Interlayer Antiferromagnetic Interaction Research Articles

Probing the weak limit of magnetocrystalline anisotropy through a spin‒flop transition in the van der Waals antiferromagnet CrPS4

The influence of magnetocrystalline anisotropy (MCA) on antiferromagnetism is elucidated through the characterization of the spin‒flop transition. However, due to a lack of suitable candidates for investigation, a detailed understanding of the preservation of the spin‒flop transition in the presence of low MCA energy remains elusive. In this study, we introduce CrPS4, which is a two-dimensional van der Waals antiferromagnet, as an ideal system to explore the exceedingly weak limit of the thermally-evolved MCA energy. By employing a uniaxially anisotropic spin model and fitting it to the experimental magnetic properties, we quantify the MCA energy and identify the discernible spin configurations in different magnetic phases. Notably, even at the limit of extremely weak MCA, with a mere 0.12% of the interlayer antiferromagnetic exchange interaction at T = 33 K, which is slightly below the Néel temperature (TN) of 38 K, the spin‒flop transition remains intact. We further establish a direct correlation between the visualized spin arrangements and the progressive reversal of magnetic torque induced by rotating magnetic fields. This analysis reveals the essential role of MCA in antiferromagnetism, thus extending our understanding to previously undetected limits and providing valuable insights for the development of spin-processing functionalities based on van der Waals magnets.

Search for an antiferromagnetic Weyl semimetal in (MnTe) m (Sb2Te3) n and (MnTe) m (Bi2Te3) n superlattices

The interaction between topology and magnetism can lead to novel topological materials including Chern insulators, axion insulators, and Dirac and Weyl semimetals. In this work, a family of van der Waals layered materials using MnTe and Sb2Te3 or Bi2Te3 superlattices as building blocks are systematically examined in a search for antiferromagnetic Weyl semimetals, preferably with a simple node structure. The approach is based on controlling the strength of the exchange interaction as a function of layer composition to induce the phase transition between the topological and the normal insulators. Our calculations, utilizing a combination of first-principles density functional theory and tight-binding analyses based on maximally localized Wannier functions, clearly indicate a promising candidate for a type-I magnetic Weyl semimetal. This centrosymmetric material, Mn10Sb8Te22 (or (MnTe) m (Sb2Te3) n with m = 10 and n = 4), shows ferromagnetic intralayer and antiferromagnetic interlayer interactions in the antiferromagnetic ground state. The obtained electronic bandstructure also exhibits a single pair of Weyl points in the spin-split bands consistent with a Weyl semimetal. The presence of Weyl nodes is further verified with Berry curvature, Wannier charge center, and surface state (i.e. Fermi arc) calculations. Other combinations of the MnSbTe-family materials are found to be antiferromagnetic topological or normal insulators on either side of the Mn:Sb ratio, respectively, illustrating the topological phase transition as anticipated. A similar investigation in the homologous (MnTe) m (Bi2Te3) n system produces mostly nontrivial antiferromagnetic insulators due to the strong spin–orbit coupling. When realized, the antiferromagnetic Weyl semimetals in the simplest form (i.e. a single pair of Weyl nodes) are expected to provide a promising candidate for low-power spintronic applications.

Stacking-dependent interlayer magnetic interactions in CrSe2.

Recently, CrSe2, a new ferromagnetic van der Waals two-dimensional material, was discovered to be highly stable under ambient conditions, making it an attractive candidate for fundamental research and potential device applications. Here, we study the interlayer interactions of bilayer CrSe2using first-principles calculations. We demonstrate that the interlayer interaction depends on the stacking structure. The AA and AB stackings exhibit antiferromagnetic (AFM) interlayer interactions, while the AC stacking exhibits ferromagnetic (FM) interlayer interaction. Furthermore, the interlayer interaction can be further tuned by tensile strain and charge doping. Specifically, under large tensile strain, most stacking structures exhibit FM interlayer interactions. Conversely, under heavy electron doping, all stacking structures exhibit AFM interlayer interactions. These findings are useful for designing spintronic devices based on CrSe2.

The interlayer magnetic interaction in the CrI$_3$/CrSe$_2$ heterostructure

Abstract Based on first-principles calculations, we systematically studied the stacking energy and interlayer magnetic interaction of the heterobilayer composed of CrI$_3$ and CrSe$_2$ monolayers. We found that the stacking order plays a crucial role in the interlayer magnetic coupling. Among all possible stacking structures, the AA-stacking is the most stable heterostructure, exhibiting interlayer antiferromagnetic interactions. Interestingly, the interlayer magnetic interaction can be effectively tuned by biaxial strain. A 4.3% compressive strain would result in a ferromagnetic interlayer interaction in all stacking orders. These results reveal the magnetic properties of CrI$_3$/CrSe$_2$ heterostructure, which is expected to be applied to spintronic devices.

Interlayer magnetic interactions and ferroelectricity in π/3-twisted CrX2 (X = Se, Te) bilayers

Recently, two-dimensional (2D) bilayer magnetic systems have been widely studied. Their interlayer magnetic interactions play a vital role in the magnetic properties. In this paper, we theoretically studied the interlayer magnetic interactions, magnetic states, and ferroelectricity of π/3-twisted CrX2 (X = Se, Te) bilayers (π/3-CrX2). Our study reveals that the lateral shift could switch the magnetic state of the π/3-CrSe2 between interlayer ferromagnetic and antiferromagnetic, while just tuning the strength of the interlayer antiferromagnetic interactions in π/3-CrTe2. Furthermore, the lateral shift can alter the off-plane electric polarization in both π/3-CrSe2 and π/3-CrTe2. These results show that stacking is an effective way to tune both the magnetic and ferroelectric properties of 1T-CrX2 bilayers, making the 1T-CrX2 bilayers hold promise for 2D spintronic devices.

Spin-wave analysis of the ferromagnetic-ferromagnetic Heisenberg spin bilayer with intralayer single-ion anisotropy and interlayer antiferromagnetic interaction

In this paper, the spin wave theory is applied to the Heisenberg spin bilayer with intralayer ferromagnetic interaction [Formula: see text], intralayer single-ion anisotropy D and interlayer antiferromagnetic interaction [Formula: see text]. It is found that the effects of both D and [Formula: see text] on the thermodynamic quantities give rise to the two different low-temperature asymptotic behaviors with and without exponential law. For [Formula: see text], the interlayer antiferromagnetic interaction can induce the appearance of the maximum of the layer magnetization at finite temperatures. At the location of the layer magnetization maximum, the approximate behaviors (such as the power, linear, rational, exponential and logarithmic laws) which are driven by the temperature or the anisotropy, are obtained for the low-temperature thermodynamic properties. It is shown that the presence of antiferromagnetic interlayer interaction [Formula: see text] clearly induces more quantum fluctuations than the case where the interlayer interaction [Formula: see text] is ferromagnetic. Our results of the layer magnetization agree with the experimental data of the layered van der Waals crystal FeCl2 at low temperatures. In the monolayer case of [Formula: see text], our results are in agreement with the findings obtained by the existing theories and the quantum Monte Carlo data.

Classical model emerges in quantum entanglement: Quantum Monte Carlo study for an Ising-Heisenberg bilayer

By developing a cluster sampling of stochastic series expansion quantum Monte Carlo method, we investigate a spin-$1/2$ model on a bilayer square lattice with intra-layer ferromagnetic (FM) Ising coupling and inter-layer antiferromagnetic Heisenberg interaction. The continuous quantum phase transition which occurs at $g_c=3.045(2)$ between the FM Ising phase and the dimerized phase is studied via large scale simulations. From the analyzes of critical exponents we show that this phase transition belongs to the (2+1)-dimensional Ising universality class. Besides, the quantum entanglement is strong between the two layers, especially in dimerized phase. The effective Hamiltonian of single layer seems like a transverse field Ising model. However, we found the quantum entanglement Hamiltonian is a pure classical Ising model without any quantum fluctuations. Furthermore, we give a more general explanation about how a classical entanglement Hamiltonian emerges.

Preparation and Characterization of Francisite Solid Solutions Cu3Bi(Se1–xTexO3)2O2Br (x = 0–1): Possibility for Francisites as Starting Materials for Oxide van der Waals Ferromagnets

We synthesized the solid solutions Cu3Bi(Se1–xTexO3)2O2Br (x = 0, 0.25, 0.5, 0.75, 1) for the first time and characterized their structures by X-ray diffraction (XRD) measurements and their magnetic properties by electron spin resonance (ESR), magnetic susceptibility, magnetization, and specific heat measurements as well as by density functional theory (DFT) calculations. The Néel temperature TN and the critical field μ0HC needed for the metamagnetic transition increase with x, while the magnetization at a given magnetic field and the Curie–Weiss temperature Θ decrease with x. We show that the tendency for the interlayer antiferromagnetic (AFM) coupling in francisites is not explained by interlayer spin exchange but by the interlayer high-spin orbital interaction that occur across the van der Waals (vdW) gaps, hence indicating that francisites are vdW ferromagnets. This is surprising because, so far, well-established vdW ferromagnets are either layered tellurides or layered iodides. The trends in TN, μ0HC, and the magnetization of Cu3Bi(Se1–xTexO3)2O2Br as a function of x are well explained by the interlayer AFM interactions, and that in the Θ is explained by the intralayer spin exchanges. We proposed how one might modify francisites to make their interlayer interactions ferromagnetic (FM), hence leading to oxide vdW ferromagnets.

Field-orientation dependence of quantum phase transitions in the S=12 triangular-lattice antiferromagnet Ba3CoSb2O9

Ba$_3$CoSb$_2$O$_9$ approximates the two-dimensional spin-1/2 triangular-lattice Heisenberg antiferromagnet. This compound displays magnetic-field-induced quantum phase transitions, including the 1/3-magnetization-plateau, but its magnetization processes for the magnetic field $H$ parallel and perpendicular to the $c$ axis are different due to the weak easy-plane anisotropy and the weak interlayer antiferromagnetic exchange interaction. To elucidate how the quantum phase transitions change between these two field directions, we measured the field-angle dependence of the magnetization process in Ba$_3$CoSb$_2$O$_9$ using pulsed high magnetic fields. We compared obtained magnetic field-field angle phase diagram with those obtained by the large-size cluster mean-field method combined with a scaling scheme and the semiclassical theory. We also found a narrow 1/3-magnetization plateau and a high-field transition with a small magnetization jump for $H\,{\parallel}\,c$, not observed in the previous studies.

Revealing 2D Magnetism in a Bulk CrSBr Single Crystal by Electron Spin Resonance

Abstract2D magnets represent material systems in which magnetic order and topological phase transitions can be observed. Based on these phenomena, novel types of computing architectures and magnetoelectronic devices can be envisaged. Unlike conventional magnetic films, their magnetism is independent of the substrate and interface qualities, and 2D magnetic properties manifest even in formally bulk single crystals. However, 2D magnetism in layered materials is rarely reported often due to weak exchange interactions and magnetic anisotropy, and low magnetic transition temperatures. Here, the electron spin resonance (ESR) properties of a layered antiferromagnetic CrSBr single crystal are reported. The W‐like shape angular dependence of the ESR linewidth provides a signature for room temperature spin–spin correlations and for the XY spin model. By approaching the Néel temperature the arising of competing intralayer ferromagnetic and interlayer antiferromagnetic interactions might lead to the formation of vortex and antivortex pairs. This argument is inferred by modeling the temperature dependence of the ESR linewidth with the topological Berezinskii‐Kosterlitz‐Thouless phase transition. These findings together with the chemical stability and semiconducting properties, make CrSBr a promising layered magnet for future magneto‐ and topological‐electronics.

Skyrmion crystal and spiral phases in centrosymmetric bilayer magnets with staggered Dzyaloshinskii-Moriya interaction

We theoretically study a stabilization mechanism of the skyrmion crystal in centrosymmetric magnets with a bilayer structure. We show that the interplay between a layer-dependent staggered Dzyaloshinskii-Moriya interaction that arises from the absence of local inversion symmetry and the interlayer exchange interaction gives rise to a plethora of multiple-$Q$ states including the skyrmion crystal with a quantized topological number. By performing the simulated annealing for the bilayer triangular-lattice model under an external magnetic field, we demonstrate that the skyrmion forms the triangular-shaped crystals with different helicities in each layer owing to the staggered Dzyaloshinskii-Moriya interaction. Although the relative positions of the skyrmion core in each layer are different depending on the sign of the interlayer exchange interactions, the skyrmion crystal phases robustly appear under both ferromagnetic and antiferromagnetic interlayer interactions. We also find another two triple-$Q$ states with a uniform scalar chirality but without a quantized topological number in the low- and high-field regions. Especially, the low-field triple-$Q$ state exhibits the opposite sign of the scalar chirality to the skyrmion crystal, which is not found in the single-layer system. Our results indicate that the lack of local inversion symmetry in the lattice structure is another key ingredient to induce topological spin textures in centrosymmetric magnets.

Interlayer magnetic interactions in π/3-twisted bilayer CrI3

The interlayer magnetic interaction in bilayer CrI3 plays a crucial role for its device applications. In this work, we studied the interlayer magnetic interaction in π/3-twisted bilayer CrI3 using first-principles calculations. Our calculations show that the interlayer coupling can be ferromagnetic or antiferromagnetic depending crucially on lateral shift. The strongest antiferromagnetic interlayer interaction appears in the A¯A-stacking. The magnetic force theory calculations demonstrate that such an antiferromagnetic interaction is dominated by the eg–eg channel. Particularly, the interlayer antiferromagnetic interaction is very sensitive to external pressure. This highly tunable interlayer interaction makes π/3-twisted bilayer CrI3 a potential building block for magnetic field effect transistors and pressure sensors.

Magnetic and electronic structures of antiferromagnetic topological material candidate EuMg2Bi2

EuMg2Bi2 has been investigated to understand the electronic and magnetic behaviors as an antiferromagnetic (AFM) topological semimetal candidate. High-quality single crystals of EuMg2Bi2 were grown via a Bi flux and, subsequently, characterized to be consistent with the previously reported bulk magnetic and resistivity properties. A ferromagnetic interaction is indicated by the positive Curie–Weiss temperature obtained through fitting the bulk magnetic susceptibility data. The bulk resistivity measurements reveal an interesting electronic behavior that is potentially influenced by a competing antiferromagnetic and ferromagnetic interaction in and out of the ab plane. From the resulting refinement of the neutron diffraction data, EuMg2Bi2 was found to exhibit an A-type magnetic structure with Eu2+ moments ferromagnetically aligned in the plane and antiferromagnetically stacked between neighbor ferromagnetic Eu layers. The power law fitting magnetic ordering parameter below TN ∼ 8 K agrees with the 2D Heisenberg model, indicating a weak interlayer antiferromagnetic interaction. Considering the magnetic structure determined by neutron diffraction, the surface state calculation suggests that EuMg2Bi2 is an AFM topological insulator candidate. Linearly dispersed Dirac surface states were also observed in our angle-resolved photoemission spectroscopy measurements, consistent with the calculation.

Unique magnetic properties of Nd based cuprate francisite: Major enhancement upon Co doping

To understand the physical mechanism of intralayer ferromagnetic (FM) and interlayer antiferromagnetic (AFM) interactions in quasi-two-dimensional model of a real three-dimensional system, rare earth (RE)-Nd based cuprate francisite, Cu3Nd(SeO3)2O2Cl (NdCufr) was doped with Co and studied using structural (X-ray diffraction technique), magnetic (temperature and field dependent magnetization and specific heat measurements) and local structural (X-ray absorption technique) techniques supported by first principle theoretical calculation. The structure of the samples is orthorhombic and doped specimens indicate more or less substitutional incorporation of Co at Cu site. The magnetic properties highlighted with two transitions, viz. AFM to paramagnetic (PM) transition around 30 K and a spin reorientation transition (SRT) below 10 K. Two phenomena viz. magnetic hysteresis below SRT and magnetic field induced metamagnetic transition (MMT) were observed. Co doping significantly enhanced these two phenomena in addition to change the transition temperatures. The concomitant change and enhancement of magnetic properties by Co doping has been interpreted using splitting scheme of Cu-d and Nd-f states. The local structure study corroborates the overall findings and detects the cause of unexpected trend of magnetism with increasing Co doping.

Interlayer hydrogen bonding directed magnetic properties for a different number of water-intercalated structural heterometallic phosphates based on paddlewheel units Ru2(PO4)46−

Layered heterometallic phosphates {Mn(H2O)4}2Mn(H2O)2Ru2(PO4)4(H2O)2 (1) with a new topology were constructed from Ru2(PO4)46- and Mn2+ in the presence of anions as assisting reactants whose alkaline strength plays a key role in directing a different number of lattice water-intercalated structures. In the presence of CO32- and SO42- as assisting reactants, the assembling reaction in the aqueous solution at room temperature results in compounds 1·10H2O and 1·4H2O, respectively. Single-crystal X-ray diffraction analysis reveals that compounds 1·10H2O and 1·4H2O crystallize in orthorhombic space group Pbca and monoclinic space group P21/c, respectively. The layered structure of 1 is constructed by alternating Ru2O10 tetragonal dipyramid and MnO6 octahedra bridged by PO4 tetrahedra. The neutral heterometallic phosphate layers of 1 are separated by a different number of interlayer lattice water molecules, and hydrogen bonds are responsible for the neutral inorganic layer connection. Magnetism measurements show that compound 1·10H2O exhibits a soft magnet behaviour ordering below 8.5 K with indirect hydrogen bonding between these ferrimagnetic layers, and a reentrant spin-glass-like transition is observed for compound 1·4H2O, exhibiting two steps transition at 8.0 and 12 K, due to a strong competition between intralayer magnetic coupling and interlayer antiferromagnetic interactions mediated through the direct hydrogen bonding.

Role of anisotropy to the compensation in the Blume-Capel trilayered ferrimagnet

The trilayered Blume-Capel ($S=1$) magnet with nearest neighbour intralayer ferromagnetic and nearest neighbour interlayer antiferromagnetic interaction is studied by Monte Carlo simulation. Depending on the relative interaction strength and the value of anisotropy the critical temperature (where all the sublattice magnetisations and consequently the total magnetisation vanishes) and the compensation temperature (where the total magnetisation vanishes for a special combination of nonzero sublattice magnetisations) are estimated. The comprehensive phase diagrams with lines of critical temperatures and compensation temperatures for different parameter values are drawn.

Enhancement of the Magnetic Coupling in Exfoliated CrCl3 Crystals Observed by Low-Temperature Magnetic Force Microscopy and X-ray Magnetic Circular Dichroism.

Magnetic crystals formed by 2D layers interacting by weak van der Waals forces are currently a hot research topic. When these crystals are thinned to nanometric size, they can manifest strikingly different magnetic behavior compared to the bulk form. This can be the result of, for example, quantum electronic confinement effects, the presence of defects, or pinning of the crystallographic structure in metastable phases induced by the exfoliation process. In this work, an investigation of the magnetism of micromechanically cleaved CrCl3 flakes with thickness >10 nm is performed. These flakes are characterized by superconducting quantum interference device magnetometry, surface-sensitive X-ray magnetic circular dichroism, and spatially resolved magnetic force microscopy. The results highlight an enhancement of the CrCl3 antiferromagnetic interlayer interaction that appears to be independent of the flake size when the thickness is tens of nanometers. The estimated exchange field is 9 kOe, representing an increase of ≈900% compared to the one of the bulk crystals. This effect can be attributed to the pinning of the high-temperature monoclinic structure, as recently suggested by polarized Raman spectroscopy investigations in thin (8-35 nm) CrCl3 flakes.

Effects of interlayer and bi-quadratic exchange coupling on layered triangular lattice antiferromagnets

The magnetic field evolution of ground spin states of the stacked planar triangular antiferromagnet with antiferromagnetic interlayer interaction Jc is explored using a minimal 3D classical Heisenberg model. A bi-quadratic coupling is also used to mimic the effect of spin fluctuations (Zhitomirsky 2015 J. Phys.: Conf. Ser. 592 012110) which are known to stabilize the magnetization plateau. A single ion anisotropy is included and states with a magnetic field applied in the ab plane and along the c axis are determined. For -plane, an additional new state, in contrast to 2D model (Zhitomirsky 2015 J. Phys.: Conf. Ser. 592 012110), is obtained with weak interlayer interaction, while the magnetization plateau vanishes at large Jc and other new states with z components of spins emerge. For -axis, an extra state, compared with 2D model, is obtained with a weak interlayer interaction. When Jc is large enough, only the state corresponding to the Umbrella phase in 2D model exits.

Magnetic evolution of itinerant ferromagnetism and interlayer antiferromagnetism in cerium doped LaCo2P2 crystals

ThCr2Si2-type phosphide ACo2P2 (A=Eu, La, Pr, Nd, Ce) has the same structure as iron arsenides, but their magnetic behaviors are quite distinct. In this paper, we grew a series of La1−xCexCo2P2 single crystals (x=0.0 to1.0), made structural and magnetic characterizations. We found the introduction of cerium induces a rapid decrease of c-axis and a change from ferromagnetic to antiferromagnetic states. Compared to other trivalent doped compounds, the enhancement of ferromagnetism with doping is suppressed and the transition from ferromagnetism to antiferromagnetism appear earlier. By employing first-principles band-structure calculations, we identify the increase of Ce valence suppress the itinerant ferromagnetism and leading to formation of P-P bonding with the shortening of c-axis. The bonding effectively drives an increase of interlayer antiferromagnetic interaction, eventually leads to antiferromagnetic ordering of cobalt in high-doping region.

Bona fide interaction-driven topological phase transition in correlated symmetry-protected topological states

It is expected that the interplay between non-trivial band topology and strong electron correlation will lead to very rich physics. Thus a controlled study of the competition between topology and correlation is of great interest. Here, employing large-scale quantum Monte Carlo (QMC) simulations, we provide a concrete example of the Kane-Mele-Hubbard (KMH) model on an AA stacking bilayer honeycomb lattice with inter-layer antiferromagnetic interaction. Our simulation identified several different phases: a quantum spin-Hall insulator (QSH), a $xy$-plane antiferromagnetic Mott insulator ($xy$-AFM) and an inter-layer dimer-singlet insulator (dimer-singlet). Most importantly, a bona fide topological phase transition between the QSH and the dimer-singlet insulators, purely driven by the inter-layer antiferromagnetic interaction is found. At the transition, the spin and charge gap of the system close while the single-particle excitations remain gapped, which means that this transition has no mean field analogue and it can be viewed as a transition between bosonic SPT states. At one special point, this transition is described by a $(2+1)d$ $O(4)$ nonlinear sigma model (NLSM) with {\it exact} $SO(4)$ symmetry, and a topological term at {\it exactly} $\Theta = \pi$. Relevance of this work towards more general interacting SPT states is discussed.