Hundred-Fold Enhancement in the Anomalous Hall Effect Induced by Hydrogenation.

The anomalous Hall effect (AHE) is one of the most fascinating transport properties in condensed matter physics. However, the AHE magnitude, which mainly depends on net spin polarization and band topology, is generally small in oxides and thus limits potential applications. Here, we demonstrate a giant enhancement of AHE in a LaCoO3-induced 5d itinerant ferromagnet SrIrO3 by hydrogenation. The anomalous Hall resistivity and anomalous Hall angle, which are two of the most critical parameters in AHE-based devices, are found to increase to 62.2 µΩ·cm and 3%, respectively, showing an unprecedentedly large enhancement ratio of ∼10000%. Theoretical analysis suggests the key roles of Berry curvature in enhancing AHE. Furthermore, the hydrogenation concomitantly induces the significant elevation of Curie temperature from 75 to 160 K and 40-fold reinforcement of coercivity. Such giant regulation and very large AHE magnitude observed in SrIrO3 could pave the path for 5d oxide devices.

Self-Optimized Ligand Effect of Single-Atom Modifier in Ternary Pt-Based Alloy for Efficient Hydrogen Oxidation.

Modifying the atomic and electronic structure of platinum-based alloy to enhance its activity and anti-CO poisoning ability is a vital issue in hydrogen oxidation reaction (HOR). However, the role of foreign modifier metal and the underlying ligand effect is not fully understood. Here, we propose that the ligand effect of single-atom Cu can dynamically modulate the d-band center of Pt-based alloy for boosting HOR performance. By in situ X-ray absorption spectroscopy, our research has identified that the potential-driven structural rearrangement into high-coordination Cu-Pt/Pd intensifies the ligand effect in Pt-Cu-Pd, leading to enhanced HOR performance. Thereby, modulating the d-band structure leads to near-optimal hydrogen/hydroxyl binding energies and reduced CO adsorption energies for promoting the HOR kinetics and the CO-tolerant capability. Accordingly, PtPdCu1/C exhibits excellent CO tolerance even at 1,000 ppm impurity.

Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO3.

The origin of strain-induced ferromagnetism, which is robust regardless of the type and degree of strain in LaCoO3 (LCO) thin films, is enigmatic despite intensive research efforts over the past decade. Here, by combining scanning transmission electron microscopy with ab initio density functional theory plus U calculations, we report that the ferromagnetism does not emerge directly from the strain itself but rather from the creation of compressed structural units within ferroelastically formed twin-wall domains. The compressed structural units are magnetically active with the rocksalt-type high-spin/low-spin order. Our study highlights that the ferroelastic nature of ferromagnetic structural units is important for understanding the intriguing ferromagnetic properties in LCO thin films.

Development of highly efficient ultraviolet LEDs on hybrid patterned sapphire substrates.

A hybrid patterned sapphire substrate (HPSS) aiming to achieve high-quality Al(Ga)N epilayers for the development of GaN-based ultraviolet light-emitting diodes (UV LEDs) has been prepared. The high-resolution X-ray diffraction measurements reveal that the Al(Ga)N epilayers grown on a HPSS and conventional patterned sapphire substrate (CPSS) have similar structural quality. More importantly, benefiting from the larger refractive index contrast between the patterned silica array and sapphire, the photons can escape from the hybrid substrate with an improved transmittance in the UV band. As a result, in comparison with the UV LEDs grown on the CPSS, the LEDs grown on the HPSS exhibit a significantly enhanced light output power by 14.5% and more than 22.9% higher peak external quantum efficiency, owing to the boost of the light extraction efficiency from the adoption of the HPSS which can be used as a promising substrate to realize high-efficiency and high-power UV LEDs of the future.

Metal-insulator-transition engineering by modulation tilt-control in perovskite nickelates for room temperature optical switching.

In transition metal perovskites ABO3, the physical properties are largely driven by the rotations of the BO6 octahedra, which can be tuned in thin films through strain and dimensionality control. However, both approaches have fundamental and practical limitations due to discrete and indirect variations in bond angles, bond lengths, and film symmetry by using commercially available substrates. Here, we introduce modulation tilt control as an approach to tune the ground state of perovskite oxide thin films by acting explicitly on the oxygen octahedra rotation modes-that is, directly on the bond angles. By intercalating the prototype SmNiO3 target material with a tilt-control layer, we cause the system to change the natural amplitude of a given rotation mode without affecting the interactions. In contrast to strain and dimensionality engineering, our method enables a continuous fine-tuning of the materials' properties. This is achieved through two independent adjustable parameters: the nature of the tilt-control material (through its symmetry, elastic constants, and oxygen rotation angles), and the relative thicknesses of the target and tilt-control materials. As a result, a magnetic and electronic phase diagram can be obtained, normally only accessible by A-site element substitution, within the single SmNiO3 compound. With this unique approach, we successfully adjusted the metal-insulator transition (MIT) to room temperature to fulfill the desired conditions for optical switching applications.

Spin chirality fluctuation in two-dimensional ferromagnets with perpendicular magnetic anisotropy.

Non-coplanar spin textures with scalar spin chirality can generate an effective magnetic field that deflects the motion of charge carriers, resulting in a topological Hall effect (THE)1-3. However, spin chirality fluctuations in two-dimensional ferromagnets with perpendicular magnetic anisotropy have not been considered so far. Here, we report evidence of spin chirality fluctuations by probing the THE above the Curie temperature in two different ferromagnetic ultra-thin films, SrRuO3 and V-doped Sb2Te3. The temperature, magnetic field, thickness and carrier-type dependence of the THE signal, along with Monte Carlo simulations, suggest that spin chirality fluctuations are a common phenomenon in two-dimensional ferromagnets with perpendicular magnetic anisotropy. Our results open a path for exploring spin chirality with topological Hall transport in two-dimensional magnets and beyond4-7.

Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure.

In the bulk, LaCoO_{3} (LCO) is a paramagnet, yet the low-temperature ferromagnetism (FM) is observed in tensile strained thin films, and its origin remains unresolved. Here, we quantitatively measured the distribution of atomic density and magnetization in LCO films by polarized neutron reflectometry (PNR) and found that the LCO layers near the heterointerfaces exhibit a reduced magnetization but an enhanced atomic density, whereas the film's interior (i.e., its film bulk) shows the opposite trend. We attribute the nonuniformity to the symmetry mismatch at the interface, which induces a structural distortion related to the ferroelasticity of LCO. This assertion is tested by systematic application of hydrostatic pressure during the PNR experiments. The magnetization can be controlled at a rate of -20.4% per GPa. These results provide unique insights into mechanisms driving FM in strained LCO films while offering a tantalizing observation that tunable deformation of the CoO_{6} octahedra in combination with the ferroelastic order parameter.

Spin Direction-Controlled Electronic Band Structure in Two-Dimensional Ferromagnetic CrI3.

Manipulating physical properties using the spin degree of freedom constitutes a major part of modern condensed matter physics and is a key aspect for spintronics devices. Using the newly discovered two-dimensional van der Waals ferromagnetic CrI3 as a prototype material, we theoretically demonstrated a giant magneto band-structure (GMB) effect whereby a change of magnetization direction significantly modifies the electronic band structure. Our density functional theory calculations and model analysis reveal that rotating the magnetic moment of CrI3 from out-of-plane to in-plane causes a direct-to-indirect bandgap transition, inducing a magnetic field controlled photoluminescence. Moreover, our results show a significant change of Fermi surface with different magnetization directions, giving rise to giant anisotropic magnetoresistance. Additionally, the spin reorientation is found to modify the topological states. Given that a variety of properties are determined by band structures, our predicted GMB effect in CrI3 opens a new paradigm for spintronics applications.

Quantum Anomalous Hall State in Ferromagnetic SrRuO_{3} (111) Bilayers.

SrRuO_{3} heterostructures grown in the (111) direction are a rare example of thin film ferromagnets. By means of density functional theory plus dynamical mean field theory we show that the half-metallic ferromagnetic state with an ordered magnetic moment of 2 µ_{B}/Ru survives the ultimate dimensional confinement down to a bilayer, even at elevated temperatures of 500 K. In the minority channel, the spin-orbit coupling opens a gap at the linear band crossing corresponding to 3/4 filling of the t_{2g} shell. We predict that the emergent phase is Haldane's quantum anomalous Hall state with Chern number C=1, without an external magnetic field or magnetic impurities.

Stoichiometry, Orbital Configuration, and Metal-to-Insulator Transition in Nd0.8Sr0.2NiO3 Films.

The discovery of superconductivity in the infinite-layer nickelate Nd0.8Sr0.2NiO2 has motivated tremendous efforts for its significance toward the understanding of high-temperature superconductivity. However, the synthesis of infinite-layer nickelates is instable and has become a hindrance to experimental progress. Optimizing the growth of precursor Nd0.8Sr0.2NiO3 by pulsed laser deposition is crucial for obtaining infinite-layer nickelates. By systematically investigating the growth of Nd0.8Sr0.2NiO3 with wide range of conditions, we found that the laser fluence plays a critical role in determining the stoichiometry, lattice structure, and electronic properties. A higher Ni deficiency and larger c-axis lattice constant appeared with the lower laser fluence. At 0.6 J/cm2, the Ni deficiency is as large as 25%. According to X-ray absorption spectra and X-ray linear dichroism, we further find that (i) there are no obvious changes of the Ni valence and (ii) the energy level of the dx2-y2 orbital gradually increases relative to the d3z2-r2 orbital with increasing Ni deficiency. What is more, the onset temperature and magnitude of the resistivity change at the metal-to-insulator transitions (MITs) also are found to decrease with increasing laser fluence during the growth.

A broad-spectrum gas sensor based on correlated two-dimensional electron gas.

Designing a broad-spectrum gas sensor capable of identifying gas components in complex environments, such as mixed atmospheres or extreme temperatures, is a significant concern for various technologies, including energy, geological science, and planetary exploration. The main challenge lies in finding materials that exhibit high chemical stability and wide working temperature range. Materials that amplify signals through non-chemical methods could open up new sensing avenues. Here, we present the discovery of a broad-spectrum gas sensor utilizing correlated two-dimensional electron gas at a delta-doped LaAlO3/SrTiO3 interface with LaFeO3. Our study reveals that a back-gating on this two-dimensional electron gas can induce a non-volatile metal to insulator transition, which consequently can activate the two-dimensional electron gas to sensitively and quantitatively probe very broad gas species, no matter whether they are polar, non-polar, or inert gases. Different gas species cause resistance change at their sublimation or boiling temperature and a well-defined phase transition angle can quantitatively determine their partial pressures. Such unique correlated two-dimensional electron gas sensor is not affected by gas mixtures and maintains a wide operating temperature range. Furthermore, its readout is a simple measurement of electric resistance change, thus providing a very low-cost and high-efficient broad-spectrum sensing technique.

Emergence of Insulating Ferrimagnetism and Perpendicular Magnetic Anisotropy in 3d-5d Perovskite Oxide Composite Films for Insulator Spintronics.

Magnetic insulators with strong perpendicular magnetic anisotropy (PMA) play a key role in exploring pure spin current phenomena and developing ultralow-dissipation spintronic devices, rendering them highly desirable to develop new material platforms. Here, we report the epitaxial growth of La2/3Sr1/3MnO3 (LSMO)-SrIrO3 (SIO) composite oxide films (LSMIO) with different crystalline orientations fabricated by a sequential two-target ablation process by pulsed laser deposition. The LSMIO films exhibit high crystalline quality with a homogeneous mixture of LSMO and SIO at an atomic level. Ferrimagnetic and insulating transport characteristics are observed, with the temperature-dependent electric resistivity well fitted by the Mott variable-range-hopping model. Moreover, the LSMIO films show strong PMA. By further constructing all-perovskite-oxide heterostructures of the ferrimagnetic insulator LSMIO and a strong spin-orbital-coupled SIO layer, pronounced spin Hall magnetoresistance (SMR) and spin Hall-like anomalous Hall effect (SH-AHE) were observed. These results illustrate the potential application of the ferrimagnetic insulator LSMIO in developing all-oxide ultralow-dissipation spintronic devices.

Controllable Itinerant Ferromagnetism in Weakly Correlated 5d SrIrO3.

The weakly correlated nature of 5d oxide SrIrO3 determines its rare ferromagnetism, and the control of its magnetic order is even less studied. Tailoring structure distortion is currently a main route to tune the magnetic order of 5d iridates, but only for the spatially confined insulating counterparts. Here, we have realized ferromagnetic order in metallic SrIrO3 by construction of SrIrO3/ferromagnetic-insulator (LaCoO3) superlattices, which reveal a giant coercivity of ∼10 T and saturation field of ∼25 T with strong perpendicular magnetic anisotropy. The Curie temperature of SrIrO3 can be controlled by engineering interface charge transfer, which is confirmed by Hall effect measurements collaborating with EELS and XAS. Besides, the noncoplanar spin texture is captured, which is caused by interfacial Dzyaloshinskii-Moriya interactions as well. These results indicate controllable itinerant ferromagnetism and an emergent topological magnetic state in strong spin-orbit coupled semimetal SrIrO3, showing great potential to develop efficient spintronic devices.

Emergent Ferroelectricity in Otherwise Nonferroelectric Oxides by Oxygen Vacancy Design at Heterointerfaces.

Introducing point defects in complex metal oxides is a very effective route to engineer crystal symmetry and therefore control physical properties. However, the inversion symmetry breaking, which is vital for many tantalizing properties, such as ferroelectricity and chiral spin structure, is usually hard to be induced in the bulk crystal by point defects. By designing the oxygen vacancy formation energy profile and migration path across the oxide heterostructure, our first-principles density functional theory (DFT) calculations demonstrate that the point defects can effectively break the inversion symmetry and hence create novel ferroelectricity in superlattices consisting of otherwise nonferroelectric materials SrTiO3 and SrRuO3. This induced ferroelectricity can be significantly enhanced by reducing the SrTiO3 thickness. Inspired by theory calculation, SrTiO3/SrRuO3 superlattices were experimentally fabricated and are found to exhibit surprising strong ferroelectric properties. Our finding paves a simple and effective pathway to engineer the inversion symmetry and thus properties by point defect control in oxide heterostructures.

Nanoscale ferroelastic twins formed in strained LaCoO3 films.

The coexistence and coupling of ferroelasticity and magnetic ordering in a single material offers a great opportunity to realize novel devices with multiple tuning knobs. Complex oxides are a particularly promising class of materials to find multiferroic interactions due to their rich phase diagrams, and are sensitive to external perturbations. Still, there are very few examples of these systems. Here, we report the observation of twin domains in ferroelastic LaCoO3 epitaxial films and their geometric control of structural symmetry intimately linked to the material's electronic and magnetic states. A unidirectional structural modulation is achieved by selective choice of substrates having twofold rotational symmetry. This modulation perturbs the crystal field-splitting energy, leading to unexpected in-plane anisotropy of orbital configuration and magnetization. These findings demonstrate the use of structural modulation to control multiferroic interactions and may enable a great potential for stimulation of exotic phenomena through artificial domain engineering.

Large orbital polarization in nickelate-cuprate heterostructures by dimensional control of oxygen coordination.

Artificial heterostructures composed of dissimilar transition metal oxides provide unprecedented opportunities to create remarkable physical phenomena. Here, we report a means to deliberately control the orbital polarization in LaNiO3 (LNO) through interfacing with SrCuO2 (SCO), which has an infinite-layer structure for CuO2. Dimensional control of SCO results in a planar-type (P-SCO) to chain-type (C-SCO) structure transition depending on the SCO thickness. This transition is exploited to induce either a NiO5 pyramidal or a NiO6 octahedral structure at the SCO/LNO interface. Consequently, a large change in the Ni d orbital occupation up to ~30% is achieved in P-SCO/LNO superlattices, whereas the Ni eg orbital splitting is negligible in C-SCO/LNO superlattices. The engineered oxygen coordination triggers a metal-to-insulator transition in SCO/LNO superlattices. Our results demonstrate that interfacial oxygen coordination engineering provides an effective means to manipulate the orbital configuration and associated physical properties, paving a pathway towards the advancement of oxide electronics.

Growing a LaAlO3/SrTiO3 heterostructure on Ca2Nb3O10 nanosheets.

The two-dimensional electron liquid which forms between the band insulators LaAlO3 (LAO) and SrTiO3 (STO) is a promising component for oxide electronics, but the requirement of using single crystal SrTiO3 substrates for the growth limits its applications in terms of device fabrication. It is therefore important to find ways to deposit these materials on other substrates, preferably Si, or Si-based, in order to facilitate integration with existing technology. Interesting candidates are micron-sized nanosheets of Ca2Nb3O10 which can be used as seed layers for perovskite materials on any substrate. We have used low-energy electron microscopy (LEEM) with in-situ pulsed laser deposition to study the subsequent growth of STO and LAO on such flakes which were deposited on Si. We can follow the morphology and crystallinity of the layers during growth, as well as fingerprint their electronic properties with angle resolved reflected electron spectroscopy. We find that STO layers, deposited on the nanosheets, can be made crystalline and flat; that LAO can be grown in a layer-by-layer fashion; and that the full heterostructure shows the signature of the formation of a conducting interface.

Oxygen Diode Formed in Nickelate Heterostructures by Chemical Potential Mismatch.

Deliberate control of oxygen vacancy formation and migration in perovskite oxide thin films is important for developing novel electronic and iontronic devices. Here, it is found that the concentration of oxygen vacancies (VO ) formed in LaNiO3 (LNO) during pulsed laser deposition is strongly affected by the chemical potential mismatch between the LNO film and its proximal layers. Increasing the VO concentration in LNO significantly modifies the degree of orbital polarization and drives the metal-insulator transition. Changes in the nickel oxidization state and carrier concentration in the films are confirmed by soft X-ray absorption spectroscopy and optical spectroscopy. The ability to unidirectional-control the oxygen flow across the heterointerface, e.g., a so-called "oxygen diode", by exploiting chemical potential mismatch at interfaces provides a new avenue to tune the physical and electrochemical properties of complex oxides.

The swelling transition of lepidocrocite-type protonated layered titanates into anatase under hydrothermal treatment.

The common facets of anatase crystals are the (001) and (101) planes. However, the phase transformation from lepidocrocite-type titanate into anatase by hydrothermal processing yields an anatase microstructure with high concentration of exposed (010) planes. The phase transformation of a lepidocrocite-type protonated layered titanate (HTO) into anatase was studied using XRD, TEM, FTIR, and measurement of pH and zeta potential. It was found that HTO is proton-deficient. The phase transformation process begins after uptake of a sufficient number of protons into the lepidocrocite-type structure. With the uptake of protons new hydroxyl groups form on the internal surfaces of the layered titanate and result in a bilayer state of HTO. The phase transformation reaction is a topotactic dehydration reaction in which anatase forms and water is expelled by syneresis.

In situ TEM studies of oxygen vacancy migration for electrically induced resistance change effect in cerium oxides.

Oxide materials with resistance hysteresis are very promising for next generation memory devices. However, the microscopic dynamic process of the resistance change is still elusive. Here, we use in situ transmission electron microscopy method to study the role of oxygen vacancies for the resistance switching effect in cerium oxides. The structure change during oxygen vacancy migration in CeO(2) induced by electric field was in situ imaged inside high-resolution transmission electron microscope, which gives a direct evidence for oxygen migration mechanism for the microscopic origin of resistance change effect in CeO(2). Our results have implications for understanding the nature of resistance change in metal oxides with mixed valence cations, such as fluorite, rutile and perovskite oxides.