Revealing emergent magnetic charge in an antiferromagnet with diamond quantum magnetometry.

Whirling topological textures play a key role in exotic phases of magnetic materials and are promising for logic and memory applications. In antiferromagnets, these textures exhibit enhanced stability and faster dynamics with respect to their ferromagnetic counterparts, but they are also difficult to study due to their vanishing net magnetic moment. One technique that meets the demand of highly sensitive vectorial magnetic field sensing with negligible backaction is diamond quantum magnetometry. Here we show that an archetypal antiferromagnet-haematite-hosts a rich tapestry of monopolar, dipolar and quadrupolar emergent magnetic charge distributions. The direct read-out of the previously inaccessible vorticity of an antiferromagnetic spin texture provides the crucial connection to its magnetic charge through a duality relation. Our work defines a paradigmatic class of magnetic systems to explore two-dimensional monopolar physics, and highlights the transformative role that diamond quantum magnetometry could play in exploring emergent phenomena in quantum materials.

Topological Flat Bands in Graphene Super-Moiré Lattices.

Moiré-pattern-based potential engineering has become an important way to explore exotic physics in a variety of two-dimensional condensed matter systems. While these potentials have induced correlated phenomena in almost all commonly studied 2D materials, monolayer graphene has remained an exception. We demonstrate theoretically that a single layer of graphene, when placed between two bulk boron nitride crystal substrates with the appropriate twist angles, can support a robust topological ultraflat band emerging as the second hole band. This is one of the simplest platforms to design and exploit topological flat bands.

Tunable Magnetic Properties in Sr2FeReO6 Double-Perovskite.

Double-perovskite oxides have attracted recent attention due to their attractive functionalities and application potential. In this paper, we demonstrate the effect of dual controls, i.e., the deposition pressure of oxygen (PO2) and lattice mismatch (ε), on tuning magnetic properties in epitaxial double-perovskite Sr2FeReO6 films. In a nearly lattice matched Sr2FeReO6/SrTiO3 film, the ferrimagnetic-to-paramagnetic phase transition occurs when PO2 is reduced to 30 mTorr, probably due to the formation of Re4+ ions that replace the stoichiometric Re5+ to cause disorders of B-site ions. On the other hand, a large compressive strain or tensile strain shifts this critical PO2 to below 1 mTorr or above 40 mTorr, respectively. The observations can be attributed to the modulation of B-site ordering by epitaxial strain through affecting elemental valence. Our results provide a feasible way to expand the functional tunability of magnetic double-perovskite oxides that hold great promise for spintronic devices.

Chemical Vapor Deposition of Superconducting FeTe1-xSex Nanosheets.

FeTe1-xSex, a promising layered material used to realize Majorana zero modes, has attracted enormous attention in recent years. Pulsed laser deposition (PLD) and molecular-beam epitaxy (MBE) are the routine growth methods used to prepare FeTe1-xSex thin films. However, both methods require high-vacuum conditions and polished crystalline substrates, which hinder the exploration of the topological superconductivity and related nanodevices of this material. Here we demonstrate the growth of the ultrathin FeTe1-xSex superconductor by a facile, atmospheric pressure chemical vapor deposition (CVD) method. The composition and thickness of the two-dimensional (2D) FeTe1-xSex nanosheets are well controlled by tuning the experimental conditions. The as-prepared FeTe0.8Se0.2 nanosheet exhibits an onset superconducting transition temperature of 12.4 K, proving its high quality. Our work offers an effective strategy for preparing the ultrathin FeTe1-xSex superconductor, which could become a promising platform for further study of the unconventional superconductivity in the FeTe1-xSex system.

Magnetic Anisotropy of a Quasi Two-Dimensional Canted Antiferromagnet.

We report the control of the interplane magnetic exchange coupling in CaIrO3 perovskite thin films and superlattices with SrTiO3. By analyzing the anisotropic magneto-transport data, we demonstrate that a semimetallic paramagnetic CaIrO3 turns into a canted antiferromagnetic Mott insulator at reduced dimensions. The emergence of a biaxial magneto-crystalline anisotropy indicates the canted moment responding to the cubic symmetry. Extending to superlattices and probing oxygen octahedral rotation by half-integer X-ray Braggs diffraction, a more complete picture about the canted moment evolution with interplane coupling can be understood. Remarkably, a rotation of the canted moments' easy axes by 45° is also observed by a sign reversal of the in-plane strain. These results demonstrate the robustness of anisotropic magnetoresistance in revealing quasi two-dimensional canted antiferromagnets, as well as valuable insights about quadrupolar magnetoelastic coupling, relevant for designing future antiferromagnetic spintronic devices.

Characteristic Lengths of Interlayer Charge Transfer in Correlated Oxide Heterostructures.

Using interlayer interaction to control functional heterostructures with atomic-scale designs has become one of the most effective interface-engineering strategies nowadays. Here, we demonstrate the effect of a crystalline LaFeO3 buffer layer on amorphous and crystalline LaAlO3/SrTiO3 heterostructures. The LaFeO3 buffer layer acts as an energetically favored electron acceptor in both LaAlO3/SrTiO3 systems, resulting in modulation of interfacial carrier density and hence metal-to-insulator transition. For amorphous and crystalline LaAlO3/SrTiO3 heterostructures, the metal-to-insulator transition is found when the LaFeO3 layer thickness crosses 3 and 6 unit cells, respectively. Such different critical LaFeO3 thicknesses are explained in terms of distinct characteristic lengths of the redox-reaction-mediated and polar-catastrophe-dominated charge transfer, controlled by the interfacial atomic contact and Thomas-Fermi screening effect, respectively. Our results not only shed light on the complex interlayer charge transfer across oxide heterostructures but also provide a new route to precisely tailor the charge-transfer process at a functional interface.

Emergent Topological Hall Effect at a Charge-Transfer Interface.

Exploring exotic interface magnetism due to charge transfer and strong spin-orbit coupling has profound application in the future development of spintronic memory. Here, the emergence and tuning of topological Hall effect (THE) from a CaMnO3 /CaIrO3 /CaMnO3 trilayer structure are studied in detail, which suggests the presence of magnetic Skyrmion-like bubbles. First, by tilting the magnetic field direction, the evolution of the Hall signal suggests a transformation of Skyrmions into topologically-trivial stripe domains, consistent with behaviors predicted by micromagnetic simulations. Second, by varying the thickness of CaMnO3 , the optimal thicknesses for the THE signal emergence are found, which allow identification of the source of Dzyaloshinskii-Moriya interaction (DMI) and its competition with antiferromagnetic superexchange. Employing high-resolution transmission electron microscopy, randomly distributed stacking faults are identified only at the bottom interface and may avoid mutual cancellation of DMI. Last, a spin-transfer torque experiment also reveals a low threshold current density of ≈109 A m-2 for initiating the bubbles' motion. This discovery sheds light on a possible strategy for integrating Skyrmions with antiferromagnetic spintronics.

Phase Diagram and Superconducting Dome of Infinite-Layer Nd_{1-x}Sr_{x}NiO_{2} Thin Films.

Infinite-layer Nd_{1-x}Sr_{x}NiO_{2} thin films with Sr doping level x from 0.08 to 0.3 are synthesized and investigated. We find a superconducting dome x between 0.12 and 0.235 accompanied by a weakly insulating behavior in both under- and overdoped regimes. The dome is akin to that in the electron-doped 214-type and infinite-layer cuprate superconductors. For x≥0.18, the normal state Hall coefficient (R_{H}) changes the sign from negative to positive as the temperature decreases. The temperature of the sign changes decreases monotonically with decreasing x from the overdoped side and approaches the superconducting dome at the midpoint, suggesting a reconstruction of the Fermi surface with the dopant concentration across the dome.

Electromechanically Reconfigurable Terahertz Stereo Metasurfaces.

Dynamic terahertz devices are vital for the next generation of wireless communication, sensing, and non-destructive imaging technologies. Metasurfaces have emerged as a paradigm-shifting platform, offering varied functionalities, miniaturization, and simplified fabrication compared to their 3D counterparts. However, the presence of in-plane mirror symmetry and reduced degree of freedom impose fundamental limitations on achieving advanced chiral response, beamforming, and reconfiguration capabilities. In this work, a platform composed of electrically actuated resonators that can be colossally reconfigured between planar and 3D geometries is demonstrated. To illustrate the platform, metadevices with 3D Split Ring Resonators are fabricated, wherein two counteracting driving forces are combined: i) folding induced by stress mismatch, which enables non-volatile state design and ii) unfolding triggered by the strain associated with insulator-to-metal transition in VO2, which facilitates volatile structural reconfiguration. This large structural reconfiguration space allows for resonance mode switching, widely tunable magnetic and electric polarizabilities, and increased frequency agility. Moreover, the unique properties of VO2, such as the hysteretic nature of its phase transition is harnessed to demonstrate a multi-state memory. Therefore, these VO2 integrated metadevices are highly attractive for the realization of 6G communication devices such as reconfigurable intelligent surfaces, holographic beam formers, and spatial light modulators.

Superconductivity in infinite-layer nickelate La1-xCaxNiO2 thin films.

We report the observation of superconductivity in infinite-layer Ca-doped LaNiO2 (La1-xCaxNiO2) thin films and construct their phase diagram. Unlike the metal-insulator transition in Nd- and Pr-based nickelates, the undoped and underdoped La1-xCaxNiO2 thin films are entirely insulating from 300 K down to 2 K. A superconducting dome is observed at 0.15 < x < 0.3 with weakly insulating behavior at the overdoped regime. Moreover, the sign of the Hall coefficient RH changes at low temperature for samples with a higher doping level. However, distinct from the Nd- and Pr-based nickelates, the RH-sign-change temperature remains at around 35 K as the doping increases, which begs further theoretical and experimental investigation to reveal the role of the 4f orbital to the (multi)band nature of the superconducting nickelates. Our results also emphasize a notable role of lattice correlation on the multiband structures of the infinite-layer nickelates.

Optically Controllable 2D Material/Complex Oxide Heterointerface.

Heterostructures play a vital role in functional devices on the basis of the individual constituents. Non-conventional heterostructures formed by stacking 2D materials onto structurally distinct materials are of great interest in achieving novel phenomena that are both scientifically and technologically relevant. Here, a heterostructure based on a 2D (molybdenum ditelluride) MoTe2 and an amorphous strontium titanium oxide (a-STO) thin film is reported. The heterostructure functions as a high-performance photodetector, which exhibits anomalous negative photoresponse in the pristine device due to the scattering effect from the light-induced Oδ- ions. The photoresponsivity and the specific detectivity are found to be >104 AW-1 and >1013 Jones, respectively, which are significantly higher than those in standard MoTe2 devices. Moreover, through tuning the light programming time, the photodetection behavior of the MoTe2/a-STO heterostructure experiences a dynamic evolution from negative to positive. This is due to the optically controllable modulation of the interfacial states, which is further confirmed by the X-ray photoelectron spectroscopy and photoluminescence measurements. It is envisioned that the 2D material/a-STO heterostructure could be a potential platform for exploring new functional devices.

Atomic Origin of Interface-Dependent Oxygen Migration by Electrochemical Gating at the LaAlO3-SrTiO3 Heterointerface.

Electrical control of material properties based on ionic liquids (IL) has seen great development and emerging applications in the field of functional oxides, mainly understood by the electrostatic and electrochemical gating mechanisms. Compared to the fast, flexible, and reproducible electrostatic gating, electrochemical gating is less controllable owing to the complex behaviors of ion migration. Here, the interface-dependent oxygen migration by electrochemical gating is resolved at the atomic scale in the LaAlO3-SrTiO3 system through ex situ IL gating experiments and on-site atomic-resolution characterization. The difference between interface structures leads to the controllable electrochemical oxygen migration by filling oxygen vacancies. The findings not only provide an atomic-scale insight into the origin of interface-dependent electrochemical gating but also demonstrate an effective way of engineering interface structure to control the electrochemical gating.

Room-Temperature Colossal Magnetoresistance in Terraced Single-Layer Graphene.

Disorder-induced magnetoresistance (MR) effect is quadratic at low perpendicular magnetic fields and linear at high fields. This effect is technologically appealing, especially in 2D materials such as graphene, since it offers potential applications in magnetic sensors with nanoscale spatial resolution. However, it is a great challenge to realize a graphene magnetic sensor based on this effect because of the difficulty in controlling the spatial distribution of disorder and enhancing the MR sensitivity in the single-layer regime. Here, a room-temperature colossal MR of up to 5000% at 9 T is reported in terraced single-layer graphene. By laminating single-layer graphene on a terraced substrate, such as TiO2 -terminated SrTiO3 , a universal one order of magnitude enhancement in the MR compared to conventional single-layer graphene devices is demonstrated. Strikingly, a colossal MR of >1000% is also achieved in the terraced graphene even at a high carrier density of ≈1012 cm-2 . Systematic studies of the MR of single-layer graphene on various oxide- and non-oxide-based terraced surfaces demonstrate that the terraced structure is the dominant factor driving the MR enhancement. The results open a new route for tailoring the physical property of 2D materials by engineering the strain through a terraced substrate.

Interfacial Oxygen-Driven Charge Localization and Plasmon Excitation in Unconventional Superconductors.

Charge localization is critical to the control of charge dynamics in systems such as perovskite solar cells, organic-, and nanostructure-based photovoltaics. However, the precise control of charge localization via electronic transport or defect engineering is challenging due to the complexity in reaction pathways and environmental factors. Here, charge localization in optimal-doped La1.85 Sr0.15 CuO4 thin-film on SrTiO3 substrate (LSCO/STO) is investigated, and also a high-energy plasmon is observed. Charge localization manifests as a near-infrared mid-gap state in LSCO/STO. This is ascribed to the interfacial hybridization between the Ti3d-orbitals of the substrate and O2p-orbitals of the film. The interfacial effect leads to significant changes in the many-body correlations and local-field effect. The local-field effect results in an inhomogeneous charge distribution, and due to perturbation by an external field, the high polarizability of this nonuniform charge system eventually generates the high-energy plasmon. Transformation of the electronic correlations in LSCO/STO is further demonstrated via temperature-dependent spectral-weight transfer. This study of charge localization in cuprates and interfacial hybridization provides important clues to their electronic structures and superconductive properties.

Phase-controllable growth of ultrathin 2D magnetic FeTe crystals.

Two-dimensional (2D) magnets with intrinsic ferromagnetic/antiferromagnetic (FM/AFM) ordering are highly desirable for future spintronic devices. However, the direct growth of their crystals is in its infancy. Here we report a chemical vapor deposition approach to controllably grow layered tetragonal and non-layered hexagonal FeTe nanoplates with their thicknesses down to 3.6 and 2.8 nm, respectively. Moreover, transport measurements reveal these obtained FeTe nanoflakes show a thickness-dependent magnetic transition. Antiferromagnetic tetragonal FeTe with the Néel temperature (TN) gradually decreases from 70 to 45 K as the thickness declines from 32 to 5 nm. And ferromagnetic hexagonal FeTe is accompanied by a drop of the Curie temperature (TC) from 220 K (30 nm) to 170 K (4 nm). Theoretical calculations indicate that the ferromagnetic order in hexagonal FeTe is originated from its concomitant lattice distortion and Stoner instability. This study highlights its potential applications in future spintronic devices.

Erasable and recreatable two-dimensional electron gas at the heterointerface of SrTiO3 and a water-dissolvable overlayer.

While benefiting greatly from electronics, our society also faces a major problem of electronic waste, which has already caused environmental pollution and adverse human health effects. Therefore, recyclability becomes a must-have feature in future electronics. Here, we demonstrate an erasable and recreatable two-dimensional electron gas (2DEG), which can be easily created and patterned by depositing a water-dissolvable overlayer of amorphous Sr3Al2O6 (a-SAO) on SrTiO3 (STO) at room temperature. The 2DEG can be repeatedly erased or recreated by depositing the a-SAO or dissolving in water, respectively. Photoluminescence results show that the 2DEG arises from the a-SAO-induced oxygen vacancy. Furthermore, by gradually depleting the 2DEG, a transition of nonlinear to linear Hall effect is observed, demonstrating an unexpected interfacial band structure. The convenience and repeatability in the creation of the water-dissolvable 2DEG with rich physics could potentially contribute to the exploration of next generation electronics, such as environment-friendly or water-soluble electronics.

Modulation of New Excitons in Transition Metal Dichalcogenide-Perovskite Oxide System.

The exciton, a quasi-particle that creates a bound state of an electron and a hole, is typically found in semiconductors. It has attracted major attention in the context of both fundamental science and practical applications. Transition metal dichalcogenides (TMDs) are a new class of 2D materials that include direct band-gap semiconductors with strong spin-orbit coupling and many-body interactions. Manipulating new excitons in semiconducting TMDs could generate a novel means of application in nanodevices. Here, the observation of high-energy excitonic peaks in the monolayer-MoS2 on a SrTiO3 heterointerface generated by a new complex mechanism is reported, based on a comprehensive study that comprises temperature-dependent optical spectroscopies and first-principles calculations. The appearance of these excitons is attributed to the change in many-body interactions that occurs alongside the interfacial orbital hybridization and spin-orbit coupling brought about by the excitonic effect propagated from the substrate. This has further led to the formation of a Fermi-surface feature at the interface. The results provide an atomic-scale understanding of the heterointerface between monolayer-TMDs and perovskite oxide and highlight the importance of spin-orbit-charge-lattice coupling on the intrinsic properties of atomic-layer heterostructures, which open up a way to manipulate the excitonic effects in monolayer TMDs via an interfacial system.