2D Electron Gas with 100% Spin‐Polarization in the (LaMnO3)2/(SrTiO3)2 Superlattice under Uniaxial Strain

By first‐principles calculations we investigate the structural, electronic, and magnetic properties of the (LaMnO₃)₂/(SrTiO₃)₂ superlattice. We find that a monoclinic C_2h symmetry is energetically favorable and that the spins order ferromagnetically. Under both compressive and tensile uniaxial strain the electronic structure of the superlattice shows a half‐metallic character. In particular, a fully spin‐polarized two‐dimensional electron gas, which traces back to the Ti 3d_xy orbitals, is achieved under compressive uniaxial strain.     

Evidence of Spin Frustration in a Vanadium Diselenide Monolayer Magnet

Monolayer VSe₂, featuring both charge density wave and magnetism phenomena, represents a unique van der Waals magnet in the family of metallic 2D transition‐metal dichalcogenides (2D‐TMDs). Herein, by means of in situ microscopy and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X‐ray and angle‐resolved photoemission, and X‐ray absorption, direct spectroscopic signatures are established, that identify the metallic 1T‐phase and vanadium 3d¹ electronic configuration in monolayer VSe₂ grown on graphite by molecular‐beam epitaxy. Element‐specific X‐ray magnetic circular dichroism, complemented with magnetic susceptibility measurements, further reveals monolayer VSe₂ as a frustrated magnet, with its spins exhibiting subtle correlations, albeit in the absence of a long‐range magnetic order down to 2 K and up to a 7 T magnetic field. This observation is attributed to the relative stability of the ferromagnetic and antiferromagnetic ground states, arising from its atomic‐scale structural features, such as rotational disorders and edges. The results of this study extend the current understanding of metallic 2D‐TMDs in the search for exotic low‐dimensional quantum phenomena, and stimulate further theoretical and experimental studies on van der Waals monolayer magnets.     

Ultrathin Two‐Dimensional Multinary Layered Metal Chalcogenide Nanomaterials

Ultrathin two‐dimensional (2D) layered transition metal dichalcogenides (TMDs), such as MoS₂, WS₂, TiS₂, TaS₂, ReS₂, MoSe₂ and WSe₂, have attracted considerable attention over the past six years owing to their unique properties and great potential in a wide range of applications. Aiming to achieve tunable properties and optimal application performances, great effort is devoted to the exploration of 2D multinary layered metal chalcogenide nanomaterials, which include ternary metal chalcogenides with well‐defined crystal structures, alloyed TMDs, heteroatom‐doped TMDs and 2D metal chalcogenide heteronanostructures. These novel 2D multinary layered metal chalcogenide nanomaterials exhibit some unique properties compared to 2D binary TMD counterparts, thus holding great promise in various potential applications including electronics/optoelectronics, catalysis, sensors, biomedicine, and energy storage and conversion with enhanced performances. This article focuses on the state‐of‐art progress on the preparation, characterization and applications of ultrathin 2D multinary layered metal chalcogenide nanomaterials.     

Study of the Structural,Electronic, Magnetic,and Optical Properties of Mn<Subscript>2</Subscript>ZrGa Full-Heusler Alloy: First-Principles Calculations

In this work, the structural, electronic, magnetic, and optical properties of Mn₂ZrGa full-Heusler alloy were investigated by using density functional theory (DFT) calculations. It is found that the spin-up states have a metallic character, but the spin-down bands have a pseudo-gap at the Fermi level. The total spin magnetic moment of Mn₂ZrGa (per formula unit) is 3.00 µ _B at an equilibrium lattice parameter of 6.15 Å. The calculations show that Mn₂ZrGa is a ferrimagnetic with 81% spin polarization at equilibrium lattice parameter. The effect of lattice parameter distortion on the magnetic properties and spin polarization is also studied. It is found that the total magnetic moment preserves its value for a lattice parameter range of 5.96–6.30 Å. The decreasing of the lattice parameter leads to improvement of spin polarization. The real and imaginary parts of dielectric function and hence the optical properties including energy absorption spectrum, reflectivity, and optical conductivity are also calculated. The value of plasma frequency for spin-up and down electrons is located at 1.78 and 0.74 eV, respectively.     

Spin–Orbit Torque Switching in a Nearly Compensated Heusler Ferrimagnet

Ferrimagnetic materials combine the advantages of the low magnetic moment of an antiferromagnet and the ease of realizing magnetic reading of a ferromagnet. Recently, it was demonstrated that compensated ferrimagnetic half metals can be realized in Heusler alloys, where high spin polarization, zero magnetic moment, and low magnetic damping can be achieved at the same time. In this work, by studying the spin–orbit torque induced switching in the Heusler alloy Mn₂Ru_{1? x} Ga, it is found that efficient current‐induced magnetic switching can be realized in a nearly compensated sample with strong perpendicular anisotropy and large film thickness. This work demonstrates the possibility of employing compensated Heusler alloys for fast, energy‐efficient spintronic devices.     

Edge‐Epitaxial Growth of 2D NbS2‐WS2 Lateral Metal‐Semiconductor Heterostructures

2D metal‐semiconductor heterostructures based on transition metal dichalcogenides (TMDs) are considered as intriguing building blocks for various fields, such as contact engineering and high‐frequency devices. Although, a series of p–n junctions utilizing semiconducting TMDs have been constructed hitherto, the realization of such a scheme using 2D metallic analogs has not been reported. Here, the synthesis of uniform monolayer metallic NbS₂ on sapphire substrate with domain size reaching to a millimeter scale via a facile chemical vapor deposition (CVD) route is demonstrated. More importantly, the epitaxial growth of NbS₂‐WS₂ lateral metal‐semiconductor heterostructures via a “two‐step” CVD method is realized. Both the lateral and vertical NbS₂‐WS₂ heterostructures are achieved here. Transmission electron microscopy studies reveal a clear chemical modulation with distinct interfaces. Raman and photoluminescence maps confirm the precisely controlled spatial modulation of the as‐grown NbS₂‐WS₂ heterostructures. The existence of the NbS₂‐WS₂ heterostructures is further manifested by electrical transport measurements. This work broadens the horizon of the in situ synthesis of TMD‐based heterostructures and enlightens the possibility of applications based on 2D metal‐semiconductor heterostructures.     

Synthesis of In‐Plane Artificial Lattices of Monolayer Multijunctions

Recently, monolayers of van der Waals materials, including transition metal dichalcogenides (TMDs), are considered ideal building blocks for constructing 2D artificial lattices and heterostructures. Heterostructures with multijunctions of more than two monolayer TMDs are intriguing for exploring new physics and materials properties. Obtaining in‐plane heterojunctions of monolayer TMDs with atomically sharp interfaces is very significant for fundamental research and applications. Currently, multistep synthesis for more than two monolayer TMDs remains a challenge because decomposition or compositional alloying is thermodynamically favored at the high growth temperature. Here, a multistep chemical vapor deposition (CVD) synthesis of the in‐plane multijunctions of monolayer TMDs is presented. A low growth temperature synthesis is developed to avoid compositional fluctuations of as‐grown TMDs, defects formations, and interfacial alloying for high heterointerface quality and thermal stability of monolayer TMDs. With optimized parameters, atomically sharp interfaces are successfully achieved in the synthesis of in‐plane artificial lattices of the WS₂/WSe₂/MoS₂ at reduced growth temperatures. Growth behaviors as well as the heterointerface quality are carefully studied in varying growth parameters. Highly oriented strain patterns are found in the second harmonic generation imaging of the TMD multijunctions, suggesting that the in‐plane heteroepitaxial growth may induce distortion for unique material symmetry.     

Study of the Electronic Structure,Magnetic and Elastic Properties and Half-Metallic Stability on Variation of Lattice Constants for CoFeCr<Emphasis Type="Italic">Z</Emphasis> (<Emphasis Type="Italic">Z</Emphasis> = P,As, Sb) Heusler Alloys

Structural, elastic, magnetic and electronic properties of CoFeCrZ (Z = P, As, Sb) Heusler alloys in their YI-type structure have been computed by density functional theory-based WIEN2k code within generalized gradient approximation for exchange correlation functions. Values of formation energy and elastic constants verify the stability of these alloys. True half metallic ferromagnetic behaviour with 100% spin polarization and good band gap in the minority spin are obtained for all the alloys. Magnetic moment of these alloys is 4.00 μ _B , which matches well with the value predicted from Slater-Pauling rule. Half-metallicity is maintained over a wide range of lattice constants making these alloys promising for spintronics device applications.     

Anisotropic Magneto‐Coulomb Properties of 2D–0D Heterostructure Single Electron Device

Fabrication and spintronics properties of 2D–0D heterostructures are reported. Devices based on graphene (“Gr”)–aluminium nanoclusters heterostructures show robust and reproducible single‐electron transport features, in addition to spin‐dependent functionality when using a top magnetic electrode. The magnetic orientation of this single ferromagnetic electrode enables the modulation of the environmental charge experienced by the aluminium nanoclusters. This anisotropic magneto‐Coulomb effect, originating from spin–orbit coupling within the ferromagnetic electrode, provides tunable spin valve‐like magnetoresistance signatures without the requirement of spin coherent charge tunneling. These results extend the capability of Gr to act both as electrode and as a platform for the growth of 2D–0D mixed‐dimensional van der Waals heterostructures, providing magnetic functionalities in the Coulomb blockade regime on scalable spintronic devices. These heterostructures pave the way towards novel device architectures at the crossroads of 2D material physics and spin electronics.     

Colloidal Single‐Layer Photocatalysts for Methanol‐Storable Solar H2 Fuel

Molecular surfactants are widely used to control low‐dimensional morphologies, including 2D nanomaterials in colloidal chemical synthesis, but it is still highly challenging to accurately control single‐layer growth for 2D materials. A scalable stacking‐hinderable strategy to not only enable exclusive single‐layer growth mode for transition metal dichalcogenides (TMDs) selectively sandwiched by surfactant molecules but also retain sandwiched single‐layer TMDs' photoredox activities is developed. The single‐layer growth mechanism is well explained by theoretical calculation. Three types of single‐layer TMDs, including MoS₂, WS₂, and ReS₂, are successfully synthesized and demonstrated in solar H₂ fuel production from hydrogen‐stored liquid carrier—methanol. Such H₂ fuel production from single‐layer MoS₂ nanosheets is CO_x‐free and reliably workable under room temperature and normal pressure with the generation rate reaching ≈617 µmole g^?1 h^?1 and excellent photoredox endurability. This strategy opens up the feasible avenue to develop methanol‐storable solar H₂ fuel with facile chemical rebonding actualized by 2D single‐layer photocatalysts.     

Composition-Controllable Syntheses and Property Modulations from 2D Ferromagnetic Fe5Se8 to Metallic Fe3Se4 Nanosheets

Exploring new-type 2D magnetic materials with high magnetic transition temperature and robust air stability has attracted wide attention for developing innovative spintronic devices. Recently, intercalation of native metal atoms into the van der Waals gaps of 2D layered transition metal dichalcogenides (TMDs) has been developed to form 2D non-layered magnetic TMDs, while only succeeded in limited systems (e.g., Cr₂S₃, Cr₅Te₈). Herein, composition-controllable syntheses of 2D non-layered iron selenide nanosheets (25% Fe-intercalated triclinic Fe₅Se₈ and 50% Fe-intercalated monoclinic Fe₃Se₄) are firstly reported, via a robust chemical vapor deposition strategy. Specifically, the 2D Fe₅Se₈ exhibits intrinsic room-temperature ferromagnetic property, which is explained by the change of electron spin states from layered 1T'-FeSe₂ to non-layered Fe-intercalated Fe₅Se₈ based on density functional theory calculations. In contrast, the ultrathin Fe₃Se₄ presents novel metallic features comparable with that of metallic TMDs. This work hereby sheds light on the composition-controllable synthesis and fundamental property exploration of 2D self-intercalation induced novel TMDs compounds, by propelling their application explorations in nanoelectronics and spintronics-related fields.     

Emerging 0D Transition‐Metal Dichalcogenides for Sensors,Biomedicine, and Clean Energy

Following research on two‐dimensional (2D) transition metal dichalcogenides (TMDs), zero‐dimensional (0D) TMDs nanostructures have also garnered some attention due to their unique properties; exploitable for new applications. The 0D TMDs nanostructures stand distinct from their larger 2D TMDs cousins in terms of their general structure and properties. 0D TMDs possess higher bandgaps, ultra‐small sizes, high surface‐to‐volume ratios with more active edge sites per unit mass. So far, reported 0D TMDs can be mainly classified as quantum dots, nanodots, nanoparticles, and small nanoflakes. All exhibited diverse applications in various fields due to their unique and excellent properties. Of significance, through exploiting inherent characteristics of 0D TMDs materials, enhanced catalytic, biomedical, and photoluminescence applications can be realized through this exciting sub‐class of TMDs. Herein, we comprehensively review the properties and synthesis methods of 0D TMDs nanostructures and focus on their potential applications in sensor, biomedicine, and energy fields. This article aims to educate potential adopters of these excitingly new nanomaterials as well as to inspire and promote the development of more impactful applications. Especially in this rapidly evolving field, this review may be a good resource of critical insights and in‐depth comparisons between the 0D and 2D TMDs.     

Ultrafast Orbital‐Oriented Control of Magnetization in Half‐Metallic La0.7Sr0.3MnO3 Films

Manipulating spins by ultrafast pulse laser provides a new avenue to switch the magnetization for spintronic applications. While the spin–orbit coupling is known to play a pivotal role in the ultrafast laser‐induced demagnetization, the effect of the anisotropic spin–orbit coupling on the transient magnetization remains an open issue. This study uncovers the role of anisotropic spin–orbit coupling in the spin dynamics in a half‐metallic La_0.7Sr_0.3MnO₃ film by ultrafast pump–probe technique. The magnetic order is found to be transiently enhanced or attenuated within the initial sub‐picosecond when the probe light is tuned to be s‐ or p‐polarized, respectively. The subsequent slow demagnetization amplitude follows the fourfold symmetry of the ${\mathrm{d}}_{x^2?y^2}$ orbitals as a function of the polarization angles of the probe light. A model based on the Elliott–Yafet spin‐flip scatterings is proposed to reveal that the transient magnetization enhancement is related to the spin‐mixed states arising from the anisotropic spin–orbit coupling. The findings provide new insights into the spin dynamics in magnetic systems with anisotropic spin–orbit coupling as well as perspectives for the ultrafast control of information process in spintronic devices.     

Recent Developments in Controlled Vapor‐Phase Growth of 2D Group 6 Transition Metal Dichalcogenides

An overview of recent developments in controlled vapor‐phase growth of 2D transition metal dichalcogenide (2D TMD) films is presented. Investigations of thin‐film formation mechanisms and strategies for realizing 2D TMD films with less‐defective large domains are of central importance because single‐crystal‐like 2D TMDs exhibit the most beneficial electronic and optoelectronic properties. The focus is on the role of the various growth parameters, including strategies for efficiently delivering the precursors, the selection and preparation of the substrate surface as a growth assistant, and the introduction of growth promoters (e.g., organic molecules and alkali metal halides) to facilitate the layered growth of (Mo, W)(S, Se, Te)₂ atomic crystals on inert substrates. Critical factors governing the thermodynamic and kinetic factors related to chemical reaction pathways and the growth mechanism are reviewed. With modification of classical nucleation theory, strategies for designing and growing various vertical/lateral TMD‐based heterostructures are discussed. Then, several pioneering techniques for facile observation of structural defects in TMDs, which substantially degrade the properties of macroscale TMDs, are introduced. Technical challenges to be overcome and future research directions in the vapor‐phase growth of 2D TMDs for heterojunction devices are discussed in light of recent advances in the field.     

Site dependent metal adsorption on (3 × 3) h-BN monolayer: Stability, magnetic and optical properties

Cu, Pd and Au metal adatom adsorption on different adsorption sites of graphene analog h-BN monolayer is presented. The results demonstrate that the atop N (A_N) being the most favorable site for Cu while atop B (A_B) for Pd/Au; as well as occurrence of chemisorption is also found in these sites. A general model has been proposed which essentially indicate electronegativity (χ) to be the governing reason regarding the choice of adsorption sites on h-BN sheet in a way such that the adatoms with χ < 2.04 are the most stable on A_N site while adatoms with χ lying in the range 2.04-3.04 are the most stable on A_B site. A detail study regarding magnetic properties reveal 100% spin polarization at Fermi level i.e. half metallic characteristics and 1μ_B/supercell magnetic moment in case of Cu and Au adatom adsorption at the most favorable sites. For Cu adsorbed h-BN system, the half metallic characteristics and strong chemical bonds arise from good hybridization at 0 eV between the outermost 2p orbital of nitrogen and the outermost 4s orbital of copper and at −1.49 eV between Cu 3d and 4s orbital with N 2p orbital. A thorough optical study on the above mentioned systems exhibits evolution/disappearance of different hump/shoulder peaks in the calculated absorption coefficient vs. energy plot which may be useful for experimental identification of the adsorbed systems.     

Nanomechanical and Charge Transport Properties of Two‐Dimensional Atomic Sheets

The materials properties of graphene and other two‐dimensional atomic sheets are influenced by atomic‐scale defects, mechanical deformation, and microstructures. Thus, for graphene‐based applications, it is essential to uncover the roles of atomic‐scale defects and domain structures of two‐dimensional layers in charge transport properties. This review highlights recent studies of nanomechanical and charge transport properties of two‐dimensional atomic sheets, including graphene, MoS₂, and boron nitrides. Because of intrinsic structural differences, two‐dimensional atomic sheets give rise to unique nanomechanical properties, including a dependence on layer thickness and chemical modification that is in contrast to three‐dimensional continuum media. Mapping of local conductance and nanomechanical properties on a graphene layer can be used to image the domain and microstructures of two‐dimensional atomic layers. This paper also reviews recent experimental and theoretical findings on the role of bending, defects, and microstructures on nanomechanical and transport properties of graphene‐derived materials.     

Spin Valve Effect of 2D‐Materials Based Magnetic Junctions

The magnetotransport properties of spin valve structure are highly influenced by the type of intervening layer inserted between the ferromagnetic electrodes. In this scenario, spin filtering effect at the interfaces plays a crucial role in determining the magnetoresistance (MR) of such magnetic structures, which can be enhanced by using a suitable intervening layer. Here, the authors investigate the spin filtering effect of the two‐dimensional layers such as hexagonal boron nitride (hBN), graphene (Gr), and Gr‐hBN hybrid system for modifying the magnetotransport characteristics of the vertical spin valve architectures (Ni/hBN/Ni, Ni/Gr/Ni, and Ni/Gr‐hBN/Ni). Compared to graphene, hBN incorporated magnetic junction reveals higher MR and spin polarizations (P) suggesting better spin filtering at the interfaces. The MR for hBN incorporated junction is calculated to be ≈0.83%, while that of graphene junction it is estimated to be ≈0.16%. Similar contrast is observed in the ‘P’ of ferromagnets (FMs) for the two junctions, that is, ≈6.4% for hBN based magnetic junction and ≈2.8% for graphene device. However, for Gr‐hBN device, the signal not only get inverts, but it also suggests efficient spin filtering mechanism at the FM interfaces. Their results can be useful to comprehend the origin of spin filtering and the choice of non‐magnetic spacer for magnetotransport characteristics.

     

Controllable,Wide‐Ranging n‐Doping and p‐Doping of Monolayer Group 6 Transition‐Metal Disulfides and Diselenides

Developing processes to controllably dope transition‐metal dichalcogenides (TMDs) is critical for optical and electrical applications. Here, molecular reductants and oxidants are introduced onto monolayer TMDs, specifically MoS₂, WS₂, MoSe₂, and WSe₂. Doping is achieved by exposing the TMD surface to solutions of pentamethylrhodocene dimer as the reductant (n‐dopant) and “Magic Blue,” [N(C₆H₄‐p‐Br)₃]SbCl₆, as the oxidant (p‐dopant). Current–voltage characteristics of field‐effect transistors show that, regardless of their initial transport behavior, all four TMDs can be used in either p‐ or n‐channel devices when appropriately doped. The extent of doping can be controlled by varying the concentration of dopant solutions and treatment time, and, in some cases, both nondegenerate and degenerate regimes are accessible. For all four TMD materials, the photoluminescence intensity; for all four materials the PL intensity is enhanced with p‐doping but reduced with n‐doping. Raman and X‐ray photoelectron spectroscopy (XPS) also provide insight into the underlying physical mechanism by which the molecular dopants react with the monolayer. Estimates of changes of carrier density from electrical, PL, and XPS results are compared. Overall a simple and effective route to tailor the electrical and optical properties of TMDs is demonstrated.     

High‐Performance Three‐Dimensional Li Anode Scaffold Enabled by Homogeneous Zn Nanoclusters

The large‐scale implementation of lithium metal batteries (LMBs) has long been plagued by the uncontrollable Li deposition triggered safety issues. Herein, a lithiophilic three‐dimensional Li anode scaffold, which is prepared by molten Li infusion aided by confined growth of low‐cost Zn clusters, is rationally constructed for high‐performance LMBs. Owing to the synergy of the carbon host and the effective regulation from the Zn nanoclusters, the large volumetric change of Li metal is well mitigated and shows a smooth and dendrite‐free behavior. The Li anode scaffold can deliver much improved Coulombic efficiency, superior rate performance, and long cycle lifespan with much lower voltage polarization. Furthermore, the half cells of Li anode scaffold paired with LiFePO₄/LiCoO₂/sulfur can achieve a higher specific capacity and longer stable cycling life than those with conventional Li foil. The Li|LFP cells can achieve a stable cycling over 250 cycles at 1C with a higher capacity retention of ≈90.8%, and a higher initial discharge capacity of 924.6 mAh g^?1 with a high capacity retention over 300 cycles can also be obtained in Li|S cells at 1C. This work demonstrates a cost‐effective and scalable strategy for stable Li metal anode toward next‐generation and high‐performance LMBs.     

Half-Metallic Magnetism of Quaternary Heusler Compounds Co2Fe x Mn1−x Si(x =0,0.5, and 1.0): First-Principles Calculations

Using first-principles calculations, the structural, electronic, and magnetic properties of ferromagnetic half-metallic full-Heusler Co₂FeSi, Co₂MnSi and Co₂ Fe _0.5Mn _0.5Si alloy via the full-potential linearized augmented plane-wave (FP-LAPW) method in the generalized gradient (GGA) and GGA + U approximations are compared with other experimental and theoretical results. The electronic band structures and density of states (DOS) of the compounds indicate they are half metallic because of the existence of the energy gap in the minority spin (DOS and band structure), which yields perfect spin polarization. The half metallicity of the obtained material may prove useful for applications in spin-polarizers and spin-injectors of magnetic nanodevices. The calculated total spin magnetic moments are almost exactly that expected from the Slater-Pauling rule.