Antiferromagnetic Interlayer Coupling Research Articles

Evidence of Ferromagnetism and Ultrafast Dynamics of Demagnetization in an Epitaxial FeCl2 Monolayer.

The development of two-dimensional (2D) magnetism is driven not only by the interest of low-dimensional physics but also by potential applications in high-density miniaturized spintronic devices. However, 2D materials possessing a ferromagnetic order with a relatively high Curie temperature (Tc) are rare. In this paper, the evidence of ferromagnetism in monolayer FeCl2 on Au(111) surfaces, as well as the interlayer antiferromagnetic coupling of bilayer FeCl2, is characterized by using spin-polarized scanning tunneling microscopy. A Curie temperature (Tc) of ∼147 K is revealed for monolayer FeCl2, based on our static magneto-optical Kerr effect measurements. Furthermore, temperature-dependent magnetization dynamics is investigated by the time-resolved magneto-optical Kerr effect. A transition from one- to two-step demagnetization occurs as the lattice temperature approaches Tc, which supports the Elliott-Yafet spin relaxation mechanism. The findings contribute to a deeper understanding of the underlying mechanisms governing ultrafast magnetization in 2D ferromagnetic materials.

Sub-terahertz excitations in a synthetic antiferromagnet with perpendicular anisotropy

In this paper, micromagnetic simulations are employed to investigate terahertz (THz) magnetic excitations in a spin torque nano-oscillator (STNO) with a perpendicularly magnetized synthetic antiferromagnetic (SAF) free layer. The magnetization precession of the free layer can be finely tuned into the sub-THz range without the necessity of external magnetic fields. The excited frequency exhibits two distinctive regions, namely region-I and region-II, depending on the applied current strength. In region-I, characterized by relatively small currents, the two ferromagnetic layers are stabilized at two separate precession orbits. The frequency in this region decreases with current strength, exhibiting similar features as the Néel vector change observed in antiferromagnets. In contrast, region-II is defined by currents where the two ferromagnetic layers synchronize into the same precession orbit. The frequency increases with current, correlating with the variation in the net magnetization of the SAF layer. An analytical model is developed through the canonical transformation of Lagrange’s equation, which can describe the frequency dependence on both the applied current and the antiferromagnetic interlayer coupling strengths. The simulations and the analytical model show good agreement, offering a more profound understanding of the magnetic excitation properties in STNOs with ultrathin SAF free layers. These insights are crucial for the design of advanced terahertz spintronic devices.

Bi2Te3-intercalated MnBi2Te4: ideal candidate to explore intrinsic Chern insulator and high-temperature quantum anomalous Hall effect

The recently discovered magnetic topological insulator of MnBi2Te4 (MBT), has been demonstrated to realize the quantum anomalous Hall (QAH) effect, while the naturally antiferromagnetic (AFM) interlayer coupling in MBT results in that the QAH effect can only be realized in odd-layered systems and at low temperature. Using first-principles calculations, we find that intercalating Bi2Te3 (BT) layers into MBT by forming MBT/(BT) n /MBT (n = 1–6) heterostructures can induce magnetic phase transition from AFM to ferromagnetic (FM) interlayer coupling when n⩾ 3. Specifically, MBT/(BT)3/MBT and MBT/(BT)4/MBT respectively host Curie temperatures T c of 14 K and 11 K, which fits well the experimentally measured T c of 12 K. Detailed band structure calculations and topological identification show that the QAH phases are well preserved for all FM heterostructures. And the topological mechanism of MBT/(BT) n /MBT as a function of n is revealed by employing continuum model analysis. Most importantly, the FM MBT/(BT)4/MBT has already been experimentally fabricated. Thus, our work provides a practical guideline to explore high-temperature QAH effect in MBT family of materials.

Interlayer antiferromagnetic coupling in Tb3Fe5O12/Y3Fe5O12 bilayers

The interlayer antiferromagnetic (AFM) coupling between thin films plays a significant role in the application of spintronics and magnetic memory devices. Previously, we observed AFM coupling phenomenon at low temperatures in rare-earth iron garnet bilayers epitaxially grown on Y3Al5O12 substrates. Here, we report a detailed study on the impacts of various factors, including temperature, crystallographic orientation, and layer thickness, on the AMF coupling and magnetization reversal behavior of such a bilayer system. A simple energy model qualitatively described the coupling behavior of the two layers during the magnetization reversal process. The interlayer coupling strength was calculated by measuring the minor magnetic hysteresis loops. The current results can serve as a reminder for future research on interlayer AFM coupling phenomena and highlight the potential of manipulating the magnetic properties in rare-earth garnet bilayers for spintronics studies and other applications.

Classification of hysteresis loops for exchange biased F/NM/F trilayer with antiferromagnetic interlayer coupling

Major hysteresis loops of the F/NM/F/AF structure are classified according to the magnetization process, with the assumption of coherent rotation for each F component and antiferromagnetic coupling between the two F layers. Magnetic stable states of the system as well as specific reversal modes of magnetization during each stage of the major hysteresis cycle are studied in detail based on energetics analysis, in the whole range of exchange bias field and interlayer antiferromagnetic coupling strength. The analysis shows 12 different types of major hysteresis loops for this system and is confirmed by simulation. Strategies to determine key material parameters for the F/NM/F/AF structure from major hysteresis loops are proposed and illustrated by numerical simulation. The research shows a subtle tuning of the magnetization process in the F/NM/F/AF structure, collectively by exchange biasing and interlayer antiferromagnetic coupling. Practically, this serves as a theoretical grounding for the identification of root causes of failure in the product analysis of GMR (giant magnetoresistance) sensors.

Electrically tunable lateral spin-valve transistor based on bilayer CrI3

The recent discovery of two-dimensional (2D) magnetic materials has opened new frontiers for the design of nanoscale spintronic devices. Among 2D nano-magnets, bilayer CrI3 outstands for its antiferromagnetic interlayer coupling and its electrically-mediated magnetic state control. Here, leveraging on CrI3 magnetic and electrical properties, we propose a lateral spin-valve transistor based on bilayer CrI3, where the spin transport is fully controlled via an external electric field. The proposed proof-of-concept device, working in the ballistic regime, is able to both filter (>99%) and select ON/OFF the spin current up to a ratio of ≈102, using a double split-gate architecture. Our results obtained exploiting a multiscale approach ranging from first-principles to out-of-equilibrium transport calculations, open unexplored paths towards the exploitation of bilayer CrI3 or related 2D nano-magnets, as a promising platform for future electrically tunable, compact, and scalable spintronic devices.

Electrical tuning of robust layered antiferromagnetism in MXene monolayer

A-type antiferromagnetism, with an in-plane ferromagnetic order and the interlayer antiferromagnetic coupling, owns inborn advantages for electrical manipulations but is naturally rare in real materials except in those artificial antiferromagnetic heterostructures. Here, a robust layered antiferromagnetism with a high Néel temperature is predicted in a MXene Cr2CCl2 monolayer, which provides an ideal platform as a magnetoelectric field effect transistor. Based on first-principles calculations, we demonstrate that an electric field can induce the band splitting between spin-up and spin-down channels. Although no net magnetization is generated, the inversion symmetry between the lower Cr layer and the upper Cr layer is broken via electronic cloud distortions. Moreover, this electric field can be replaced by a proximate ferroelectric layer for non-volatility. The magneto-optic Kerr effect can be used to detect this magnetoelectricity, even if it is a collinear antiferromagnet with zero magnetization.

Efficient characteristics of exchange coupling and spin–flop transition in Py/Gd bilayer using anisotropic magnetoresistance

Interlayer antiferromagnetic coupling rare-earth/transition-metal bilayer ferrimagnet systems have attracted much attention because they present different unusual temperature- and field-dependent nontrivial magnetic states and dynamics. These properties and the implementation of their applications in spintronics highly depend on the significant temperature dependence of the magnetic exchange stiffness constant A. Here, we quantitatively determine the temperature dependence of magnetic exchange stiffness APy−Gd and AGd in the artificially layered ferrimagnet consisting of a Py/Gd bilayer, using a measurement of anisotropic magnetoresistance of the bilayer thin film at different temperatures and magnetic fields. The obtained temperature dependencies of APy−Gd and AGd exhibit a scaling power law with the magnetization of Gd. The critical field of spin–flop transition and its temperature dependence can also be directly obtained by this method. Additionally, the experimental results are well reproduced by micromagnetic simulations with the obtained parameters APy−Gd and AGd, which further confirms the reliability of this easily accessible technique.

Layer-Dependent Magnetic Structure and Anomalous Hall Effect in the Magnetic Topological Insulator MnBi4Te7.

The intrinsic antiferromagnetic topological insulator (TI) MnBi4Te7 provides a capacious playground for the realization of topological quantum phenomena, such as the axion insulator states and quantum anomalous Hall (QAH) effect. In addition to nontrivial band topology, magnetism is another necessary ingredient for realizing these quantum phenomena. Here, we investigate signatures of thickness-dependent magnetism in exfoliated MnBi4Te7 thin flakes. We observe an obvious odd-even layer-number effect in few-layer MnBi4Te7. Noticeably, we show that in monolayer MnBi4Te7 the anomalous Hall effect exhibits a sign reversal. Compared with the case of MnBi2Te4, interlayer antiferromagnetic exchange coupling, which is essential for the realization of the QAH effect, is greatly suppressed in MnBi4Te7. The demonstration of thickness-dependent magnetic properties is helpful to further explore the topological quantum phenomena in MnBi4Te7.

Theoretical Analysis of Magnetic Coupling in the Ti2C Bare MXene.

The nature of the electronic ground state of the Ti2C MXene is unambiguously determined by making use of density functional theory-based calculations including hybrid functionals together with a stringent computational setup providing numerically converged results up to 1 meV. All the explored density functionals (i.e., PBE, PBE0, and HSE06) consistently predict that the Ti2C MXene has a magnetic ground state corresponding to antiferromagnetic (AFM)-coupled ferromagnetic (FM) layers. A spin model, with one unpaired electron per Ti center, consistent with the nature of the chemical bond emerging from the calculations, is presented in which the relevant magnetic coupling constants are extracted from total energy differences of the involved magnetic solutions using an appropriate mapping approach. The use of different density functionals enables us to define a realistic range for the magnitude of each of the magnetic coupling constants. The intralayer FM interaction is the dominant term, but the other two AFM interlayer couplings are noticeable and cannot be neglected. Thus, the spin model cannot be reduced to include nearest-neighbor interactions only. The Néel temperature is roughly estimated to be in the 220 ± 30 K, suggesting that this material can be used in practical applications in spintronics and related fields.

Magnon corner states in twisted bilayer honeycomb magnets

Search for higher-order topological insulators, characterized by topologically protected gapless boundary states of codimension higher than one, in bosonic systems has attracted growing interest. Here, we establish twisted bilayer honeycomb magnets as a new platform for hosting second-order topological magnon insulators (SOTMIs) without fine-tuning. We employ a simple, minimal Heisenberg spin model to describe misaligned bilayer sheets of honeycomb ferromagnetic magnets with a large commensurate twist angle. We found that the higher-order topology in this bilayer system shows a significant dependence on the interlayer exchange coupling. The SOTMI, featuring topologically protected magnon corner states, appears for ferromagnetic interlayer couplings, while the twisted bilayer exhibits a nodal phase in the case of antiferromagnetic interlayer coupling.

Interplay between magnetic order and electronic band structure in ultrathin GdGe2 metalloxene films.

Dimensionality can strongly influence the magnetic structure of solid systems. Here, we predict theoretically and confirm experimentally that the antiferromagnetic (AFM) ground state of bulk gadolinium germanide metalloxene, which has a quasi-layered defective GdGe2 structure, is preserved in the ultrathin film limit. Ab initio calculations demonstrate that ultrathin GdGe2 films present in-plane intra-layer ferromagnetic coupling and AFM inter-layer coupling in the ground state. Angle-resolved photoemission spectroscopy finds the AFM-induced band splitting expected for the 2 and 3 GdGe2 trilayer (TL) films, which disappear above the Néel temperature. The comparative analysis of isostructural ultrathin DyGe2 and GdSi2 films confirms the magnetic origin of the observed band splitting. These findings are in contrast with the recent report of ferromagnetism in ultrathin metalloxene films, which we ascribe to the presence of uncompensated magnetic moments.

Strain-tunable magnetism and topological states in layered VBi2Te4.

Similar to the magnetic topological insulator of MnBi2Te4, recent studies have demonstrated that VBi2Te4 is also an ideal candidate to explore many intriguing quantum states. Different from the strong interlayer antiferromagnetic (AFM) coupling in layered MnBi2Te4, based on first-principles calculations, we find that the energy difference between AFM and ferromagnetic (FM) orders in layered VBi2Te4 is much smaller than that of MnBi2Te4. Specifically, it is found that the interlayer FM coupling can be readily achieved by applying strain. Further electronic band structures reveal that the VBi2Te4 bilayer is a time-reversal symmetry broken quantum spin Hall insulator with a spin Chern number of CS = 1, which is essentially different from the QAH state with a Chern number of C = 1 in the MnBi2Te4 bilayer. Most strikingly, the topological states of the magnetic VBi2Te4 bilayer can be well tuned by strain, whose topological phase diagram is mapped out as a function of strain by employing continuum model analyses. All of these results indicate that the layered VBi2Te4 not only enriches the family of magnetic topological materials, but also provides a promising platform to explore more exotic quantum phenomena.

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.

Spin excitations in the kagome-lattice metallic antiferromagnet Fe0.89Co0.11Sn

Kagome-lattice materials have attracted tremendous interest due to the broad prospect for seeking superconductivity, quantum spin liquid states, and topological electronic structures. Among them, the transition-metal kagome lattices are high-profile objects for the combination of topological properties, rich magnetism, and multiple-orbital physics. Here we report an inelastic neutron scattering study on the spin dynamics of a kagome-lattice antiferromagnetic metal ${\mathrm{Fe}}_{0.89}{\mathrm{Co}}_{0.11}\mathrm{Sn}$. Although the magnetic excitations can be observed up to $\ensuremath{\sim}250$ meV, well-defined spin waves are only identified below $\ensuremath{\sim}90$ meV and can be modeled using Heisenberg exchange with ferromagnetic in-plane nearest-neighbor coupling ${J}_{1}$, in-plane next-nearest-neighbor coupling ${J}_{2}$, and antiferromagnetic (AFM) interlayer coupling ${J}_{c}$ under linear spin-wave theory. Above $\ensuremath{\sim}90$ meV, the spin waves enter the itinerant Stoner continuum and become highly damped particle-hole excitations. At the $K$ point of the Brillouin zone, we reveal a possible band crossing of the spin wave, which indicates a potential Dirac magnon. Our results uncover the evolution of the spin excitations from the planar AFM state to the axial AFM state in ${\mathrm{Fe}}_{0.89}{\mathrm{Co}}_{0.11}\mathrm{Sn}$, solve the magnetic Hamiltonian for both states, and confirm the significant influence of the itinerant magnetism on the spin excitations.

Electric field induced tunable half-metallicity in an A -type antiferromagnetic bilayer LaBr2

How to achieve half-metallicity is always a central topic in spintronics and the polarity-tunable half-metallicity is particularly interesting for spin manipulation. In this work, motivated by the intrinsic ferromagnetism in the monolayer electride ${\mathrm{LaBr}}_{2}$, based on density functional theory calculations, we investigate the electronic and magnetic properties of bilayer ${\mathrm{LaBr}}_{2}$, with an aim to search for polarity-tunable half-metallicity. We first find that the antiferromagnetic interlayer coupling state is the ground state and the band structure is spin degenerate, with an indirect band gap of 0.454 eV. By applying a vertical electric field, spin splitting occurs and when the electric field is strong enough ($\ensuremath{\ge}0.33$ V/\AA{}), half-metallicity can be achieved. More interestingly, the spin polarity of the half-metallicity can be tuned by reversing the electric field direction. It originates from the spatial separation of the two spin channels in both the valence band and conduction band and their localization at different layers. Based on the polarity-tunable half-metallicity under vertical electric field, a magnetic tunnel junction based on bilayer ${\mathrm{LaBr}}_{2}$ is designed and the ON/OFF switching can be achived by applying parallel or anti-parallel vertical electric fields in the two leads, which leads to giant tunnel magnetoresistance up to $1\ifmmode\times\else\texttimes\fi{}{10}^{6}$. The findings suggest new potential of ${\mathrm{LaBr}}_{2}$, and more generally, $A$-type antiferromagnets of application in spintronic devices.

Tailoring the magnetic exchange interaction in MnBi2Te4 superlattices via the intercalation of ferromagnetic layers

The intrinsic magnetic topological insulator MnBi2Te4 (MBT) provides a platform for the creation of exotic quantum phenomena. Novel properties can be created by modification of the MnBi2Te4 framework, but the design of stable magnetic structures remains challenging. Here we report ferromagnet-intercalated MnBi2Te4 superlattices with tunable magnetic exchange interactions. Using molecular beam epitaxy, we intercalate ferromagnetic MnTe layers into MnBi2Te4 to create [(MBT)(MnTe)m]N superlattices and examine their magnetic interaction properties using polarized neutron reflectometry and magnetoresistance measurements. Incorporation of the ferromagnetic spacer tunes the antiferromagnetic interlayer coupling of the MnBi2Te4 layers through the exchange-spring effect at MnBi2Te4/MnTe hetero-interfaces. The MnTe thickness can be used to modulate the relative strengths of the ferromagnetic and antiferromagnetic order, and the superlattice periodicity can tailor the spin configurations of the synthesized multilayers.

Tunnel magnetoresistance sensors with dual soft-pinned free layers exhibiting highly symmetric resistance-field response curves

We report on tunnel magnetoresistance (TMR) sensors with two ferromagnetic free layers (FLs) on both sides of a MgO tunnel barrier. The magnetizations of these FLs are weakly (softly) pinned in an anti-parallel configuration by the exchange bias of IrMn antiferromagnetic layers through ferromagnetic and/or antiferromagnetic interlayer couplings of non-magnetic spacer layers. These dual soft-pinned FL (SPFL) sensors show a symmetric resistance (R) change with respect to the polarity of the external magnetic field (H) applied to the hard axis (HA) of the SPFLs and TMR ratios of over 200%, which is much higher than those of the single-SPFL sensors, where one side of the ferromagnetic layers is an SPFL and the other side is a strongly pinned reference layer. When the applied H exhibits an angular misalignment from the HA, dual-SPFL sensors show much-reduced asymmetry in the R–H curves than single-SPFL sensors. Macrospin simulations of the magnetization behavior and R–H curve for both dual- and single-SPFL sensors revealed that the small asymmetry in the R–H curves of dual-SPFL sensors was owing to their significantly smaller dependence of relative magnetization angle between the SPFLs on the magnetic field misalignment from the HA. These results suggest that dual-SPFL TMR sensors are promising for use in magnetic sensors such as encoder sensors for position and rotation detections.

Anomalous Second Harmonic Generation from Atomically Thin MnBi2Te4

MnBi2Te4 is a van der Waals topological insulator with intrinsic intralayer ferromagnetic exchange and A-type antiferromagnetic interlayer coupling. Theoretically, it belongs to a class of structurally centrosymmetric crystals whose layered antiferromagnetic order breaks inversion symmetry for even layer numbers, making optical second harmonic generation (SHG) an ideal probe of the coupling between the crystal and magnetic structures. Here, we perform magnetic field and temperature-dependent SHG measurements on MnBi2Te4 flakes ranging from bulk to monolayer thickness. We find that the dominant SHG signal from MnBi2Te4 is unexpectedly unrelated to both magnetic state and layer number. We suggest that surface SHG is the likely source of the observed strong SHG, whose symmetry matches that of the MnBi2Te4-vacuum interface. Our results highlight the importance of considering the surface contribution to inversion symmetry-breaking in van der Waals centrosymmetric magnets.

Engineering Spin Configurations of Synthetic Antiferromagnet by Controlling Long-Range Oscillatory Interlayer Coupling and Neighboring Ferrimagnetic Coupling.

Controllable manipulation of specific spin configurations of magnetic materials is the key to constructing functional spintronic devices. Here, it is demonstrated by integrating the merits of ferromagnetic, ferrimagnetic, and antiferromagnetic spin configurations into one synthetic antiferromagnetic (SAF) heterostructure by controlling both long-range oscillatory interlayer coupling and neighboring ferrimagnetic coupling. A controllable manipulation of four types of spin configurations of the Pt/[Co/Pt/Co]/Ru/CoTb SAF heterostructures composed of ferromagnetic Co/Pt/Co and ferrimagnetic CoTb layers is successfully achieved. In particular, the compensated magnetization, enhanced anomalous Hall resistance in the remanence state, wide-temperature spin-orbit torque switching of magnetization, and high immunity to the external magnetic field are simultaneously obtained in one of the SAF heterojunctions with macroscopic interlayer antiferromagnetic coupling. This design concept of engineering spin configurations may enable efficient spin manipulation for customized memory and logic applications.