy associated with epitaxial constraints and domain formation. These observations have implications for the creation of new states of matter (such as dipolar skyrmions, hedgehog states) and associated phenomena in ferroic materials, such as electrically controllable chirality.

Chirality switching and winding or unwinding of the antiferromagnetic NiO domain walls in Fe/NiO/Fe/CoO/Ag(001).

Fe/NiO/Fe/CoO/Ag(001) single crystalline films were grown epitaxially and investigated by x-ray magnetic circular dichroism and x-ray magnetic linear dichroism. The bottom Fe layer magnetization is pinned through exchange coupling to the CoO layer and the top Fe layer magnetization can be rotated by an in-plane external magnetic field. We find that the NiO spins wind up to form a domain wall due to the perpendicular NiO/Fe interfacial coupling as the top layer Fe magnetization rotates from 0° to 90°, but switch wall chirality and unwind the wall as the Fe magnetization rotates from 90° to 180°. This observation shows that Mauri's 180° domain wall does not exist in perpendicularly coupled ferromagnetic-antiferromagnetic systems in the strong coupling regime.

Tailoring the topology of an artificial magnetic skyrmion.

Despite theoretical predictions, it remains an experimental challenge to realize an artificial magnetic skyrmion whose topology can be well controlled and tailored so that its topological effect can be revealed explicitly in a deformation of the spin textures. Here we report epitaxial magnetic thin films in which an artificial skyrmion is created by embedding a magnetic vortex into an out-of-plane aligned spin environment. By changing the relative orientation between the central vortex core polarity and the surrounding out-of-plane spins, we are able to control and tailor the system between two skyrmion topological states. An in-plane magnetic field is used to annihilate the skyrmion core by converting the central vortex state into a single domain state. Our result shows distinct annihilation behaviour of the skyrmion core for the two different skyrmion states, suggesting a topological effect of the magnetic skyrmions in the core annihilation process.

Ferrous iron formation following the co-aggregation of ferric iron and the Alzheimer's disease peptide ß-amyloid (1-42).

For decades, a link between increased levels of iron and areas of Alzheimer's disease (AD) pathology has been recognized, including AD lesions comprised of the peptide ß-amyloid (Aß). Despite many observations of this association, the relationship between Aß and iron is poorly understood. Using X-ray microspectroscopy, X-ray absorption spectroscopy, electron microscopy and spectrophotometric iron(II) quantification techniques, we examine the interaction between Aß(1-42) and synthetic iron(III), reminiscent of ferric iron stores in the brain. We report Aß to be capable of accumulating iron(III) within amyloid aggregates, with this process resulting in Aß-mediated reduction of iron(III) to a redox-active iron(II) phase. Additionally, we show that the presence of aluminium increases the reductive capacity of Aß, enabling the redox cycling of the iron. These results demonstrate the ability of Aß to accumulate iron, offering an explanation for previously observed local increases in iron concentration associated with AD lesions. Furthermore, the ability of iron to form redox-active iron phases from ferric precursors provides an origin both for the redox-active iron previously witnessed in AD tissue, and the increased levels of oxidative stress characteristic of AD. These interactions between Aß and iron deliver valuable insights into the process of AD progression, which may ultimately provide targets for disease therapies.

Room-temperature antiferromagnetic memory resistor.

The bistability of ordered spin states in ferromagnets provides the basis for magnetic memory functionality. The latest generation of magnetic random access memories rely on an efficient approach in which magnetic fields are replaced by electrical means for writing and reading the information in ferromagnets. This concept may eventually reduce the sensitivity of ferromagnets to magnetic field perturbations to being a weakness for data retention and the ferromagnetic stray fields to an obstacle for high-density memory integration. Here we report a room-temperature bistable antiferromagnetic (AFM) memory that produces negligible stray fields and is insensitive to strong magnetic fields. We use a resistor made of a FeRh AFM, which orders ferromagnetically roughly 100 K above room temperature, and therefore allows us to set different collective directions for the Fe moments by applied magnetic field. On cooling to room temperature, AFM order sets in with the direction of the AFM moments predetermined by the field and moment direction in the high-temperature ferromagnetic state. For electrical reading, we use an AFM analogue of the anisotropic magnetoresistance. Our microscopic theory modelling confirms that this archetypical spintronic effect, discovered more than 150 years ago in ferromagnets, is also present in AFMs. Our work demonstrates the feasibility of fabricating room-temperature spintronic memories with AFMs, which in turn expands the base of available magnetic materials for devices with properties that cannot be achieved with ferromagnets.