Atomic-Limit Mott Insulator in [4]Triangulene Frameworks.

Triangulene, one unique class of zigzag-edged triangular graphene molecules, has attracted tremendous research interest. In this work, as an ultimate phase of the Mott insulator, we present the realization of the atomic-limit Mott insulator in experimentally synthesized [4]triangulene frameworks ([4]-TGFs) from first-principles calculations. The frontier molecular orbitals of the nonmagnetic [4]triangulene consist of three coupled corner modes. After the isolated [4]triangulene is assembled into [4]-TGF, one special enantiomorphic flat band is created through the coupling of these corner modes, which is identified to be a second-order topological insulator with half-filled topological corner states at the Fermi level. Moreover, [4]-TGF prefers an antiferromagnetic ground state under Hubbard interactions, which further splits these metallic zero-energy states into an atomic-limit Mott insulator with spin-polarized corners. Since the fractional filling of topological corner states is a smoking-gun signature of higher-order topology, our results demonstrate a universal approach to explore the atomic-limit Mott insulators in higher-order topological materials.

Magnetochiral tunneling in paramagnetic Co1/3NbS2.

Electric currents have the intriguing ability to induce magnetization in nonmagnetic crystals with sufficiently low crystallographic symmetry. Some associated phenomena include the non-linear anomalous Hall effect in polar crystals and the nonreciprocal directional dichroism in chiral crystals when magnetic fields are applied. In this work, we demonstrate that the same underlying physics is also manifested in the electronic tunneling process between the surface of a nonmagnetic chiral material and a magnetized scanning probe. In the paramagnetic but chiral metallic compound Co1/3NbS2, the magnetization induced by the tunneling current is shown to become detectable by its coupling to the magnetization of the tip itself. This results in a contrast across different chiral domains, achieving atomic-scale spatial resolution of structural chirality. To support the proposed mechanism, we used first-principles theory to compute the chirality-dependent current-induced magnetization and Berry curvature in the bulk of the material. Our demonstration of this magnetochiral tunneling effect opens up an avenue for investigating atomic-scale variations in the local crystallographic symmetry and electronic structure across the structural domain boundaries of low-symmetry nonmagnetic crystals.

Enhanced Spin-Polarized Electric Field Modulating p-Band Center on Ni-Doped CdS for Boosting Photocatalytic Hydrogen Evolution.

It is a challenge to regulate charge separation dynamics and redox reaction kinetics at the atomic level to synergistically boost photocatalytic hydrogen (H2) evolution. Herein, a robust Ni-doped CdS (Ni-CdS) photocatalyst is synthesized by incorporating highly dispersed Ni atoms into the CdS lattice in substitution for Cd atoms. Combined characterizations with theoretical analysis indicate that local lattice distortion and S-vacancy of Ni-CdS induced by Ni incorporation lead to an increased dipole moment and enhanced spin-polarized electric field, which promotes the separation and transfer of photoinduced carriers. In this contribution, charge redistribution caused by enhanced internal electric field results in the downshift of the S p-band center, which is conducive to the desorption of intermediate H* for boosting the H2 evolution reaction. Accordingly, the Ni-CdS photocatalyst shows a remarkably improved photocatalytic performance with an H2 evolution rate of 20.28 mmol g-1 h-1 under visible-light irradiation, which is 5.58 times higher than that of pristine CdS. This work supplied an insightful understanding that the enhanced polarization electric field governs the p-band center for efficient photocatalytic H2 evolution activity.

Magnetocapacitance at the Ni/BiInO3 Schottky Interface.

We report the observation of a magnetocapacitance effect at the interface between Ni and epitaxial nonpolar BiInO3 thin films at room temperature. A detailed surface study using X-ray photoelectron spectroscopy (XPS) reveals the formation of an intermetallic Ni-Bi alloy at the Ni/BiInO3 interface and a shift in the Bi 4f and In 3d core levels to higher binding energies with increasing Ni thickness. The latter infers band bending in BiInO3, corresponding to the formation of a p-type Schottky barrier. The current-voltage characteristics of the Ni/BiInO3/(Ba,Sr)RuO3/NdScO3(110) heterostructure show a significant dependence on the applied magnetic field and voltage cycling, which can be attributed to voltage-controlled band bending and spin-polarized charge accumulation in the vicinity of the Ni/BiInO3 interface. The magnetocapacitance effect can be realized at room temperature without involving multiferroic materials.

Spin-Polarized Surface Capacitance Effects Enable Fe3 O4 Anode Superior Wide Operation-Temperature Sodium Storage.

Fe3 O4 is widely investigated as an anode for ambient sodium-ion batteries (SIBs), but its electrochemical properties in the wide operation-temperature range have rarely been studied. Herein, the Fe3 O4 nanoparticles, which are well encapsulated by carbon nanolayers, are uniformly dispersed on the graphene basal plane (named Fe3 O4 /C@G) to be used as the anode for SIBs. The existence of graphene can reduce the size of Fe3 O4 /C nanoparticles from 150 to 80 nm and greatly boost charge transport capability of electrode, resulting in an obvious size decrease of superparamagnetic Fe nanoparticles generated from the conversion reaction from 5 to 2 nm. Importantly, the ultra-small superparamagnetic Fe nanoparticles (≈2 nm) can induce a strong spin-polarized surface capacitance effect at operating temperatures ranging from -40 to 60 °C, thus achieving highly efficient Na-ion transport and storage in a wide operation-temperature range. Consequently, the Fe3 O4 /C@G anode shows high capacity, excellent fast-charging capability, and cycling stability ranging from -40 to 60 °C in half/full cells. This work demonstrates the viability of Fe3 O4 as anode for wide operation-temperature SIBs and reveals that spin-polarized surface capacitance effects can promote Na-ion storage over a wide operation temperature range.

2H-2M Phase Control of WSe2 Nanosheets by Se Enrichment Toward Enhanced Electrocatalytic Hydrogen Evolution Reaction.

The phase control of transition metal dichalcogenides (TMDs) is an intriguing approach for tuning the electronic structure toward extensive applications. In this study, WSe2 nanosheets synthesized via a colloidal reaction exhibit a phase conversion from semiconducting 2H to metallic 2M under Se-rich growth conditions (i.e., increasing the concentration of Se precursor or lowering the growth temperature). High-resolution scanning transmission electron microscopy images are used to identify the stacking sequence of the 2M phase, which is distinctive from that of the 1T' phase. First-principles calculations employing various Se-rich models (intercalation and substitution) indicated that Se enrichment induces conversion to the 2M phase. The 2M phase WSe2 nanosheets with the Se excess exhibited enhanced electrocatalytic performance in the hydrogen evolution reaction (HER). In situ X-ray absorption fine structure studies suggested that the excess Se atoms in the 2M phase WSe2 enhanced the HER catalytic activity, which is supported by the Gibbs free energy (ΔGH* ) of H adsorption and the Fermi abundance function. These results provide an appealing strategy for phase control of TMD catalysts.

Manipulation of Electron Spins with Oxygen Vacancy on Amorphous/Crystalline Composite-Type Catalyst.

By substituting the oxygen evolution reaction (OER) with the anodic urea oxidation reaction (UOR), it not only reduces energy consumption for green hydrogen generation but also allows purification of urea-rich wastewater. Spin engineering of the d orbital and oxygen-containing adsorbates has been recognized as an effective pathway for enhancing the performance of electrocatalysts. In this work, we report the fabrication of a bifunctional electrocatalyst composed of amorphous RuO2-coated NiO ultrathin nanosheets (a-RuO2/NiO) with abundant amorphous/crystalline interfaces for hydrogen evolution reaction (HER) and UOR. Impressively, only 1.372 V of voltage is required to attain a current density of 10 mA cm-2 over a urea electrolyzer. The increased oxygen vacancies in a-RuO2/NiO by incorporation of amorphous RuO2 enhance the total magnetization and entail numerous spin-polarized electrons during the reaction, which speeds up the UOR reaction kinetics. The density functional theory study reveals that the amorphous/crystalline interfaces promote charge-carrier transfer, and the tailored d-band center endows the optimized adsorption of oxygen-generated intermediates. This kind of oxygen vacancy induced spin-polarized electrons toward boosting HER and UOR kinetics and provides a reliable reference for exploration of advanced electrocatalysts.

Probing Spin-Dependent Ballistic Charge Transport at Single-Nanometer Length Scales.

The coherent transport of charge and spin is a key requirement of future devices for quantum computing and communication. Scattering at defects or impurities may significantly reduce the coherence of quantum-mechanical states, thereby affecting the device functionality. While numerous methods exist to experimentally assess charge transport, the real-space detection of a material's ballistic spin transport properties with nanometer resolution remains a challenge. Here we report on a novel approach that utilizes a combination of spin-polarized scanning tunneling microscopy (SP-STM) and the recently introduced molecular nanoprobe (MONA) technique. It relies on the local injection of spin-polarized charge carriers from a magnetic STM tip and their detection by a single surface-deposited phthalocyanine molecule via reversible electron-induced tautomerization events. Based on the particular electronic structure of the Rashba alloy BiAg2, which is governed by a spin-momentum-locked surface state, we prove that the current direction inverses upon tip magnetization reversal.

Monte Carlo Computer Simulations of Spin-Transfer Torque.

This article performs computer simulations of the change in magnetization in the ferromagnetic film when polarized electric current passes through it. The model examines multilayer structures from ferromagnetic and nonmagnetic films. A sandwich system comprises two ferromagnetic layers separated by a nonmagnetic gasket. Ferromagnetic films have different magnetic susceptibility. The first ferromagnetic film is magnetically hard and acts as a fixed layer. The second ferromagnetic film is magnetically soft, with a switched direction of magnetization. The current direction is perpendicular to the film plane (CPP geometry). Spin transfer is carried out by electrons that polarize in the first ferromagnetic film and transmit spin to the second ferromagnetic film. We use the Ising model to describe the magnetic properties of the system and the Metropolis algorithm to form the thermodynamic states of the spin system. Simulations are performed at temperatures below the Curie points for both materials. The result of computer simulation is the dependence of magnetization in the magnetically soft film on the current strength in the system. Calculations show that there is a critical value of the current at which the magnetization sign of the controlled film changes. The magnetization versus current plot is stepwise. The change in the magnetization sign is due to an increase in the polarization of the electron gas. The plot of electron gas polarization versus current is also stepwise.

High-mobility spin-polarized two-dimensional electron gas at the interface of EuTiO3/SrTiO3heterostructures.

Spin polarization of two-dimensional electron gas (2DEG) at the interface of EuTiO3/SrTiO3(STO) heterostructures has been theoretical predicted and experimentally observed via x-ray magnetic circular dichroism and polarized x-ray absorption spectroscopy, which, however, is lack of magnetotransport evidence. Here, we report the fabrication of high-quality EuTiO3/STO heterostructures by depositing antiferromagnetic insulating EuTiO3thin films onto STO substrates. Shubnikov-de Haas oscillation, Hall, and magnetoresistance (MR) measurements show that the interface is not only highly conducting, with electron mobility up to5.5×103cm2V-1s-1at 1.8 K, but also shows low-field hysteretic MR effects. MR of ∼9% is observed at 1.8 K and 20 Oe, which is one order of magnitude higher than those observed in other spin-polarized 2DEG oxide systems. Moreover, the heterostructures show ferromagnetic hysteresis loops. These results demonstrate that the high-mobility 2DEG is spin polarized, whose origin is attributed to the interfacial Ti3+-3dstates due to oxygen deficiency and the exchange interactions between interfacial Eu spins and itinerant Ti-3delectrons.

Exciton Chirality Transfer Empowers Self-Triggered Spin-Polarized Amplified Spontaneous Emission from 1D-Anchoring-3D Perovskites.

Spin-polarized lasers, arising from stimulated emission of imbalanced spin populations, play a vital role in spin-optoelectronics. It is usually tackled by external spin injection, inevitably suffering from additional losses across the barriers from injection sources to gain materials. Herein, spin-polarized coherent light emission is self-triggered from the 1D-anchoring-3D perovskites, where the imbalanced populations in achiral 3D perovskites are endowed with the spin selectivity of exciton chirality (EC) underpinned by chiral 1D perovskites. Efficient transfer of EC is enabled by rapid energy transfer, thereby creating an imbalance of the spin population of excited states. Stimulated emission of such populations brings self-triggered spin-polarized amplified spontaneous emission in the composite perovskites, yielding a higher degree of polarization (DOP) than that based on optical spin injection into bare achiral 3D perovskites. Chemical diversity of composite perovskites not only enables to adjust band gap for broadband output of spin-polarized light signals but also promises to manipulate radiative decay and spin relaxation toward remarkably increased DOP. These results highlight the importance of EC transfer mechanism for spin-polarized lasing and represent a crucial step toward the development of chiral-spintronics.

Transport Property of Wrinkled Graphene Nanoribbon Tuned by Spin-Polarized Gate Made of Vanadium-Benzene Nanowire.

A series of four-terminal V7(Bz)8-WGNR devices were established with wrinkled graphene nanoribbon (WGNR) and vanadium-benzene nanowire (V7(Bz)8). The spin-polarized V7(Bz)8 as the gate channel was placed crossing the plane, the concave (endo-positioned) and the convex (endo-positioned) surface of WGNR with different curvatures via Van der Waals interaction. The density functional theory (DFT) and nonequilibrium Green's function (NEGF) methods were adopted to calculate the transport properties of these devices at various bias voltages (VS) and gate voltages (VG), such as the conductance, spin-polarized currents, transmission spectra (TS), local density of states (LDOS), and scattering states. The results indicate that the position of V7(Bz)8 and the bending curvature of WGNR play important roles in tuning the transport properties of these four-terminal devices. A spin-polarized transport property is induced for these four-terminal devices by the spin-polarized nature of V7(Bz)8. Particularly, the down-spin channel disturbs strongly on the source-to-drain conductance of WGNR when V7(Bz)8 is endo-positioned crossing the WGNR. Our findings on the novel property of four-terminal V7(Bz)8-WGNR devices provide useful guidelines for achieving flexible graphene-based electronic nanodevices by attaching other similar multidecker metal-arene nanowires.

Ferromagnetism in Defected TMD (MoX2, X = S, Se) Monolayer and Its Sustainability under O2, O3, and H2O Gas Exposure: DFT Study.

Spin-polarized density-functional theory (DFT) has been employed to study the effects of atmospheric gases on the electronic and magnetic properties of a defective transition-metal dichalcogenide (TMD) monolayer, MoX2 with X = S or Se. This study focuses on three single vacancies: (i) molybdenum "VMo"; (ii) chalcogenide "VX"; and (iii) di-chalcogenide "VX2". Five different samples of sizes ranging from 4 × 4 to 8 × 8 primitive cells (PCs) were considered in order to assess the effect of vacancy-vacancy interaction. The results showed that all defected samples were paramagnetic semiconductors, except in the case of VMo in MoSe2, which yielded a magnetic moment of 3.99 µB that was independent of the sample size. Moreover, the samples of MoSe2 with VMo and sizes of 4 × 4 and 5 × 5 PCs exhibited half-metallicity, where the spin-up state becomes conductive and is predominantly composed of dxy and dz2 orbital mixing attributed to Mo atoms located in the neighborhood of VMo. The requirement for the establishment of half-metallicity is confirmed to be the provision of ferromagnetic-coupling (FMC) interactions between localized magnetic moments (such as VMo). The critical distance for the existence of FMC is estimated to be dc≅ 16 Å, which allows small sample sizes in MoSe2 to exhibit half-metallicity while the FMC represents the ground state. The adsorption of atmospheric gases (H2O, O2, O3) can drastically change the electronic and magnetic properties, for instance, it can demolish the half-metallicity characteristics. Hence, the maintenance of half-metallicity requires keeping the samples isolated from the atmosphere. We benchmarked our theoretical results with the available data in the literature throughout our study. The conditions that govern the appearance/disappearance of half-metallicity are of great relevance for spintronic device applications.

Direct Probing of a Large Spin-Orbit Coupling in the FeSe Superconducting Monolayer on STO.

Spin-orbit coupling (SOC) is a fundamental physical interaction, which describes how the electrons' spin couples to their orbital motion. It is the source of a vast variety of fascinating phenomena in nanostructures. Although in most theoretical descriptions of high-temperature superconductivity SOC has been neglected, including this interaction can, in principle, revise the microscopic picture. Here by preforming energy-, momentum-, and spin-resolved spectroscopy experiments we demonstrate that while probing the dynamic charge response of the FeSe monolayer on strontium titanate, a prototype two-dimensional high-temperature superconductor using electrons, the scattering cross-section is spin dependent. We unravel the origin of the observed phenomenon and show that SOC in this two-dimensional superconductor is strong. We anticipate that such a strong SOC can have several consequences on the electronic structures and may compete with other pairing scenarios and be crucial for the mechanism of superconductivity.

Enhancement of the Josephson Current in a Quantum Dot Connected to Majorana Nanowires.

We investigate the behavior of the Josephson current in a system composed of a quantum dot (QD) sandwiched between two nanowires by using the nonequilibrium Green's function technique. We consider that the nanowires are in proximity to s-wave superconducror substrates, and Majorana bound states (MBSs) are induced at their ends. It is also assumed that the two nanowires are not aligned in the same orientation, but form a bent angle with respect to each other. It is found that when only one spin state on the QD is coupled to the left nanowire, the Josephson current is the typical sinusoidal function of the phase difference between the two nanowires. If both spin states hybridize to the MBSs with equal coupling strengths, the Josephson current then is not a sinusoidal function of the phase difference. In particular, when the bent angle between the two nanowires is π/2 and the two modes of the MBSs in each nanowire are decoupled from each other, the Josephson current is enhanced by about twenty times in magnitude as compared to the former case. Moreover, the simultaneously enhanced currents of the two spin directions are of the same magnitude but flow in opposite directions and they induce a large pure spin current. Our results also show that this abnormally enhanced Josephson current will be suppressed by a vertical magnetic field applied to the QD.

Inducing Single Spin-Polarized Flat Bands in Monolayer Graphene.

Due to the fundamental and technological implications in driving the appearance of non-trivial, exotic topological spin textures and emerging symmetry-broken phases, flat electronic bands in 2D materials, including graphene, are nowadays a relevant topic in the field of spintronics. Here, via europium doping, single spin-polarized bands are generated in monolayer graphene supported by the Co(0001) surface. The doping is controlled by Eu positioning, allowing for the formation of a K ¯ $\bar{\mathrm{K}}$ -valley localized single spin-polarized low-dispersive parabolic band close to the Fermi energy when Eu is on top, and of a π* flat band with single spin character when Eu is intercalated underneath graphene. In the latter case, Eu also induces a bandgap opening at the Dirac point while the Eu 4f states act as a spin filter, splitting the π band into two spin-polarized branches. The generation of flat bands with single spin character, as revealed by the spin- and angle-resolved photoemission spectroscopy (ARPES) experiments, complemented by density functional theory (DFT) calculations, opens up new pathways toward the realization of spintronic devices exploiting such novel exotic electronic and magnetic states.

Single-Atomic-Layer Stanene on Ferromagnetic Co Nanoislands with Topological Band Structures.

Introducing magnetism to two-dimensional topological insulators is a central issue in the pursuit of magnetic topological materials in low dimensionality. By means of low-temperature growth at 80 K, we succeeded in fabricating a monolayer stanene on Co/Cu(111) and resolving ferromagnetic spin contrast by field-dependent spin-polarized scanning tunneling microscopy (SP-STM). Increases of both remanence to saturation magnetization ratio (Mr/Ms) and coercive field (Hc) due to an enhanced perpendicular magnetic anisotropy (PMA) are further identified by out-of-plane magneto-optical Kerr effect (MOKE). In addition to ultraflat stanene fully relaxed on bilayer Co/Cu(111) from density functional theory (DFT), characteristic topological properties including an in-plane s-p band inversion and a spin-orbit coupling (SOC) induced gap about 0.25 eV at the Γ̅ point have also been verified in the Sn-projected band structure. Interfacial coupling of single-atomic-layer stanene with ferromagnetic Co biatomic layers allows topological band features to coexist with ferromagnetism, facilitating a conceptual design of atomically thin magnetic topological heterostructures.

Two-dimensional half-metallicity and fully spin-polarized topological fermions in monolayer EuOBr.

Two-dimensional (2D) half-metal and topological states have been the current research focus in condensed matter physics. Herein, we report a novel 2D material named EuOBr monolayer, which can simultaneously show 2D half-metal and topological fermions. This material shows a metallic state in the spin-up channel but a large insulating gap of 4.38 eV in the spin-down channel. In the conducting spin channel, the EuOBr monolayer shows the coexistence of Weyl points and nodal-lines near the Fermi level. These nodal-lines are classified by type-I, hybrid, closed, and open nodal-lines. The symmetry analysis suggests these nodal-lines are protected by the mirror symmetry, which cannot be broken even spin-orbit coupling is included because the ground magnetization direction in the material is out-of-plane [001]. The topological fermions in the EuOBr monolayer are fully spin-polarized, which can be meaningful for future applications in topological spintronic nano-devices.

Single-Layered MoS2 Fabricated by Charge-Driven Interlayer Expansion for Superior Lithium/Sodium/Potassium-Ion-Battery Anodes.

Single-layered MoS2 is a promising anode material for lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), and potassium-ion batteries (PIBs) due to its high capacity and isotropic ion transport paths. However, the low intrinsic conductivity and easy-agglomerated feature hamper its applications. Here, a charge-driven interlayer expansion strategy that Co2+ replaces Mo4+ in the doping form to endow MoS2 layers with negative charges, thus inducing electrostatic repulsion, together with the insertion of gaseous groups, to drive interlayer expansion which once breaks the confinement of interlayer van der Waals force, single-layered MoS2 is obtained and uniformly dispersed into carbon matrix arising from the transformation of carbonaceous gaseous groups under high vapor pressure, is proposed. Co atom doping helps enhance the intrinsic conductivity of single-layered MoS2 . Carbon matrix effectively prevents agglomeration of single-layered MoS2 . The doped Co atoms can be fully transformed into ultrasmall Co nanoparticles during conversion reaction, which enables strong spin-polarized surface capacitance and thus significantly boosts ion transport and storage. Consequently, the prepared material delivers superb Li/Na/K-ion storage performances, which are best in the reported MoS2 -based anodes. The proposed charge-driven interlayer expansion strategy provides a novel perspective for preparing single-layered MoS2, which shows huge potential for energy storage.

The spin polarization of palladium on magneto-electric Cr2O3.

While induced spin polarization of a palladium (Pd) overlayer on antiferromagnetic and magneto-electric Cr2O3(0001) is possible because of the boundary polarization at the Cr2O3(0001), in the single domain state, the Pd thin film appears to be ferromagnetic on its own, likely as a result of strain. In the conduction band, we find the experimental evidence of ferromagnetic spin polarized in Pd thin films on a Cr2O3(0001) single crystal, especially in the thin limit, Pd thickness of around 1-4 nm. Indeed there is significant spin polarization in 10 Å thick Pd films on Cr2O3(0001) at 310 K, i.e. above the Néel temperature of bulk Cr2O3. While Cr2O3(0001) has surface moments that tend to align along the surface normal, for Pd on Cr2O3, the spin polarization contains an in-plane component. Strain in the Pd adlayer on Cr2O3(0001) appears correlated to the spin polarization measured in spin polarized inverse photoemission spectroscopy. Further evidence for magnetization of Pd on Cr2O3is provided by measurement of the exchange bias fields in Cr2O3/Pd(buffer)/[Co/Pd]nexchange bias systems. The magnitude of the exchange bias field is, over a wide temperature range, virtually unaffected by the Pd thickness variation between 1 and 2 nm.