Ferromagnetic Exchange Research Articles

Dissipative nonlinear dynamics of ferromagnetic bilayer

Within the framework of the classical Landau–Lifshitz equations with damping in the Landau form, the relaxation of highly excited magnetic multilayers, consisting of two ferromagnetic layers with magnetic anisotropy of the easy plane type and ferromagnetic exchange interaction between the layers, is analytically and numerically studied. It is shown that the relaxation of the energy and magnetization of the system is of a non-trivial behavior. In the region of strong excitation of the system, the time dependence of the magnetization is non-monotonic, and the smooth time dependencies of energy and magnetization are superimposed by oscillations associated with the essentially nonlinear dynamics of the magnetization vectors in the layers.

Supramolecular Spin Chains via Radical-Radical Contacts Stabilizing Ferromagnetic Interactions between Heisenberg or Ising-like Spins.

A new paramagnetic ligand, 4-(2'-4-(2''-furyl)-pyrimidyl)-1,2,3,5-dithiadiazolyl (furylpymDTDA) and three transition metal coordination complexes, M(hfac)2(furylpymDTDA) M = Mn, Co, Ni; hfac = 1,1,1,5,5,5-hexafluoroacetylacetonato-), are reported. The solid-state structures are influenced by the geometry of the coordination sphere of the M(II) centers: trigonal (Mn) vs. octahedral (Co and Ni). While the hs-Mn(II) complex exhibits pairwise multi-centre 2-electron bonds (i.e., pancake bonds) between the planar π radical DTDA moieties, the hs-Co(II) and Ni(II) complexes crystallize with close contacts between coordinated furylpymDTDA radical ligands that define linear 1D arrays of molecular units. The magnetic data for the hs-Co(II) and Ni(II) complexes indicate ferromagnetic (FM) interactions between molecular units, apparently mediated by radical-radical contacts along the supramolecular chains. Computational analysis suggests proximity between regions of large α- and β-spin density on neighbouring molecular sites enabling FM exchange, in accordance with the McConnell I mechanism. The magnetic data for the Ni(II) complex are consistent with a Heisenberg spin chain, whereas the hs-Co(II) complex exhibits Ising-like spin chain behaviour and a magnetic phase transition to an FM ordered state at 4.6 K.

Magnetic Excitations in Ferromagnetically Coupled Spin‐1 Nanographenes

In the pursuit of high‐spin building blocks for the formation of covalently bonded 1D or 2D materials with controlled magnetic interactions, $\pi$‐electron magnetism offers an ideal framework to engineer ferromagnetic interactions between nanographenes. As a first step in this direction, we explore the spin properties of ferromagnetically coupled triangulenes ‐‐ triangular nanographenes with spin $S = 1$. By combining in‐solution synthesis of rationally designed molecular precursors with on‐surface synthesis, we successfully achieve covalently bonded $S = 2$ triangulene dimers and $S = 3$ trimers on Au(111). Starting with the triangulene dimer, we meticulously characterize its low‐energy magnetic excitations using inelastic electron tunneling spectroscopy (IETS). IETS reveals conductance steps corresponding to a quintet‐to‐triplet excitation, and a zero‐bias peak resulting from higher‐order spin‐spin scattering of the five‐fold degenerate ferromagnetic ground state. The Heisenberg model captures the key parameters of inter‐triangulene ferromagnetic exchange, and its successful extension to the larger $S = 3$ system validates the model's accuracy. We anticipate that incorporating ferromagnetically coupled building blocks into the repertoire of magnetic nanographenes will unlock new possibilities for designing carbon nanomaterials with complex magnetic ground states.

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.

Antiferromagnetic to ferromagnetic phase transition as a transition to partial ordered spins. Application to La1−xCaxMnO3 in the doping range x ≥ 0.50

Magnetic state is a partial ordered state if only part of the electrons in the system give contribution to the magnetic order. We study Heisenberg model of two sublattice spin system, on the body-centered cubic lattice, with antiferromagnetic nearest neighbors exchange of sublattice A and B spins and two different ferromagnetic exchange constants for sublattice A (JA) and B (JB) spins. When JA>JB the system undergoes transition from paramagnetism to ferromagnetism at Curie temperature TC. Only the sublattice A spins give contribution to the magnetization of the system. Upon cooling, the system possesses ferromagnetism to antiferromagnetism transition at Néel temperature TN<TC. Below TN sublattice A and B electrons give contribution to the magnetization. The transition is a partial ordered transition. There is thermodynamic evidence for this transition in the magnetic specific heat of the system. As a function of temperature there are two maxima. At high temperature TC it is λ-type. At lower temperature TN it characterizes the transition from ferromagnetism to antiferromagnetism. As an example of ferromagnetism to antiferromagnetism partial ordered transition we consider the material La1−xCaxMnO3 in the doping range x≥0.50. Our calculations reproduce the experimental magnetization-temperature curve.

Investigation of the electronic, optical and magnetic properties of a novel two-dimensional lead-free perovskite: High visible-light absorption and long-range magnetic ordering.

Recently, big issues that need to be solved in photovoltaic solar cells area are the toxicity and instability of lead halide perovskites which have shown exceptional photoelectric performances. Herein, we report the synthesis and physico-chemical characterization of a novel two-dimensional (2D) lead-free perovskite. The 2D Cu(II)-based perovskite (C4N3H16)[CuCl4]∙Cl was successfully stabilized by the slow evaporation method under room temperature. The X-ray diffraction shows a layered structure with an inorganic network formed by four corners sharing CuCl6 octahedra. The UV-Vis absorption analysis confirms the manifestation of the cooperative Jahn-Teller effect around the Cu(II) ions. In addition to the ligand-to-metal charge transfer transitions, crystal field transitions (d-d) enhance the visible-light absorbance and make the material suitable for green solar cell applications with a band gap energy of 2.17 eV. The thermal analysis revealed the thermal stability of (C4N3H16)[CuCl4]∙Cl. Magnetic measurements revealed the presence of dominant ferromagnetic exchange interactions with J/kB = 22.85 K within the 2d planes, with a weak antiferromagnetic exchange interaction yielding a long-range magnetic ordering at 12 K.

Kinetic ferromagnetism and topological magnons of the hole-doped Kitaev spin liquid

We study the effect of hole doping on the Kitaev spin liquid (KSL) and find that for ferromagnetic (FM) Kitaev exchange K the system is very susceptible to the formation of a FM spin polarization. Through density matrix renormalization group simulations on finite systems, we uncover that the introduction of a single hole, corresponding to ≈1% hole doping for the system size we consider, with a hopping strength of just t ~ 0.28K is enough to disrupt fractionalization and polarize the spins in the [001] direction due to an order-by-disorder mechanism. Taking into account a material relevant FM anisotropic exchange Γ drives the polarization towards the [111] direction via a transition into a topological FM state with chiral magnon excitations. We develop a parton mean-field theory incorporating fermionic holons and bosonic magnons, which accounts for the doping induced FM phases and topological magnon excitations. We discuss experimental implications for Kitaev candidate materials.

Shot noise and tunneling magnetoresistance in silicene-based ferromagnet/antiferromagnet/ferromagnet/p-wave superconductor junctions

We investigate the transport properties in silicene-based ferromagnet/antiferromagnet/ferromagnet/p-wave superconductor junctions within the Blonder–Tinkham–Klapwijk formalism by solving the Dirac–Bogoliubov-de Gennes equation. The results show that the conductance and the shot noise strongly depend on the p-wave superconducting pair potentials and the magnetic configurations of the ferromagnetic regions. The simultaneous diminution of the conductance and enhancement of the shot noise can be achieved with the increase of the antiferromagnetic exchange field strength. The conductance and the shot noise can be effectively modulated by the external electric field and the ferromagnetic exchange field strength, and the corresponding switch effects are also achieved. The tunneling magnetoresistance (TMR) outside the subgap energy interval is always larger than the one obtained in the subgap energy interval. When the antiferromagnetic exchange field strength is large enough, a larger TMR can be obtained by tuning the external electric field.

Enhanced magnetic refrigeration capacities of Er6FeSb2 by manganese substitution

Er6FeSb2 is a potential magnetic refrigeration material that can work at the liquid hydrogen temperature range. This work enhances the magnetic refrigeration performance of Er6Fe1-xMnxSb2 by Mn substitution. Mn doping increases the cell volume while maintaining the compound’s crystal structure type. It also results in an increase in the charge density distribution between Er1 and Fe/Mn. As the Mn content increases, the ferromagnetic exchange is enhanced, and the TC continuously increases. The Mn doping induces spin reorientation at low temperature, transforming compounds from traditional magnetocaloric effects to table-like magnetocaloric effects, greatly enlarge the cooling temperature range. When the content of Mn increases from x = 0 to x = 0.3, the δTFWHM increases from 26 K to 62 K, the −(ΔSM)max decreases from 12.1 J/(kg·K) to 5.9 J/(kg·K), and the RCP first increases and then decreases, reaching the maximum value of 435.0 J/kg at x = 0.2. This study opens a new path for the search of magnetic refrigeration material with large cooling temperature range.

FenB2+2n (n = 1, 2), an intrinsic room temperature ferromagnetic MBene with significant magnetic performance enhancement achievable by carbon substitution

From spintronics to data storage technology, two-dimensional (2D) ferromagnetic materials show great promise for various applications. This work reports a series of stable ferromagnetic transition metal boride FenB2+2n (n = 1, 2), where robust long-range ferromagnetic exchange coupling and large perpendicular magnetic anisotropy energy (MAE) allow the ferromagnetic transition temperature (Tc) of the FenB2+2n monolayer to reach above room temperature. The metallic FenB2+2n exhibits n- and p-type Dirac transport in both spin channels with a high Fermi velocity. Furthermore, the application of biaxial compressive strain and electron doping can greatly increase the ferromagnetic coupling and MAE of FeB4 monolayers. On this basis, the FeB2C2 alloy with a high concentration of carbon substitution has been designed, which allows the nonvolatile integration of in-plane compressive strain and electron doping. As expected, this substitution doping resulted in a significant increase in the Tc and MAE of the system. Our findings provide perspectives for the study of 2D magnetic materials.

A Monte Carlo study of Magnetic and thermodynamic behaviors of L[formula omitted] structure like quadrangular frustum pyramid nanoisland

Based on the Monte Carlo simulation, research has been conducted on the magnetic and thermodynamic behaviors of a ferrimagnetic mixed-spin (5/2, 1/2) L10 nanoisland with a like quadrangular frustum pyramid structure. We studied the effects of the magneto-crystal anisotropy and exchange coupling on the magnetization, susceptibility, internal energy, and hysteresis loops. The ferrimagnetic system exhibits more abundant magnetic and thermodynamic behavior than the cubic L10 nanoisland. We found eight saturation values of magnetization, five-loop hysteresis loops, and abrupt transitions in the low-temperature region. In addition, the exchange coupling effect of ferrimagnetism also promotes magnetic properties. Interestingly, in this system, the ferromagnetic exchange coupling (Jaa) and external magnetic field (h) linearly depend on the blocking temperature TB. The hysteresis loops of the system have more magnetization steps, which reflects that it has more ground state spin configurations.

Comparative study on the magnetic properties of Fe-substituted Co2Sn1−x Fe x O4 spinel oxides and its exchange bias effect

Herein, we report the Fe-substituted Co2Sn1−x Fe x O4 (0 ⩽ x ⩽ 0.4) inverse spinel’s oxide using the solid-state reaction method. X-ray reveals the single-phase cubic structure with space group Fd3m. With increasing Fe in Co2Sn1−x Fe x O4 spinel oxide, the transition temperature rise. The ac susceptibility at different frequencies also confirms a spin-glassy state at lower temperatures. The strong exchange bias effect appears in the sample having Fe substitution (x = 0.2) under the presence of constant temperature ∼10 K. The high-temperature susceptibility of Curie-Wise fitting shows that the system changes from antiferromagnetic exchange (x < 0.2) to ferromagnetic exchange (x > 0.2).

Effect of Ferromagnetic Exchange Interaction and Crystalline Anisotropy on a Double-Cubic Spin-½ Spin-1 Ising System with a Free Surface

In this study, we employ Monte Carlo simulations to explore the magnetic characteristics of a double-cubic spin-½ and spin-1 ferromagnetic Ising superlattice system, focusing on the impact of surface exchange coupling, anisotropy, and layer thickness. We implemented free boundary conditions along the dimension with an exposed surface. Our findings illuminate the key role played by surface exchange coupling (JAS), which significantly influences the critical temperature (Tc), underscoring its ability to strengthen ferromagnetic interactions within the system. In contrast, the compensation temperature (Tcomp) exhibits relative stability. Furthermore, we unveil the crucial influence of crystalline anisotropy on Tcomp, with higher anisotropy values leading to its augmentation, while Tc remains unaffected. Moreover, when the number of layers is increased from 11 to 21, a marked rise in Tc is observed, accompanied by a minor increment in Tcomp, particularly evident under negative anisotropy conditions.

Air-Stable Wafer-Scale Ferromagnetic Metallo-Carbon Nitride Monolayer.

The pursuit of robust, long-range magnetic ordering in two-dimensional (2D) materials holds immense promise for driving technological advances. However, achieving this goal remains a grand challenge due to enhanced quantum and thermal fluctuations as well as chemical instability in the 2D limit. While magnetic ordering has been realized in atomically thin flakes of transition metal chalcogenides and metal halides, these materials often suffer from air instability. In contrast, 2D carbon-based materials are stable enough, yet the challenge lies in creating a high density of local magnetic moments and controlling their long-range magnetic ordering. Here, we report a novel wafer-scale synthesis of an air-stable metallo-carbon nitride monolayer (MCN, denoted as MN4/CNx), featuring ultradense single magnetic atoms and exhibiting robust room-temperature ferromagnetism. Under low-pressure chemical vapor deposition conditions, thermal dehydrogenation and polymerization of metal phthalocyanine (MPc) on copper foil at elevated temperature generate a substantial number of nitrogen coordination sites for anchoring magnetic single atoms in monolayer MN4/CNx (where M = Fe, Co, and Ni). The incorporation of densely populating MN4 sites into monolayer MCN networks leads to robust ferromagnetism up to room temperature, enabling the observation of anomalous Hall effects with excellent chemical stability. Detailed electronic structure calculations indicate that the presence of high-density metal sites results in the emergence of spin-split d-bands near the Fermi level, causing a favorable long-range ferromagnetic exchange coupling through direct exchange interactions. Our work demonstrates a novel synthesis approach for wafer-scale MCN monolayers with robust room-temperature ferromagnetism and may shed light on practical electronic and spintronic applications.

Study of the Berezinskii–Kosterlitz–Thouless transition: an unsupervised machine learning approach

The Berezinskii–Kosterlitz–Thouless (BKT) transition in magnetic systems is an intriguing phenomenon, and estimating the BKT transition temperature is a long-standing problem. In this work, we explore anisotropic classical Heisenberg XY and XXZ models with ferromagnetic exchange on a square lattice and antiferromagnetic exchange on a triangular lattice using an unsupervised machine learning approach called principal component analysis (PCA). The earlier PCA studies of the BKT transition temperature ( TBKT ) using the vorticities as input fail to give any conclusive results, whereas, in this work, we show that the proper analysis of the first principal component-temperature curve can estimate TBKT which is consistent with the existing literature. This analysis works well for the anisotropic classical Heisenberg with a ferromagnetic exchange on a square lattice and for frustrated antiferromagnetic exchange on a triangular lattice. The classical anisotropic Heisenberg antiferromagnetic model on the triangular lattice has two close transitions: the TBKT and Ising-like phase transition for chirality at Tc , and it is difficult to separate these transition points. It is also noted that using the PCA method and manipulation of their first principal component not only makes the separation of transition points possible but also determines transition temperature.

Large magnetocaloric refrigeration performance near room temperature in monolayer transition metal dihalides

Magnetocaloric effect (MCE) exhibits highly efficient and ecological cooling abilities for solid-state refrigeration in contrast to traditional vapor-compression refrigeration. Successive emerging two-dimensional (2D) magnetic materials provide a fertile platform for exploring low-dimensional MCE systems. Here, we focus on a series of 2D transition metal dihalides MX2 (M = Fe, Ru, Os; X = Cl, Br) to explore the maximum isothermal magnetic entropy change (−ΔSmagmax) and adiabatic temperature change (ΔTadmax) under external magnetic field. It is found that FeCl2, FeBr2, and RuCl2 have intrinsically sizable −ΔSmagmax, ΔTadmax, and high thermal conductivity near room temperature, demonstrating superior comprehensive refrigeration performance in comparison with other 2D magnets. It is revealed that strong nearest-neighbor ferromagnetic exchange interaction plays a decisive role in −ΔSmagmax, and the high lattice thermal conductivities of FeCl2 and RuCl2 are attributed to the longer phonon lifetime and larger group velocity of low-frequency acoustic branch. Moreover, moderate strain and carriers doping are able to effectively regulate Curie temperature and magnetocrystalline anisotropy energy and correspondingly enhance −ΔSmagmax. The present work provides important insights for the exploration of 2D magnets for magnetocaloric refrigeration near room temperature.

Critical behavior of the van der Waals ferromagnet Fe4.8GeTe2

The van der Waals ferromagnet Fe5-xGeTe2 has drawn significant interest due to its approximately room-temperature Curie temperature (TC) of 270 to 310 K, which can be regulated through iron deficiency. To comprehend the tunable TC associated with the ferromagnetic exchange mechanism, we systematically investigate the critical phenomenon of Fe5-xGeTe2 (Fe4.8GeTe2) crystals around TC. Employing diverse analytical methods for magnetization study, we derived reliable critical exponent values: TC = 285 K, β = 0.364(2), γ = 1.293(1), and δ = 4.62(1). Through a comparative analysis of these critical exponents, the magnetic behavior of Fe4.8GeTe2 is expounded as a three-dimensional (3D) magnetic exchange mechanism, with exchange distance decay modeled as J(r) ≈ r−4.85, closely resembling long-range magnetic coupling in the 3D Heisenberg mode.

Bimetallic Ba(II)-Cr(III) and trimetallic Ba(II)-Ln(III)-Cr(III) (Ln(III) = Gd, Tb, Dy, Ho, Er, Yb, Y) coordination polymers formed by Cr(III)-containing building blocks with cyclopropane-1,1-dicarboxylate anions

The reaction of chromium(III) nitrate with Ba(cpdc) (H2cpdc = cyclopropane-1,1-dicarboxylic acid) in a ratio of 1:3 yielded a 1D coordination polymer {[Ba2Cr2(OH)2(cpdc)4(H2O)8]·5H2O}n (1) formed by binuclear units [Cr2(OH)2(cpdc)4]4− and a 3D polymer [Ba2Cr(cpdc)3(NO3)(H2O)6]n (2) constructed from tris-chelate blocks [Cr(cpdc)3]3−. The addition of rare-earth metal nitrates (Cr:Ln = 1:2) in this reaction led to the formation of a series of trimetallic 3D coordination polymers {[Ba3Ln2Cr4(cpdc)12(H2O)24]·8H2O}n (3Ln, Ln = Gd, Tb, Dy, Ho, Er, Yb, Y), in whose structures tris-chelate fragments [Cr(cpdc)3]3− are bound in layers by Ln3+ ions and, further, in a framework due to the coordination of Ba2+ ions. The crystal structures of 1, 2, and 3Gd were determined by single-crystal X-ray diffraction (XRD), and isostructurality of all the compounds in the series 3Ln was proved by powder X-ray diffraction (PXRD). DC-magnetic susceptibility measurements revealed weak ferromagnetic exchange interactions between Cr3+ ions in compound 1 (J = +0.74 cm−1). According to ac-magnetic susceptibility measurements, complexes 3Er and 3Y exhibit field-induced slow relaxation of magnetization. According to the data of simultaneous thermal analysis (STA) and differential scanning calorimetry (DSC) performed under Ar atmosphere, dehydration of the compounds obtained takes place in one (for 1 and 3Gd) or three stages (for 2). The initial temperature of the organic part degradation process decreases when moving from compound 1 containing dimerized bis-chelate fragments [Cr2(OH)2(cpdc)4]4− (330 °C) to compounds 2 (276 °C) and 3Gd (261 °C) based on tris-chelate units [Cr(cpdc)3]3−.

Polymeric dichlorido-bridged copper(II) offset stacked dimer coordination compounds and molecular spin stairs

A family of oxygen coordinated dichlorido-bridged n-X-2-pyridone (1, n = 3, X = Cl; 2, n = 3, X = Br; 3, n = 4, X = Cl; 4, n = 4, X = Br; 5, n = 5, X = Cl; 6, n = 5, X = Br) Cu(II) offset stacked dimer compounds, denoted molecular spin stairs, have been prepared and analyzed by single-crystal X-ray diffraction (1–4), powder X-ray diffraction (1–6), and variable temperature magnetic susceptibility measurements (1–6). Ferromagnetism is dominant in all compounds with a weaker antiferromagnetic exchange present in 1–4. The ferromagnetic exchange correlates to increased twist angles which are defined by the extent of the tetrahedral distortion of the copper coordination sphere and the identity of the halogen on the ring. The compounds were qualitatively fit to a ferromagnetic Heisenberg chain model with a Curie-Weiss interchain correction. The general Hamiltonian used is of the form H = − J ∑ S 1 S 2 . The ratio of exchange energies denoted α ( α = J FM | J AFM | ) ranges between 2.6 and 4.7. This family of compounds constitutes possible S = ½ Haldane-like materials.

Macroscopic tunneling probe of Moiré spin textures in twisted CrI3

Various noncollinear spin textures and magnetic phases have been predicted in twisted two-dimensional CrI3 due to competing ferromagnetic (FM) and antiferromagnetic (AFM) interlayer exchange from moiré stacking—with potential spintronic applications even when the underlying material possesses a negligible Dzyaloshinskii–Moriya or dipole–dipole interaction. Recent measurements have shown evidence of coexisting FM and AFM layer order in small-twist-angle CrI3 bilayers and double bilayers. Yet, the nature of the magnetic textures remains unresolved and possibilities for their manipulation and electrical readout are unexplored. Here, we use tunneling magnetoresistance to investigate the collective spin states of twisted double-bilayer CrI3 under both out-of-plane and in-plane magnetic fields together with detailed micromagnetic simulations of domain dynamics based on magnetic circular dichroism. Our results capture hysteretic and anisotropic field evolutions of the magnetic states and we further uncover two distinct non-volatile spin textures (out-of-plane and in-plane domains) at ≈1° twist angle, with a different global tunneling resistance that can be switched by magnetic field.