Two-dimensional Magnets Research Articles

Large diversity of magnetic phases in two-dimensional magnets with spin-orbit coupling and superconductivity

Large diversity of magnetic phases in two-dimensional magnets with spin-orbit coupling and superconductivity

Theoretical investigations of two-dimensional intrinsic magnets derived from transition-metal borides M3B4 (M = Cr, Mn, and Fe)

ABSTRACT Two-dimensional (2D) magnetic materials with high critical temperatures (T C ) and robust magnetic anisotropy energies (MAE) hold significant potential for spintronic applications. However, most of 2D magnetic materials are derived from the van der Waals (vdW) layered bulks, which greatly limits the synthesis of 2D magnetic materials. Here, 2D M3B4 (M = Cr, Mn, and Fe; B = Boron), derived from hexagonal and orthorhombic M3AlB4 phases by selectively etching Al layers, was studied for its structural stability, electronic structure, and magnetic properties. By utilizing ab initio calculations and Monte Carlo simulations, we found that the orthorhombic Cr3B4 shows ferromagnetic (FM) metal and possesses an in-plane magnetic easy axis, while the remaining hexagonal and orthorhombic M3B4 structures exhibit antiferromagnetic (AFM) metals with a magnetic easy axis which is perpendicular to the two-dimensional plane. The critical temperatures of these 2D M3B4 structures are found to be above the 130 K. Notably, the ort-Mn3B4 possesses highest T C (~600 K) and strongest MAE (~220 µeV/atom) among these borides-based 2D magnetic materials. Our findings reveal that the 2D M3B4 compounds exhibit much better resistance to deformation compared to M2B2 MBenes and other 2D magnetic materials. The combination of high critical temperature, robust MAE, and excellent mechanical properties makes 2D Mn3B4 monolayer exhibits a favorable potential for spintronic applications. Our research also sheds light on the magnetic coupling mechanism of 2D M3B4, providing valuable insights into its fundamental characteristics.

Strain-induced intrinsic antiferromagnetic skyrmions in two-dimensional Janus magnets

Strain-induced intrinsic antiferromagnetic skyrmions in two-dimensional Janus magnets

Fractional topological charges in two-dimensional magnets

Fractional topological charges in two-dimensional magnets

Rich magnon topology in triangular lattice magnets

The two-dimensional magnet has been an emerging and rapidly growing field. The nontrivial topological phenomenon in these materials is an attracting subject. Yet, the realization of such magnets exhibiting topological magnons remains a challenge. Here, employing the linear spin-wave theory and the first-principles calculations, we propose that variety of topological phases exist in the triangular ferromagnet. These include magnon Chern insulators and high-order topological insulators. Interestingly, these topological states can coexist within a certain parameter space, leading to a hybrid topological state. We propose that these topological phases can be realized via atomic substitutions inMnSe2orMnTe2single-layers. The following detailed analysis suggests that non-uniform Dzyaloshinsky-Moriya interactions are crucial in achieving topological magnons. Our work unveil a unique approach to obtaining non-trivial topological magnons in two-dimensional materials.

Enhancement of interlayer exchange coupling via intercalation in 2D magnetic bilayers: towards high Curie temperature.

Two-dimensional magnetic materials are considered as promising candidates for developing next-generation spintronic devices by providing the possibility of scaling down to nanometers. However, a low Curie temperature is a crucial problem for practical applications, being intimately related to weak interlayer exchange coupling. Here, by using density functional theory calculations, we show that interlayer exchange coupling can be enhanced by intercalating 3d transition metals (Sc to Zn) into a bilayer of CrI3 and NiI2. It is found that intercalated Ni and Cr atoms exhibit strong antiferromagnetic coupling with the CrI3 and NiI2 host layers, respectively. This enhances the ferromagnetic interlayer exchange coupling between the host layers by many folds compared to pristine CrI3 and NiI2 bilayers. Moreover, both intercalated compounds show out-of-plane magnetic anisotropy with half metallic nature, which makes them ideal candidates for spintronics applications. Thereby our work provides a rational approach to raise the Curie temperature of non-metallic two-dimensional magnets by intercalation.

Ferrimagnetic second-order topological insulator with valley polarization in two-dimensional magnet

Two-dimensional (2D) ferromagnetic and antiferromagnetic second-order topological insulators (SOTIs) coexisting with valley polarization have received increasing attention recently, while 2D valley-polarized ferrimagnetic (ferri-valley) SOTI has not been reported yet. In this work, we propose an effective six-band tight-binding model based on structural symmetry to confirm the possibility of coexistence of ferrimagnetism, second-order topological corner states, and valley polarization in 2D systems, and predict Mo2CSCl monolayer as the robust 2D ferri-valley SOTI with good structural stability, considerable Curie temperature estimated to be 100 K, and distinct valley polarization up to 109 meV under out-of-plane exchange field based on our model and first-principles calculations. Also, we find that the spin polarization direction of corner states combined with valley polarization can be controlled by switching the direction of the magnetization direction using an external magnetic field. These findings of the combination of intrinsic ferrimagnetism, second-order topological properties, and valley polarization in single 2D materials provide an ideal platform for practical applications in multifield-control spintronic devices.

Prospect for detecting magnetism in two-dimensional perovskite oxides by electron magnetic circular dichroism

Two-dimensional (2D) magnets, especially strongly correlated 2D transition-metal perovskite oxides, have attracted significant attention due to their intriguing electromagnetic properties for potential applications in spintronic devices. Potentially electron magnetic circular dichroism (EMCD) under zone axis conditions can provide three-dimensional components of magnetic moments in 2D materials, but the collection efficiency and the signal-to-noise ratio for out-of-plane (OOP) components is limited due to the limited collection angle. Here we conducted a comprehensive computational simulation to optimize the experimental setting of EMCD for detecting the OOP components of magnetic moments in three beam conditions (3BCs) on 2D perovskite oxides La1-xSrxMnO3 (LSMO) in a TEM. The key parameters are sample thickness, accelerating voltage, Sr doping concentration, collection semi-angle and position, and sample orientation including systematic reflections excited and tilt angle. Our simulation results demonstrate that the relative dynamical diffraction coefficients of Mn OOP EMCD of LaMnO3 with a thickness ranging from 1 unit cell (uc) to 4 uc can be optimized in a 3BC with (110) systematic reflections excited and a relatively large collection semi-angle of 19 mrad at the relatively low accelerating voltage of 80 kV. In most cases, the relative dynamic diffraction coefficients for La1-xSrxMnO3 with the thickness ranging from 1 uc to 4 uc decrease with the increase of the Sr doping concentrations. The optimal tilt angle from a zone axis to a 3BC is 18° for the cases of the LSMO thickness of 2 uc, 3 uc and 4 uc, and 22° for the monolayer LSMO. Our work provides the theoretical simulation foundation for optimized EMCD experiments for measuring OOP components of magnetic moments in 2D transition-metal perovskite oxides.

Unveiling the spin evolution in van der Waals antiferromagnets via magneto-exciton effects

Among the fascinating phenomena observed in two-dimensional (2D) magnets, the magneto-exciton effect stands out as a pivotal link between optics and magnetism. Although the excitonic effect has been revealed and exhibits a considerable correlation with the spin structures in certain 2D magnets, the underlying mechanism of the magneto-exciton effect remains underexplored, especially under high magnetic fields. Here we perform a systematic investigation of the spin-exciton coupling in 2D antiferromagnetic NiPS3 under high magnetic fields. When an in-plane magnetic field is applied, the exceptional sharp excitonic emission at ~1.4756 eV exhibits a Zeeman-like splitting with g ≈ 2.0, experimentally identifying the exciton as an excitation of dominant triplet-singlet character. By examining the polarization of excitonic emission and simulating the spin evolution, we further verify the correlation between excitonic emission and Néel vector in NiPS3. Our work elucidates the mechanism behind the spin-exciton coupling in NiPS3 and establishes a strategy for optically probing the spin evolutions in 2D magnets.

Target-field design of surface permanent magnets

We present a target-field approach to analytically design magnetic fields using permanent magnets. We assume that their magnetization is bound to a two-dimensional surface and is composed of a complete basis of surface modes. By posing the Poisson’s equation relating the magnetic scalar potential to the magnetization using Green’s functions, we derive simple integrals that determine the magnetic field generated by each mode. This approach is demonstrated by deriving the governing integrals for optimizing axial magnetization on cylindrical and circular-planar surfaces. We approximate the governing integrals numerically and implement them into a regularized least-squares optimization routine to design permanent magnets that generate uniform axial and transverse target magnetic fields. The resulting uniform axial magnetic field profiles demonstrate more than a tenfold increase in uniformity across equivalent target regions compared to the field generated by an optimally separated axially magnetized pair of rings, as validated using finite element method simulations. We use a simple example to examine how two-dimensional surface magnetization profiles can be emulated using thin three-dimensional volumes and determine how many discrete intervals are required to accurately approximate a continuously varying surface pattern. Magnets designed using our approach may enable higher-quality bias fields for electric machines, nuclear fusion, fundamental physics, magnetic trapping, and beyond. Published by the American Physical Society 2024

Multiple Valley Modulations in Noncollinear Antiferromagnets.

Two-dimensional valleys and magnetism are rising areas with intriguing properties and practical uses in advanced information technology. By coupling valleys to collinear magnetism, valley degeneracy is lifted in a large number of magnetic valley materials to exploit the valley degree of freedom. Beyond collinear magnetism, new coupling modes between valley and magnetism are few but highly desirable. By tight-binding calculations of a breathing Kagome lattice, we demonstrate a tunable valley structure and valley-contrasting physical properties in noncollinear antiferromagnets. Distinct from collinear magnetism, noncollinear antiferromagnetic order enables valley splittings even without spin-orbit coupling. Both the canting and azimuthal angles of magnetic moments can be used as experimentally accessible knobs to tune valley splittings. Our first-principles calculations of the Fe3C6O6-silicene-Fe3C6O6 heterostructure also exhibit tunable valley splittings in noncollinear antiferromagnetism, agreeing with our tight-binding results. Our work paves avenues for designing novel magnetic valley materials and energy-efficient valleytronic devices based on noncollinear magnetism.

Exact staggered dimer ground state and its stability in a two-dimensional magnet

Exact staggered dimer ground state and its stability in a two-dimensional magnet

Effect of Magnetic Field and Temperature on the Magnetic Structure of a Two-Dimensional Magnet on a Substrate

Effect of Magnetic Field and Temperature on the Magnetic Structure of a Two-Dimensional Magnet on a Substrate

Synthesis and properties of Sr2La2NiW2O12, a new S= 1 triangular lattice magnet.

Magnetic materials featuring triangular arrangements of spins are frequently investigated as platforms hosting magnetic frustration. Hexagonal perovskites with ordered vacancies serve as excellent candidates for two-dimensional triangular magnetism due to the considerable separation of the magnetic planes. In this work, the effects of chemical pressure on the ferromagnetic ground state of Ba2La2NiW2O12 by substitution of Ba2+ with Sr2+ to produce Sr2La2NiW2O12 are investigated. The two materials are characterized using synchrotron-based XRD, XANES and EXAFS in addition to magnetometry in order to correlate their crystal structures and magnetic properties. Both materials form in space group R3, yet as a result of the enhanced bending of key bond angles due to the effects of chemical pressure, the TC value of the magnetic Ni2+ sublattice is reduced from ∼6 K in Ba2La2NiW2O12 to 4 K in Sr2La2NiW2O12.

Electronic excitations and spin interactions in chromium trihalides from embedded many-body wavefunctions

Although chromium trihalides are widely regarded as a promising class of two-dimensional magnets for next-generation devices, an accurate description of their electronic structure and magnetic interactions has proven challenging to achieve. Here, we quantify electronic excitations and spin interactions in CrX3 (X = Cl, Br, I) using embedded many-body wavefunction calculations and fully generalized spin Hamiltonians. We find that the three trihalides feature comparable d-shell excitations, consisting of a high-spin 4A2(t2g3eg0)\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$({t}_{2g}^{3}{e}_{g}^{0})$$\\end{document} ground state lying 1.5–1.7 eV below the first excited state 4T2 (t2g2eg1\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${t}_{2g}^{2}{e}_{g}^{1}$$\\end{document}). CrCl3 exhibits a single-ion anisotropy Asia = − 0.02 meV, while the Cr spin-3/2 moments are ferromagnetically coupled through bilinear and biquadratic exchange interactions of J1 = − 0.97 meV and J2 = − 0.05 meV, respectively. The corresponding values for CrBr3 and CrI3 increase to Asia = −0.08 meV and Asia= − 0.12 meV for the single-ion anisotropy, J1 = −1.21 meV, J2 = −0.05 meV and J1 = −1.38 meV, J2 = −0.06 meV for the exchange couplings, respectively. We find that the overall magnetic anisotropy is defined by the interplay between Asia and Adip due to magnetic dipole–dipole interaction that favors in-plane orientation of magnetic moments in ferromagnetic monolayers and bulk layered magnets. The competition between the two contributions sets CrCl3 and CrI3 as the easy-plane (Asia + Adip >0) and easy-axis (Asia + Adip <0) ferromagnets, respectively. The differences between the magnets trace back to the atomic radii of the halogen ligands and the magnitude of spin–orbit coupling. Our findings are in excellent agreement with recent experiments, thus providing reference values for the fundamental interactions in chromium trihalides.

Phonon-induced renormalization of exchange interactions in metallic two-dimensional magnets

Phonon-induced renormalization of exchange interactions in metallic two-dimensional magnets

Room-Temperature CrI3 Magnets through Lithiation.

The pursuit of two-dimensional (2D) magnetism is promising for energy-efficient electronic devices, including magnetoelectric random access memory and radio frequency/microwave magnonics, and it is gaining fundamental insights into quantum sensing technology. The key challenge resides in overseeing magnetic exchange interactions through a precise chemical reduction process, wherein manipulation of the arrangement of atoms and electrons is essential for achieving room-temperature 2D magnetism tailoring in a manner compatible with device architectures. Here, we report an electrochemically crafted CrI3 layered magnet─a van der Waals material─with precisely tailored lithiation and delithiation degrees. The crystalline and packing structure within the intralayer are preserved during the lithium intercalation within the interlayer, owing to weak interlayer coupling. Intrinsic ferromagnetism featuring a Curie temperature reaching 420 K has been unequivocally demonstrated, showcasing a coercivity of 1120 Oe at room temperature. The degree of lithiation through the reduction from Cr3+ to Cr2+ plays a crucial role in determining a 28.5% change in magnetization and a 0.29 eV shift in the bandgap. Room temperature ferromagnetism and magnetoelectricity are critical for noncontact, specifically photon-driven, dynamic magnetism control of 2D magnet-based magnonics devices.

Understanding two-dimensional tractor magnets: Theory and realizations

We present a comparative investigation of two-dimensional tractor magnet configurations, analyzing both theoretical predictions and experimental results with a focus on the minimal tractor magnet. The minimal tractor magnet consists of a rigid assembly of one attracting magnet (attractor), two repelling magnets (repulsors), and a fourth magnet (follower) that is magnetically stabilized in a local energy minimum. The theoretical framework relies on magnetostatics and stability analysis of stationary equilibria. To calculate the magnetostatic force and energy, we use a multipole method. In a first approximation, we derive analytical results from the point dipole approximation. The point dipole analysis defines an upper bound criterion for the magnetic moment ratio and provides analytical expressions for stability bounds in relation to geometry parameters. Our experimental results are consistent with the predictions from the fourth-order multipole expansion. Beyond the minimal tractor magnet, we introduce a more advanced configuration that allows for a higher magnetic binding energy and follower capture at larger distances.

Probing intrinsic magnetic domain in bare CrI3 bulk with a magnetic force microscope

Two-dimensional magnetism in CrI3 links to its stacking structural order. In bulk CrI3, coexistence of monoclinic and rhombohedral phases has been observed across wide temperature range. Direct characterization of the magnetic textures on the exposed surface of bulk CrI3 has been challenging but meaningful. Here, we have employed a custom glovebox-assisted magnetic force microscope to observe the evolution of magnetic domains on the bare CrI3 surface under variable temperatures and magnetic fields for the first time. Below the Curie temperature, robust parallel stripe magnetic domains spontaneously emerge. The root mean square values of the localized weak pinning domain images at various temperatures indicate a critical transition behavior consistent with 3D Ising model with Tc ∼ 59 K. Images obtained by varying the magnetic field at low temperatures, showing magnetization saturation-reentry cycles, reveal larger hysteresis and stronger disorder compared to the VSM measurement, indicating local structural phase inhomogeneity. ​Two in-plane stripe magnetic domains oriented locally at an angle of 51-degrees compete under an out-of-plane magnetic field, presumably due to different sliding orientations induced by the magnetic field during the transition from a monoclinic to a rhombohedral phase. This study provides an experimental reference for future spin density wave manipulation in CrI3.

FePd2Te2: An Anisotropic Two-Dimensional Ferromagnet with One-Dimensional Fe Chains.

Two-dimensional (2D) magnets have attracted significant attention in recent years due to their importance in the research on both fundamental physics and spintronic applications. Here, we report the discovery of a new ternary compound FePd2Te2. It features a layered quasi-2D crystal structure with 1D Fe zigzag chains extending along the b-axis in the cleavage plane. Single crystals of FePd2Te2 with centimeter size could be grown. Density functional theory calculations, mechanical exfoliation, and atomic force microscopy on these crystals reveal that they are 2D materials that can be thinned down to ∼5 nm. Magnetic characterization shows that FePd2Te2 is an easy-plane ferromagnet with TC ∼ 183 K and strong in-plane uniaxial magnetic anisotropy. Magnetoresistance and the anomalous Hall effect demonstrate that ferromagnetism could be maintained in FePd2Te2 flakes with large coercivity. A crystal twinning effect is observed by scanning tunneling microscopy which makes the Fe chains right angle bent in the cleavage plane and creates an intriguing spin texture. Besides, a large electronic specific heat coefficient of up to γ ∼ 32.4 mJ mol-1 K-2 suggests FePd2Te2 is a strongly correlated metal. Our results show that FePd2Te2 is a correlated anisotropic 2D magnet that may attract multidisciplinary research interests.