The field-free Josephson diode in a van der Waals heterostructure.

The superconducting analogue to the semiconducting diode, the Josephson diode, has long been sought with multiple avenues to realization being proposed by theorists1-3. Showing magnetic-field-free, single-directional superconductivity with Josephson coupling, it would serve as the building block for next-generation superconducting circuit technology. Here we realized the Josephson diode by fabricating an inversion symmetry breaking van der Waals heterostructure of NbSe2/Nb3Br8/NbSe2. We demonstrate that even without a magnetic field, the junction can be superconducting with a positive current while being resistive with a negative current. The ΔIc behaviour (the difference between positive and negative critical currents) with magnetic field is symmetric and Josephson coupling is proved through the Fraunhofer pattern. Also, stable half-wave rectification of a square-wave excitation was achieved with a very low switching current density, high rectification ratio and high robustness. This non-reciprocal behaviour strongly violates the known Josephson relations and opens the door to discover new mechanisms and physical phenomena through integration of quantum materials with Josephson junctions, and provides new avenues for superconducting quantum devices.

Catalogue of flat-band stoichiometric materials.

Topological electronic flattened bands near or at the Fermi level are a promising route towards unconventional superconductivity and correlated insulating states. However, the related experiments are mostly limited to engineered materials, such as moiré systems1-3. Here we present a catalogue of the naturally occuring three-dimensional stoichiometric materials with flat bands around the Fermi level. We consider 55,206 materials from the Inorganic Crystal Structure Database catalogued using the Topological Quantum Chemistry website4,5, which provides their structural parameters, space group, band structure, density of states and topological characterization. We combine several direct signatures and properties of band flatness with a high-throughput analysis of all crystal structures. In particular, we identify materials hosting line-graph or bipartite sublattices-in either two or three dimensions-that probably lead to flat bands. From this trove of information, we create the Materials Flatband Database website, a powerful search engine for future theoretical and experimental studies. We use the database to extract a curated list of 2,379 high-quality flat-band materials, from which we identify 345 promising candidates that potentially host flat bands with charge centres that are not strongly localized on the atomic sites. We showcase five representative materials and provide a theoretical explanation for the origin of their flat bands close to the Fermi energy using the S-matrix method introduced in a parallel work6.

Heterodimensional superlattice with in-plane anomalous Hall effect.

Superlattices-a periodic stacking of two-dimensional layers of two or more materials-provide a versatile scheme for engineering materials with tailored properties1,2. Here we report an intrinsic heterodimensional superlattice consisting of alternating layers of two-dimensional vanadium disulfide (VS2) and a one-dimensional vanadium sulfide (VS) chain array, deposited directly by chemical vapour deposition. This unique superlattice features an unconventional 1T stacking with a monoclinic unit cell of VS2/VS layers identified by scanning transmission electron microscopy. An unexpected Hall effect, persisting up to 380 kelvin, is observed when the magnetic field is in-plane, a condition under which the Hall effect usually vanishes. The observation of this effect is supported by theoretical calculations, and can be attributed to an unconventional anomalous Hall effect owing to an out-of-plane Berry curvature induced by an in-plane magnetic field, which is related to the one-dimensional VS chain. Our work expands the conventional understanding of superlattices and will stimulate the synthesis of more extraordinary superstructures.

Strain-driven formation of epitaxial nanostructures in brownmillerite strontium cobaltite thin films.

Nanostructured materials can display unique physical properties and are of particular interest for their new functionalities. Epitaxial growth is a promising approach for the controlled synthesis of nanostructures with desired structures and crystallinity. SrCoOx is a particularly intriguing material owing to a topotactic phase transition between an antiferromagnetic insulating brownmillerite SrCoO2.5 (BM-SCO) phase and a ferromagnetic metallic perovskite SrCoO3-δ (P-SCO) phase depending on the oxygen concentration. Here, we present the formation and control of epitaxial BM-SCO nanostructures by substrate-induced anisotropic strain. Perovskite substrates with a (110)-orientation and which allow for compressive strain result in the creation of BM-SCO nanobars, while (111)-oriented substrates give rise to the formation of BM-SCO nanoislands. We have found that substrate-induced anisotropic strain coupled with the orientation of crystalline domains determines the shape and facet of the nanostructures, while their size can be tuned by the degree of strain. Moreover, the nanostructures can be transformed between antiferromagnetic BM-SCO and ferromagnetic P-SCO via ionic liquid gating. Thus, this study provides insights into the design of epitaxial nanostructures whose structure and physical properties can be readily controlled.

Non-Majorana modes in diluted spin chains proximitized to a superconductor.

Spin chains proximitized with superconducting condensates have emerged as one of the most promising platforms for the realization of Majorana modes. Here, we craft diluted spin chains atom by atom following a seminal theoretical proposal suggesting indirect coupling mechanisms as a viable route to trigger topological superconductivity. Starting from single adatoms hosting deep Shiba states, we use the highly anisotropic Fermi surface of the substrate to create spin chains characterized by different magnetic configurations along distinct crystallographic directions. By scrutinizing a large set of parameters we reveal the ubiquitous emergence of boundary modes. Although mimicking signatures of Majorana modes, the end modes are identified as topologically trivial Shiba states. Our work demonstrates that zero-energy modes in spin chains proximitized to superconductors are not necessarily a link to Majorana modes while simultaneously identifying other experimental platforms, driving mechanisms, and test protocols for the determination of topologically nontrivial superconducting phases.

Scaling of Berry-curvature monopole dominated large linear positive magnetoresistance.

The linear positive magnetoresistance (LPMR) is a widely observed phenomenon in topological materials, which is promising for potential applications on topological spintronics. However, its mechanism remains ambiguous yet, and the effect is thus uncontrollable. Here, we report a quantitative scaling model that correlates the LPMR with the Berry curvature, based on a ferromagnetic Weyl semimetal CoS2 that bears the largest LPMR of over 500% at 2 K and 9 T, among known magnetic topological semimetals. In this system, masses of Weyl nodes existing near the Fermi level, revealed by theoretical calculations, serve as Berry-curvature monopoles and low-effective-mass carriers. Based on the Weyl picture, we propose a relation [Formula: see text], with B being the applied magnetic field and [Formula: see text] the average Berry curvature near the Fermi surface, and further introduce temperature factor to both MR/B slope (MR per unit field) and anomalous Hall conductivity, which establishes the connection between the model and experimental measurements. A clear picture of the linearly slowing down of carriers, i.e., the LPMR effect, is demonstrated under the cooperation of the k-space Berry curvature and real-space magnetic field. Our study not only provides experimental evidence of Berry curvature-induced LPMR but also promotes the common understanding and functional designing of the large Berry-curvature MR in topological Dirac/Weyl systems for magnetic sensing or information storage.

Terahertz Spin-Conductance Spectroscopy: Probing Coherent and Incoherent Ultrafast Spin Tunneling.

Thin-film stacks F|H consisting of a ferromagnetic-metal layer F and a heavy-metal layer H are spintronic model systems. Here, we present a method to measure the ultrabroadband spin conductance across a layer X between F and H at terahertz frequencies, which are the natural frequencies of spin-transport dynamics. We apply our approach to MgO tunneling barriers with thickness d = 0-6 Å. In the time domain, the spin conductance Gs has two components. An instantaneous feature arises from processes like coherent spin tunneling. Remarkably, a longer-lived component is a hallmark of incoherent resonant spin tunneling mediated by MgO defect states, because its relaxation time grows monotonically with d to as much as 270 fs at d = 6.0 Å. Our results are in full agreement with an analytical model. They indicate that terahertz spin-conductance spectroscopy will yield new and relevant insights into ultrafast spin transport in a wide range of spintronic nanostructures.

Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels.

The niobium oxide polymorph T-Nb2O5 has been extensively investigated in its bulk form especially for applications in fast-charging batteries and electrochemical (pseudo)capacitors. Its crystal structure, which has two-dimensional (2D) layers with very low steric hindrance, allows for fast Li-ion migration. However, since its discovery in 1941, the growth of single-crystalline thin films and its electronic applications have not yet been realized, probably due to its large orthorhombic unit cell along with the existence of many polymorphs. Here we demonstrate the epitaxial growth of single-crystalline T-Nb2O5 thin films, critically with the ionic transport channels oriented perpendicular to the film's surface. These vertical 2D channels enable fast Li-ion migration, which we show gives rise to a colossal insulator-metal transition, where the resistivity drops by 11 orders of magnitude due to the population of the initially empty Nb 4d0 states by electrons. Moreover, we reveal multiple unexplored phase transitions with distinct crystal and electronic structures over a wide range of Li-ion concentrations by comprehensive in situ experiments and theoretical calculations, which allow for the reversible and repeatable manipulation of these phases and their distinct electronic properties. This work paves the way for the exploration of novel thin films with ionic channels and their potential applications.

Observation of the Fluctuation Spin Hall Effect in a Low-Resistivity Antiferromagnet.

The spin Hall effect (SHE) can generate a pure spin current by an electric current, which is promisingly used to electrically control magnetization. To reduce the power consumption of this control, a giant spin Hall angle (SHA) in the SHE is desired in low-resistivity systems for practical applications. Here, critical spin fluctuation near the antiferromagnetic (AFM) phase transition in chromium (Cr) is proven to be an effective mechanism for creating an additional part of the SHE, named the fluctuation spin Hall effect. The SHA is significantly enhanced when the temperature approaches the Néel temperature (TN) of Cr and has a peak value of -0.36 near TN. This value is higher than the room-temperature value by 153% and leads to a low normalized power consumption among known spin-orbit torque materials. This study demonstrates the critical spin fluctuation as a prospective way to increase the SHA and enriches the AFM material candidates for spin-orbitronic devices.

Interaction Effects in a 1D Flat Band at a Topological Crystalline Step Edge.

Step edges of topological crystalline insulators can be viewed as predecessors of higher-order topology, as they embody one-dimensional edge channels embedded in an effective three-dimensional electronic vacuum emanating from the topological crystalline insulator. Using scanning tunneling microscopy and spectroscopy, we investigate the behavior of such edge channels in Pb1-xSnxSe under doping. Once the energy position of the step edge is brought close to the Fermi level, we observe the opening of a correlation gap. The experimental results are rationalized in terms of interaction effects which are enhanced since the electronic density is collapsed to a one-dimensional channel. This constitutes a unique system to study how topology and many-body electronic effects intertwine, which we model theoretically through a Hartree-Fock analysis.

Zero-field polarity-reversible Josephson supercurrent diodes enabled by a proximity-magnetized Pt barrier.

Simultaneous breaking of inversion and time-reversal symmetries in a conductor yields a non-reciprocal electronic transport1-3, known as the diode or rectification effect, that is, low (ideally zero) conductance in one direction and high (ideally infinite) conductance in the other. So far, most of the diode effects observed in non-centrosymmetric polar/superconducting conductors4-7 and Josephson junctions8-10 require external magnetic fields to break the time-reversal symmetry. Here we report zero-field polarity-switchable Josephson supercurrent diodes, in which a proximity-magnetized Pt layer by ferrimagnetic insulating Y3Fe5O12 serves as the Rashba(-type) Josephson barrier. The zero-field diode efficiency of our proximity-engineered device reaches up to ±35% at 2 K, with a clear square-root dependence on temperature. Measuring in-plane field-strength/angle dependences and comparing with Cu-inserted control junctions, we demonstrate that exchange spin-splitting11-13 and Rashba(-type) spin-orbit coupling13-15 at the Pt/Y3Fe5O12 interface are key for the zero-field giant rectification efficiency. Our achievement advances the development of field-free absolute Josephson diodes.

Magnetic antiskyrmions above room temperature in tetragonal Heusler materials.

Magnetic skyrmions are topologically stable, vortex-like objects surrounded by chiral boundaries that separate a region of reversed magnetization from the surrounding magnetized material. They are closely related to nanoscopic chiral magnetic domain walls, which could be used as memory and logic elements for conventional and neuromorphic computing applications that go beyond Moore's law. Of particular interest is 'racetrack memory', which is composed of vertical magnetic nanowires, each accommodating of the order of 100 domain walls, and that shows promise as a solid state, non-volatile memory with exceptional capacity and performance. Its performance is derived from the very high speeds (up to one kilometre per second) at which chiral domain walls can be moved with nanosecond current pulses in synthetic antiferromagnet racetracks. Because skyrmions are essentially composed of a pair of chiral domain walls closed in on themselves, but are, in principle, more stable to perturbations than the component domain walls themselves, they are attractive for use in spintronic applications, notably racetrack memory. Stabilization of skyrmions has generally been achieved in systems with broken inversion symmetry, in which the asymmetric Dzyaloshinskii-Moriya interaction modifies the uniform magnetic state to a swirling state. Depending on the crystal symmetry, two distinct types of skyrmions have been observed experimentally, namely, Bloch and Néel skyrmions. Here we present the experimental manifestation of another type of skyrmion-the magnetic antiskyrmion-in acentric tetragonal Heusler compounds with D2d crystal symmetry. Antiskyrmions are characterized by boundary walls that have alternating Bloch and Néel type as one traces around the boundary. A spiral magnetic ground-state, which propagates in the tetragonal basal plane, is transformed into an antiskyrmion lattice state under magnetic fields applied along the tetragonal axis over a wide range of temperatures. Direct imaging by Lorentz transmission electron microscopy shows field-stabilized antiskyrmion lattices and isolated antiskyrmions from 100 kelvin to well beyond room temperature, and zero-field metastable antiskyrmions at low temperatures. These results enlarge the family of magnetic skyrmions and pave the way to the engineering of complex bespoke designed skyrmionic structures.

Atomic Scale Control of Spin Current Transmission at Interfaces.

Ferromagnet/heavy metal bilayers represent a central building block for spintronic devices where the magnetization of the ferromagnet can be controlled by spin currents generated in the heavy metal. The efficiency of spin current generation is paramount. Equally important is the efficient transfer of this spin current across the ferromagnet/heavy metal interface. Here, we show theoretically and experimentally that for Ta as heavy metal the interface only partially transmits the spin current while this effect is absent when Pt is used as heavy metal. This is due to magnetic moment reduction at the interface caused by 3d-5d hybridization effects. We show that this effect can be avoided by atomically thin interlayers. On the basis of our theoretical model we conclude that this is a general effect and occurs for all 5d metals with less than half-filled 5d shell.

Long-range supercurrents through a chiral non-collinear antiferromagnet in lateral Josephson junctions.

The proximity-coupling of a chiral non-collinear antiferromagnet (AFM)1-5 with a singlet superconductor allows spin-unpolarized singlet Cooper pairs to be converted into spin-polarized triplet pairs6-8, thereby enabling non-dissipative, long-range spin correlations9-14. The mechanism of this conversion derives from fictitious magnetic fields that are created by a non-zero Berry phase15 in AFMs with non-collinear atomic-scale spin arrangements1-5. Here we report long-ranged lateral Josephson supercurrents through an epitaxial thin film of the triangular chiral AFM Mn3Ge (refs. 3-5). The Josephson supercurrents in this chiral AFM decay by approximately one to two orders of magnitude slower than would be expected for singlet pair correlations9-14 and their response to an external magnetic field reflects a clear spatial quantum interference. Given the long-range supercurrents present in both single- and mixed-phase Mn3Ge, but absent in a collinear AFM IrMn16, our results pave a way for the topological generation of spin-polarized triplet pairs6-8 via Berry phase engineering15 of the chiral AFMs.

Ultrafast manipulation of the NiO antiferromagnetic order via sub-gap optical excitation.

Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s-2p core-valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p-3d resonance (L2-edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 ± 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap.

Competing Energy Scales in Topological Superconducting Heterostructures.

Artificially engineered topological superconductivity has emerged as a viable route to create Majorana modes. In this context, proximity-induced superconductivity in materials with a sizable spin-orbit coupling has been intensively investigated in recent years. Although there is convincing evidence that superconductivity may indeed be induced, it has been difficult to elucidate its topological nature. Here, we engineer an artificial topological superconductor by progressively introducing superconductivity (Nb), strong spin-orbital coupling (Pt), and topological states (Bi2Te3). Through spectroscopic imaging of superconducting vortices within the bare s-wave superconducting Nb and within proximitized Pt and Bi2Te3 layers, we detect the emergence of a zero-bias peak that is directly linked to the presence of topological surface states. Our results are rationalized in terms of competing energy trends which are found to impose an upper limit to the size of the minigap separating Majorana and trivial modes, its size being ultimately linked to fundamental materials properties.

Microscopic Manipulation of Ferroelectric Domains in SnSe Monolayers at Room Temperature.

Two-dimensional (2D) van der Waals ferroelectrics provide an unprecedented architectural freedom for the creation of artificial multiferroics and nonvolatile electronic devices based on vertical and coplanar heterojunctions of 2D ferroic materials. Nevertheless, controlled microscopic manipulation of ferroelectric domains is still rare in monolayer-thick 2D ferroelectrics with in-plane polarization. Here we report the discovery of robust ferroelectricity with a critical temperature close to 400 K in SnSe monolayer plates grown on graphene and the demonstration of controlled room-temperature ferroelectric domain manipulation by applying appropriate bias voltage pulses to the tip of a scanning tunneling microscope (STM). This study shows that STM is a powerful tool for detecting and manipulating the microscopic domain structures in 2D ferroelectric monolayers, which are difficult for conventional approaches such as piezoresponse force microscopy, thus facilitating the hunt for other 2D ferroelectric monolayers with in-plane polarization with important technological applications.

Observation of Magnetic Antiskyrmions in the Low Magnetization Ferrimagnet Mn2Rh0.95Ir0.05Sn.

Recently, magnetic antiskyrmions were discovered in Mn1.4Pt0.9Pd0.1Sn, an inverse tetragonal Heusler compound that is nominally a ferrimagnet, but which can only be formed with substantial Mn vacancies. The vacancies reduce considerably the compensation of the moments between the two expected antiferromagnetically coupled Mn sub-lattices so that the overall magnetization is very high and the compound is almost a "ferromagnet". Here, we report the observation of antiskyrmions in a second inverse tetragonal Heusler compound, Mn2Rh0.95Ir0.05Sn, which can be formed stoichiometrically without any Mn vacancies and which thus exhibits a much smaller magnetization. Individual and lattices of antiskyrmions can be stabilized over a wide range of temperature from near room temperature to 100 K, the base temperature of the Lorentz transmission electron microscope used to image them. In low magnetic fields helical spin textures are found which evolve into antiskyrmion structures in the presence of small magnetic fields. A weaker Dzyaloshinskii-Moriya interaction (DMI), that stabilizes the antiskyrmions, is expected for the 4d element Rh as compared to the 5d element Pt, so that the observation of antiskyrmions in Mn2Rh0.95Ir0.05Sn establishes the intrinsic stability of antiskyrmions in these Heusler compounds. Moreover, the finding of antiskyrmions with substantially lower magnetization promises, via chemical tuning, even zero moment antiskyrmions with important technological import.