Epitaxial Growth of Ternary Topological Insulator Bi2Te2Se 2D Crystals on Mica

Nanostructures of ternary topological insulator (TI) Bi₂Te₂Se are, in principle, advantageous to the manifestation of topologically nontrivial surface states, due to significantly enhanced surface‐to‐volume ratio compared with its bulk crystals counterparts. Herein, the synthesis of 2D Bi₂Te₂Se crystals on mica via the van der Waals epitaxy method is explored and systematically the growth behaviors during the synthesis process are investigated. Accordingly, 2D Bi₂Te₂Se crystals with domain size up to 50 µm large and thickness down to 2 nm are obtained. A pronounced weak antilocalization effect is clearly observed in the 2D Bi₂Te₂Se crystals at 2 K. The method for epitaxial growth of 2D ternary Bi₂Te₂Se crystals may inspire materials engineering toward enhanced manifestation of the subtle surface states of TIs and thereby facilitate their potential applications in next‐generation spintronics.     

Efficient Spin-Orbit Torque Switching of the Semiconducting Van Der Waals Ferromagnet Cr2Ge2Te6

Being able to electrically manipulate the magnetic properties in recently discovered van der Waals ferromagnets is essential for their integration in future spintronics devices. Here, the magnetization of a semiconducting 2D ferromagnet, i.e., Cr₂Ge₂Te₆, is studied using the anomalous Hall effect in Cr₂Ge₂Te₆/tantalum heterostructures. The thinner the flakes, hysteresis and remanence in the magnetization loop with out-of-plane magnetic fields become more prominent. In order to manipulate the magnetization in such thin flakes, a combination of an in-plane magnetic field and a charge current flowing through Ta—a heavy metal exhibiting giant spin Hall effect—is used. In the presence of in-plane fields of 20 mT, charge current densities as low as 5 × 10⁵ A cm^–2 are sufficient to switch the out-of-plane magnetization of Cr₂Ge₂Te₆. This finding highlights that current densities required for spin-orbit torque switching of Cr₂Ge₂Te₆ are about two orders of magnitude lower than those required for switching nonlayered metallic ferromagnets such as CoFeB. The results presented here show the potential of 2D ferromagnets for low-power memory and logic applications.     

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.     

Spontaneous (Anti)meron Chains in the Domain Walls of van der Waals Ferromagnetic Fe5−xGeTe2

The promise of topologically vortex-like magnetic spin textures hinges on the intriguing physical properties and theories in fundamental research and their distinguished roles as high-efficiency information units in future spintronics. The exploration of such magnetic states with unique spin configurations has never ceased. In this study, the emergence of unconventional (anti)meron chains from a domain wall pair is directly observed at zero field in 2D ferromagnetic Fe_5−xGeTe₂, closely correlated with significant enhancement of the in-plane magnetization and weak van der Waals interactions. The simultaneous appearance of a large topological Hall effect is observed at the same temperature range as that of the abnormal magnetic transition. Moreover, the distinctive features of the (anti)meron chains and their collective dynamic behavior under external fields may provide concrete experimental evidence for the recent theoretical prediction of the magnetic-domain-wall topology and endorse a broader range of possibilities for electronics, spintronics, condensed matter physics, etc.     

Emergence of a Non-Van der Waals Magnetic Phase in a Van der Waals Ferromagnet

Manipulation of long-range order in 2D van der Waals (vdW) magnetic materials (e.g., CrI₃, CrSiTe₃ ,etc.), exfoliated in few-atomic layer, can be achieved via application of electric field, mechanical-constraint, interface engineering, or even by chemical substitution/doping. Usually, active surface oxidation due to the exposure in the ambient condition and hydrolysis in the presence of water/moisture causes degradation in magnetic nanosheets that, in turn, affects the nanoelectronic /spintronic device performance. Counterintuitively, the current study reveals that exposure to the air at ambient atmosphere results in advent of a stable nonlayered secondary ferromagnetic phase in the form of Cr₂Te₃ (T_C2 ≈160 K) in the parent vdW magnetic semiconductor Cr₂Ge₂Te₆ (T_C1 ≈69 K). The coexistence of the two ferromagnetic phases in the time elapsed bulk crystal is confirmed through systematic investigation of crystal structure along with detailed dc/ac magnetic susceptibility, specific heat, and magneto-transport measurement. To capture the concurrence of the two ferromagnetic phases in a single material, Ginzburg-Landau theory with two independent order parameters (as magnetization) with a coupling term can be introduced. In contrast to the rather common poor environmental stability of the vdW magnets, the results open possibilities of finding air-stable novel materials having multiple magnetic phases.     

Preparation and Magnetic Properties of InTe–Cr2Te3 Alloys

InTe–Cr₂Te₃ alloys were prepared and characterized by temperature-dependent magnetic measurements. The results lend support to earlier phase-diagram data indicating the formation of compounds with the compositions In₉Cr₂Te₁₂ and In₂Cr₆Te₁₁. In₉Cr₂Te₁₂ is shown to be a ferromagnet, while In₂Cr₆Te₁₁ has a more complex magnetic structure.     

Toroidal spin ordering in BiFeO<Subscript>3</Subscript>, GaFeO<Subscript>3</Subscript>, and Cr<Subscript>2</Subscript>O<Subscript>3</Subscript> in the Faddeev model with a magnetic field

The Fadeev model is used for describing the recently discovered toroidal spin ordering in piezoelectric and ferrimagnetic GaFeO₃ and piezo- and magnetoelectric Cr₂O₃ and BiFeO₃. A stable toroidal solution of the Faddeev model with the topological charge Q= 1 in an external homogeneous magnetic field was obtained using the trial function method. The energy of a toroid as a function of its radius (R) was determined at various values of the external magnetic field (H). It was shown that the energy minimum is shifted toward smaller R’s with an increase in H. At a critical field value, the torus collapses so that the local spin structure disappears. It is suggested to use magnetic field for controlling the torus size in multiferroics, promising materials of spintronics.     

Intrinsic Van Der Waals Magnetic Materials from Bulk to the 2D Limit: New Frontiers of Spintronics

2D van der Waals (vdW) magnets, which present intrinsic ferromagnetic/antiferromagnetic ground states at finite temperatures down to atomic‐layer thicknesses, open a new horizon in materials science and enable the potential development of new spin‐related applications. The layered structure of vdW magnets facilitates their atomic‐layer cleavability and magnetic anisotropy, which counteracts spin fluctuations, thereby providing an ideal platform for theoretically and experimentally exploring magnetic phase transitions in the 2D limit. With reduced dimensions, the susceptibility of 2D magnets to a large variety of external stimuli also makes them more promising than their bulk counterpart in various device applications. Here, the current status of characterization and tuning of the magnetic properties of 2D vdW magnets, particularly the atomic‐layer thickness, is presented. Various state‐of‐the‐art optical and electrical techniques have been applied to reveal the magnetic states of 2D vdW magnets. Other emerging 2D vdW magnets and future perspectives on the stacking strategy are also given; it is believed that they will excite more intensive research and provide unprecedented opportunities in the field of spintronics.     

Potential 2D Materials with Phase Transitions: Structure,Synthesis, and Device Applications

Layered materials with phase transitions, such as charge density wave (CDW) and magnetic and dipole ordering, have potential to be exfoliated into monolayers and few‐layers and then become a large and important subfamily of two‐dimensional (2D) materials. Benefitting from enriched physical properties from the collective interactions, long‐range ordering, and related phase transitions, as well as the atomic thickness yet having nondangling bonds on the surface, 2D phase‐transition materials have vast potential for use in new‐concept and functional devices. Here, potential 2D phase‐transition materials with CDWs and magnetic and dipole ordering, including transition metal dichalcogenides, transition metal halides, metal thio/selenophosphates, chromium silicon/germanium tellurides, and more, are introduced. The structures and experimental phase‐transition properties are summarized for the bulk materials and some of the obtained monolayers. In addition, recent experimental progress on the synthesis and measurement of monolayers, such as 1T‐TaS₂, CrI₃, and Cr₂Ge₂Te₆, is reviewed.     

Relaxation and Magnetization Dynamics of Frustrated Spin-Chain Systems

A 3D model of the magnetization dynamics in frustrated triangular spin-chain systems Ca₃Co₂O₆ is proposed. This model is a generalization of the 2D model developed earlier. The spins are assumed to interact with the nearest neighbors and external agency (heat reservoir and external magnetic field) that causes them to change their states randomly with time. A probability of a single spin-flip process is assumed in a Glauber-like form. The 3D model allows describing the step-like behavior of a magnetization curves experimentally observed in a strong magnetic field.     

Giant Enhancements of Perpendicular Magnetic Anisotropy and Spin‐Orbit Torque by a MoS2 Layer

2D transition metal dichalcogenides have attracted much attention in the field of spintronics due to their rich spin‐dependent properties. The promise of highly compact and low‐energy‐consumption spin‐orbit torque (SOT) devices motivates the search for structures and materials that can satisfy the requirements of giant perpendicular magnetic anisotropy (PMA) and large SOT simultaneously in SOT‐based magnetic memory. Here, it is demonstrated that PMA and SOT in a heavy metal/transition metal ferromagnet structure, Pt/[Co/Ni]₂, can be greatly enhanced by introducing a molybdenum disulfide (MoS₂) underlayer. According to first‐principles calculation and X‐ray absorption spectroscopy (XAS), the enhancement of the PMA is ascribed to the modification of the orbital hybridization at the interface of Pt/Co due to MoS₂. The enhancement of SOT by the role played by MoS₂ is explained, which is strongly supported by the identical behavior of SOT and PMA as a function of Pt thickness. This work provides new possibilities to integrate 2D materials into promising spintronics devices.     

Magnetic Properties of Mg x Cu1−x Cr2O4 Spinels are Studied by Different Theoretical Methods

The external magnetic field induced the reorientation of magnetization of a ferromagnetic (or antiferromagnetic) treated within the framework of many-body Green’s function theory by considering all components of the magnetization. We present a new method for the calculation of expectation values in terms of the eigenvalues and eigenvectors of the equations of motion matrix for the set of Green’s functions. Magnetization and magnetic susceptibility are investigated when an external magnetic field is applied in (x-z)-plane. The mean field theory is applied to calculate the nearest neighbour and the next-neighbour super-exchange J ₁(Cr?Cr) and J ₂(Cr?(Mg(Cu)?O)?Cr), respectively, for the Mg _x Cu_1?x Cr₂O₄ in the range of 0 ≤ x ≤ 1. The intra-planar and the inter-planar interactions are deduced. The high-temperature series expansions (HTSEs) are derived for the magnetic susceptibility and two-spin correlation functions for a Heisenberg ferromagnetic model on the B-spinel lattice. The calculations are developed in the framework of the random-phase approximation (RPA). The magnetic-phase diagram is deduced. A spin-glass phase is predicted for intermediate range of concentration. The spin glass is obtained. The obtained results are comparable with those obtained by magnetic measurements. The critical exponents associated with the magnetic susceptibility (γ) and the correlation lengths (ν) have been deduced. The obtained values are comparable to those of 3D Heisenberg model.     

Proximity-Coupling-Induced Significant Enhancement of Coercive Field and Curie Temperature in 2D van der Waals Heterostructures

Magnetism in 2D has long been the focus of condensed matter physics due to its important applications in spintronic devices. A particularly promising aspect of 2D magnetism is the ability to fabricate 2D heterostructures with engineered optical, electrical, and quantum properties. Recently, the discovery of intrinsic ferromagnetisms in atomic thick materials has provided a new platform for investigations of fundamental magnetic physics. In contrast to 2D CrI₃ and Cr₂Ge₂Te₆ insulators, itinerant ferromagnetic Fe₃GeTe₂ (FGT), which has a larger intrinsic perpendicular anisotropy, higher Curie temperature (T_C), and relatively better stability, is a promising candidate for achieving permanent room-temperature ferromagnetism through interface or component engineering. Here, it is shown that the ferromagnetic properties of FGT thin flakes can be modulated through coupling with a FePS₃. The magneto-optical Kerr effect results show that the T_C of FGT is improved by more than 30 K and that the coercive field is increased by ≈100% due to the proximity coupling effect, which changes the spin textures of FGT at the interface. This work reveals that antiferromagnet/ferromagnet coupling is a promising way to engineer the magnetic properties of itinerant 2D ferromagnets, which paves the way for applications in advanced magnetic spintronic and memory devices.     

Toward 2D Magnets in the (MnBi2Te4)(Bi2Te3)n Bulk Crystal

2D magnets and their engineered magnetic heterostructures are intriguing materials for both fundamental physics and application prospects. On the basis of the recently discovered intrinsic magnetic topological insulators (MnBi₂Te₄)(Bi₂Te₃)_n, here, a new type of magnet, in which the magnetic layers are separated by a large number of non-magnetic layers and become magnetically independent, is proposed. This magnet is named as a single-layer magnet, regarding the vanishing interlayer exchange coupling. Theoretical calculations and magnetization measurements indicate that, the decoupling of the magnetic layers starts to emerge from n = 2 and 3, as revealed by a unique slow-relaxation behavior below a ferromagnetic-type transition at T_c = 12–14 K. Magnetization data analysis shows that the proposed new magnetic states have a strong uniaxial anisotropy along the c-axis, forming an Ising-type magnetic structure, where T_c is the ordering temperature for each magnetic layer. The characteristic slow relaxation, which exists only along the c-axis but is absent along the ab plane, can be ascribed to interlayer coherent spin rotation and/or intralayer domain wall movement. The present results will stimulate further theoretical and experimental investigations for the prototypical magnetic structures, and their combination with the topological surface states may lead to exotic physical properties.     

Controlled Growth and Thickness-Dependent Conduction-Type Transition of 2D Ferrimagnetic Cr2S3 Semiconductors

2D magnetic materials have attracted intense attention as ideal platforms for constructing multifunctional electronic and spintronic devices. However, most of the reported 2D magnetic materials are mainly achieved by the mechanical exfoliation route. The direct synthesis of such materials is still rarely reported, especially toward thickness-controlled synthesis down to the 2D limit. Herein, the thickness-tunable synthesis of nanothick rhombohedral Cr₂S₃ flakes (from ≈1.9 nm to tens of nanometers) on a chemically inert mica substrate via a facile chemical vapor deposition route is demonstrated. This is accomplished by an accurate control of the feeding rate of the Cr precursor and the growth temperature. Furthermore, it is revealed that the conduction behavior of the nanothick Cr₂S₃ is variable with increasing thickness (from 2.6 to 4.8 nm and >7 nm) from p-type to ambipolar and then to n-type. Hereby, this work can shed light on the scalable synthesis, transport, and magnetic properties explorations of 2D magnetic materials.     

Van der Waals Epitaxial Growth of 2D Metallic Vanadium Diselenide Single Crystals and their Extra‐High Electrical Conductivity

2D metallic transition‐metal dichalcogenides (MTMDs) have recently emerged as a new class of materials for the engineering of novel electronic phases, 2D superconductors, magnets, as well as novel electronic applications. However, the mechanical exfoliation route is predominantly used to obtain such metallic 2D flakes, but the batch production remains challenging. Herein, the van der Waals epitaxial growth of monocrystalline, 1T‐phase, few‐layer metallic VSe₂ nanosheets on an atomically flat mica substrate via a “one‐step” chemical vapor deposition method is reported. The thickness of the VSe₂ nanosheets is precisely tuned from several nanometers to several tenths of nanometers. More significantly, the 2D VSe₂ single crystals are found to present an excellent metallic feature, as evidenced by the extra‐high electrical conductivity of up to 10⁶ S m^?1, 1–4 orders of magnitude higher than that of various conductive 2D materials. The thickness‐dependent charge‐density‐wave phase transitions are also examined through low‐temperature transport measurements, which reveal that the synthesized 2D metallic 1T‐VSe₂ nanosheets should serve as good research platforms for the detecting novel many‐body states. These results open a new path for the synthesis and property investigations of nanoscale‐thickness 2D MTMDs crystals.     

A Single‐Electron Transistor Made of a 3D Topological Insulator Nanoplate

Quantum confined devices of 3D topological insulators are proposed to be promising and of great importance for studies of confined topological states and for applications in low‐energy‐dissipative spintronics and quantum information processing. The absence of energy gap on the topological insulator surface limits the experimental realization of a quantum confined system in 3D topological insulators. Here, the successful realization of single‐electron transistor devices in Bi₂Te₃ nanoplates using state‐of‐the‐art nanofabrication techniques is reported. Each device consists of a confined central island, two narrow constrictions that connect the central island to the source and drain, and surrounding gates. Low‐temperature transport measurements demonstrate that the two narrow constrictions function as tunneling junctions and the device shows well‐defined Coulomb current oscillations and Coulomb‐diamond‐shaped charge‐stability diagrams. This work provides a controllable and reproducible way to form quantum confined systems in 3D topological insulators, which should greatly stimulate research toward confined topological states, low‐energy‐dissipative devices, and quantum information processing.     

Hydrothermal synthesis and thermoelectric properties of nanostructured Bi0.5Sb1.5Te3 compounds

Single-phase Bi_0.5Sb_1.5Te₃ compounds have been prepared by hydrothermal synthesis at 150 °C for 24 h using SbCl₃, BiCl₃ and tellurium powder as precursors. X-ray diffraction (XRD) and field emission scanning electron microscopy (FESEM) have been applied to analyze the phase distributions, microstructures and grain sizes of the as-grown Bi_0.5Sb_1.5Te₃ products. It is found that the hydrothermally synthesized Bi_0.5Sb_1.5Te₃ nanopowders have a morphology dominated by irregular hexagonal sheets due to the anisotropic growth of the crystals. The Bi_0.5Sb_1.5Te₃ nanosheets are parallelly stacked in certain direction to form sheet-agglomerates attribute to the temperature gradients in the solution.     

Magnetic Proximity Effect in Graphene/CrBr3 van der Waals Heterostructures

2D van der Waals heterostructures serve as a promising platform to exploit various physical phenomena in a diverse range of novel spintronic device applications. Efficient spin injection is the prerequisite for these devices. The recent discovery of magnetic 2D materials leads to the possibility of fully 2D van der Waals spintronics devices by implementing spin injection through the magnetic proximity effect (MPE). Here, the investigation of MPE in 2D graphene/CrBr₃ van der Waals heterostructures is reported, which is probed by the Zeeman spin Hall effect through non-local measurements. Quantitative estimation of the Zeeman splitting field demonstrates a significant MPE field even in a low magnetic field. Furthermore, the observed anomalous longitudinal resistance changes at the Dirac point R_XX,D with increasing magnetic field near ν = 0 may be attributed to the MPE-induced new ground state phases. This MPE revealed in the graphene/CrBr₃ van der Waals heterostructures therefore provides a solid physics basis and key functionality for next-generation 2D spin logic and memory devices.     

Long-Range Spin-Triplet Superconductivity Induced by Magnetic Field in d Wave Superconductor/Ferromagnet Hybrid System

We theoretically study the long-range spin- triplet superconductivity in d wave superconductor/ ferromagnet/ferromagnet (S/F₁/F₂) trilayer junction, in which the magnetization of F₁ layer could be rotated in the y–z plane by an external magnetic field. The four-component Eilenberger equations were constructed to calculate the superconducting order parameters and density of states (DOS). Near the clean limit, the p wave equal-spin triplet component could be induced when the magnetization directions of F₁/F₂ layers are non-collinear, and the DOS exhibits a split zero-bias conductance peak. The various parameters such as ferromagnetic exchange energy, thickness of ferromagnetic layers, and angles between F₁/F₂ magnetization directions are studied for the effect on inducing triplet superconductivity. By magnetic field controlling the emergence of equal-spin triplet pairings or not, such a tunable S/F₁/F₂ trilayer junction based on long-range spin-triplet superconductivity could be used as a superconducting switch device, which would open up a new view of spintronics.