Search Results (33)

The heteroleptic halogen-substituted Fe³⁺ complex of formula [FeL₂Bipy]Cl, where L is 1-(4-fluoro-phenyl)-3-(4-bromo-phenyl)-propane-1,3-dione and Bipy is 2,2′-bipyridine, was synthesized, and its optic and magnetic properties were studied. Magnetic measurements showed that the complex at high temperatures (T > 75 K) is predominantly in the high-spin (HS) state of Fe³⁺ ions (S = 5/2, γ_HS¹ = 93%) with a small admixture of low-spin (LS) state (S = 1/2, γ_LS¹ = 7%). At T* ≈ 46 K, a partial spin-crossover transition (SCO, 5/2↔1/2) occurs. This process is accompanied not only by a change in the magnetic state (γ_HS² = 76%, γ_LS² = 24%), but also by the appearance of AFM interactions (θ_II = −2.3 K) between neighboring Fe³⁺ ions. A theoretical model was proposed to describe magnetic susceptibility, χ(T). As a result of the analysis of the ground spin state M(H) at 2.0 K, it was established that the majority of the LS states, as well as part of the HS states of Fe³⁺ ions (γ_HS ~ 53%), do not participate in exchange interactions. EPR studies confirmed the presence of HS and LS Fe³⁺ centers and made it possible to isolate I-type and II-type HS centers, corresponding to strong low-symmetry and weak distorted octahedral fields. SCO was also detected and the temperature dependences of the EPR intensities, I(T), of the HS and LS centers were analyzed. Full article

In this study, we suggest a method to amplify spin waves (SWs) in antiferromagnets (AFMs). By introducing a non-uniform Dzyaloshinskii–Moriya (DM) interaction, the potential barrier forms a resonant cavity. SWs with an opposite chirality undergo scattering and are resonantly amplified at a phase-matching condition. The calculation is performed in the insulating AFMs where the electric-field-induced DM interaction and pseudo-dipole anisotropy broaden the parabolic-like SW band for multiple resonant modes. Using a transfer matrix method, we also show numerically that scattering between SWs contributes significantly to the SW amplification. Since the electric field selectively amplifies the SWs with resonant frequencies, the proposed device works as an SW transistor and rectifier. This finding will contribute to insulating AFM-based magnon devices where Joule heating is, in principle, avoided. Full article

Two-dimensional (2D) ferromagnetic semiconductors (FM SCs) provide an ideal platform for the development of quantum information technology in nanoscale devices. However, many developed 2D FM materials present a very low Curie temperature (T_C), greatly limiting their application in spintronic devices. In this work, we predict two stable 2D transition metal chalcogenides, V₃Se₃X₂ (X = S, Te) monolayers, by using first-principles calculations. Our results show that the V₃Se₃Te₂ monolayer is a robust bipolar magnetic SC with a moderate bandgap of 0.53 eV, while V₃Se₃S₂ is a direct band-gap FM SC with a bandgap of 0.59 eV. Interestingly, the ferromagnetisms of both monolayers are robust due to the V–S/Se/Te–V superexchange interaction, and T_Cs are about 406 K and 301 K, respectively. Applying biaxial strains, the FM SC to antiferromagnetic (AFM) SC transition is revealed at 5% and 3% of biaxial tensile strain. In addition, their high mechanical, dynamical, and thermal stabilities are further verified by phonon dispersion calculations and ab initio molecular dynamics (AIMD) calculations. Their outstanding attributes render the V₃Se₃Y₂ (Y = S, Te) monolayers promising candidates as 2D FM SCs for a wide range of applications. Full article

The branched complexes of Schiff bases with various iron(III) salts, named G2-[L₂Fe]⁺A⁻ (A⁻ is NO₃⁻, Cl⁻, PF₆⁻), were synthesized using the condensation reaction between carbazole derivatives of salicylic aldehyde and N’-ethylethylenediamine and characterized by various spectroscopic methods (GPC, IR, ¹H NMR, UV/Vis). The studies revealed that the coordination of the two ligand molecules to metal occurs through the nitrogen ions and oxygen atom of azomethine to form a homoleptic system. All the synthesized coordination compounds were examined for their thermal, optical, and magnetic features. Static magnetic measurements showed that only G2-[L₂Fe]Cl was in a single-phase HS state, whereas the Fe(III) ions of G2-[L₂Fe]NO₃ and G2-[L₂Fe]PF₆ at room temperatures were in mixed low-spin (LS, S = 1/2) and high-spin (HS, S = 5/2) states: 58.9% LS/41.1% HS for G2-[L₂Fe]NO₃, 56.1% LS and 43.9% HS for G2-[L₂Fe]PF₆. All G2-[L₂Fe]⁺A⁻ complexes demonstrate antiferromagnetic exchange interactions between neighboring Fe(III) ions. The ground spin state at 2.0 K revealed a Brillouin contribution from non-interacting LS ions and a proportion of the HS Fe(III) ions not participating in AFM interactions: 57%, 18%, and 16% for G2-[L₂Fe]Cl, G2-[L₂Fe]NO₃ and G2-[L₂Fe]PF₆, respectively. EPR measurements confirmed the presence of magnetically active HS and LS states of Fe(III) ions and made it possible to distinguish two HS types-with strong low-symmetry (I-type) and weak, distorted octahedral environments (II-type). It was shown that G2-[L₂Fe]⁺A⁻ complexes are magnetically inhomogeneous and consist of two magnetic sub-lattices: AFM-correlated chains in layers from the I-type HS Fe(III) centers and dynamic short-range AFM ordered LS/II-type HS Fe(III) centers in the paramagnetic phase located between the layers. Full article

In this theoretical study, we investigate the effect of electron correlations on the electronic structure and magnetic properties of the full Heusler alloy Mn${}_2$NiAl in the framework of first-principles calculations. We investigate the electron correlation effect as employed within hybrid functional (HSE) and also within the DFT+U method with varied values of parameters between 0.9 and 6 eV. The XA-crystal structure was investigated with antiferromagnetic orderings of the magnetic moments of the manganese. It was found that with a growth of the Coulomb interaction parameter, the manganese ions magnetic moment increases, and it reaches the value of 4.15–4.46 ${\mu }_B$ per Mn. In addition, the total magnetic moment decreases because of the AFM ordering of the Mn ions and a small magnetic moment of Ni. The calculated total magnetic value agrees well with recent experiments demonstrating a low value of magnetization. This experimental value is most closely reproduced for the moderate values of the Coulomb parameter, also calculated in constrained LDA, while previous DFT studies substantially overestimated this value. It is also worth noticing that for all values of the Coulomb interaction parameter, this compound remains metallic in its electronic structure in agreement with transport measurements. Full article

We present detailed first-principles density functional theory-based studies on RbRE₂Fe₄As₄O₂ (RE = Sm, Tb, Dy, Ho) hybrid 12442-type iron-based superconducting compounds with particular emphasis on competing magnetic interactions and their effect on possible magneto-structural coupling and electronic structure. The stripe antiferromagnetic (sAFM) pattern across the xy plane emerges as the most favorable spin configuration for all the four compounds, with close competition among the different magnetic orders along the z-axis. The structural parameters, including arsenic heights, Fe-As-Fe angle, and other relevant factors that influence superconducting T${}_c$ and properties, closely match the experimental values in stripe antiferromagnetic arrangement of Fe spins. Geometry optimization with inclusion of explicit magnetic ordering predicts a spin–lattice coupling for all the four compounds, where a weak magneto–structural transition, a tetragonal-to-orthorhombic structural transition, takes place in the relaxed stripe antiferromagnetic spin configuration. Absence of any experimental evidence of such structural transition is possibly an indication of nematic transition in RE-12442 compounds. As a result of structural distortion, the lattice contracts (expands) along the direction with parallel (anti-parallel) alignment of Fe spins. Introduction of stripe antiferromagnetic order in Fe sub-lattice reconstructs the low-energy band structure, which results in significantly reduced number of bands crossing the Fermi level. Moreover, the dispersion of bands and their orbital characteristics also are severely modified in the stripe antiferromagnetic phase similar to BaFe${}_2$As${}_2$. Calculations of exchange parameters were performed for all the four compounds. Exchange coupling along the anti-parallel alignment of Fe spins J${}_{1a}$ is larger than that for the parallel aligned spins J${}_{1b}$. A crossover between the super-exchange-driven in-plane next-nearest-neighbor exchange coupling J${}_2$ and in-plane exchange coupling J${}_{1a}$ due to lanthanide substitution was found. A large super-exchange-driven next-nearest-neighbor exchange interaction is justified using the construction of 32 maximally localized Wannier functions, where the nearest-neighbor Fe-As hopping amplitudes were found to be larger than the nearest- and the next-nearest-neighbor Fe-Fe hopping amplitudes. We compare the hopping parameters in the stripe antiferromagnetic pattern with non-magnetic configuration, and increased hopping amplitude was found along the anti-parallel spin alignment with more majority-spin electrons in Fe d${}_{xz}$ and d${}_{xy}$ but not in Fe d${}_{yz}$. On the other hand, the hopping amplitudes are increased in stripe antiferromagnetic phase along the parallel spin alignment with more majority-spin electrons in only Fe d${}_{yz}$. This difference in hopping amplitudes in the stripe antiferromagnetic order enables more isotropic hopping. Full article

We report a possible coexistence of nontrivial topology and antiferromagnetism in the newly discovered compounds EuCdBi${}_2$, with magnetic Eu layer locating above and below Bi square net. The X-ray diffraction on single crystals and powder indicats that this 112-type material crystalizes in space group of $I4/mmm$, the same as SrMnBi${}_2$ and EuMnBi${}_2$. Our combined measurements of magnetization, electrical transport and specific heat consistently reveal antiferromagnetic (AFM) transition of Eu${}^{2+}$ moments at $T_N$ = 20 K. The Eu moments are not saturated under a field of 7 T at 1.8 K. The anisotropic susceptibility suggests the Eu moments lie in the $ab$ plane, and a metamagnetic (MM) transition is observed near 1 T below $T_N$. Large positive magnetoresistance (MR) present for both $H\Vert ab$ and $H\Vert c$, which are considered to contain part contributions from Dirac bands. Hall measurements show the electron-hole compensation effect is prominent above 100 K, with a crossover of Hall resistance from negative to positive values at ∼150 K. The fitted mobility of electrons is as high as 3250 cm${}^2$ V${}^{-1}$ S${}^{-1}$ at 1.8 K. Interestingly, the rapid increase of carrier density and suppression of mobility appear at around $T_N$, indicating non-negligible interaction between Eu moments and electron/hole bands. EuCdBi${}_2$ may provide a new platform to investigate the interplay of topological bands and antiferromagnetic order. Full article

By employing GPU-implemented hybrid Monte Carlo simulations, we study the robustness of the skyrmion lattice phase (SkX) in a frustrated Heisenberg antiferromagnetic (AFM) layer on a triangular lattice with a Dzyaloshinskii–Moriya interaction in the external magnetic field against the presence of lattice imperfections (nonmagnetic impurities) and lattice finiteness. Both features are typical of experimentally accessible magnetic materials and require theoretical investigation. In the pure model of infinite size, SkX is known to be stabilized in a quite wide temperature-field window. We first study the effects of such imperfections on the SkX stability and compare them with those in the nonfrustrated ferromagnetic counterpart. The partial results of this part appeared in the conference proceedings [M. Mohylnaand M. Žukovič, Proceedings of the 36th International ECMS International Conference on Modelling and Simulation, ECMS, 2022]. We further look into whether SkX can also persist in finite clusters, i.e., zero-dimensional systems of nanometric sizes. In general, both the presence of magnetic vacancies as well as the finiteness of the system tend to destabilize any ordering. We show that in the present model, SkX can survive, albeit in a somewhat distorted form, in the impure infinite system up to a fairly large concentration of impurities, and, in the pure finite systems, down to sizes comprising merely tens of particles. Distortion of the SkX phase due to the formation of bimerons, reported in the ferromagnetic model, was not observed in the present frustrated AFM case. Full article

Recently, a series of oxyfluorides, Sr_1−xBa_xFeO₂F with x = 0, 0.25, 0.50, and 0.75 obtained through a novel synthesis route, were characterized by X-ray and neutron powder diffraction (NPD), magnetization measurements, and ⁵⁷Fe Mössbauer spectroscopy (MS). The diffraction data revealed random occupancy of Sr and Ba atoms at the A-cation site, and a statistical distribution of O and F at the anionic sublattice of the perovskite-like structure specified in space group Pm-3m. MS spectra analysis consistently indicated the presence of Fe³⁺ ions at B-site, confirming the Sr_1−xBa_xFeO₂F stoichiometry. Magnetic structure determination from the NPD data at room temperature established G-type antiferromagnetic arrangement in all compositions with Fe³⁺ moments of about 3.5 μB oriented along the c axis. In this study, we present and analyze additional NPD data concerning the low-temperature chemical and magnetic structure of Sr_0.5Ba_0.5FeO₂F (x = 0.5) and SrFeO₂F (x = 0). Basically, the three-dimensional G-type magnetic structure is maintained down to 2 K, where it is fully developed with an ordered magnetic moment of 4.25(5) μ_B/Fe at this temperature for x = 0.5 and 4.14(3) μ_B/Fe for x = 0. The data processing is complemented with a new approach to analyze the temperature dependence of the magnetic order T_N on the lattice parameters, based on the magnetic hyperfine fields extracted from the temperature-dependent MS data. Full article

Band structure and topology of magneto-spin–orbit graphene is investigated using the proposed tight-binding model that incorporates both Rashba and sublattice-resolved collinear exchange couplings in a generic ferrimagnetic (FIM) setting for in-plane and out-of-plane magnetization directions. The resulting band structures were analyzed for possibilities to extract the strengths of exchange and Rashba couplings from experimental spin-resolved ARPES measurements of the valley gaps and $\pi$-state spin-splittings. It was shown that the topologically trivial in-plane FIM situation admits simple expressions for these quantities, whereas the out-of-plane FIM, which admits a nontrivial band topology, is harder to analyze. The obtained topological phase diagrams for the out-of-plane FIM case show that the anomalous Hall conductance is quite stable with respect to the antiferromagnetic (AFM) interaction, which tends to interfere with the QAHE phase; moreover, the topological phase transition has a rather smooth character with respect to the AFM coupling strength. Full article

The martensitic phase transition and exchange bias effect of the Ni-Mn-based ferromagnetic shape memory alloys (FSMAs) Ni₄₅Co₅Mn₃₇In₁₃ (Ni-Co-Mn-In) films are investigated in this paper. The martensitic transformation properties of the Ni-Co-Mn-In alloy target material are manipulated by the process of electric arc melting, melt-fast quenching, and high-temperature thermal pressure. The Ni-Co-Mn-In alloy films with martensite phase transition characteristics are obtained by adjusting deposition parameters on the (001) MgO substrate, which shows a significant exchange bias (EB) effect at different temperatures. With increasing sputtering power and time, the film thickness increases, resulting in a gradual relaxation of the constraints at the interface between the film and the substrate (the interfacial strain decreases as the increase of thin film thickness), which promotes the martensite phase transition. Between zero-field cooling (ZFC) and field-cooled (FC) curve obvious division zone, the decrease of exchange bias field (H_EB) and coercive force field (H_c) with an increase in test temperature is due to ferromagnetic (FM) interaction begins to dominate, resulting in a reduction of antiferromagnetic (AFM) anisotropy at the interface. The maximal H_EB and H_c reach ~465.7 Oe and ~306.9 Oe at 5 K, respectively. The manipulation of the martensitic transformation and EB effect of the Ni-Co-Mn-In alloy films demonstrates potential application in the field of information and spintronics. Full article

Two dinuclear copper(II) complexes with macrocyclic Schiff bases K1 and K2 were prepared by the template reaction of (R)-(+)-1,1′-binaphthalene-2,2′-diamine and 2-hydroxy-5-methyl-1,3-benzenedicarboxaldehyde K1, or 4-tert-butyl-2,6-diformylphenol K2 with copper(II) chloride dihydrate. The compounds were characterized by spectroscopic methods. X-ray crystal structure determination and DFT calculations confirmed their geometry in solution and in the solid phase. Moreover, intermolecular interactions in the crystal structure of K2 were analyzed using 3D Hirshfeld surfaces and the related 2D fingerprint plots. The magnetic study revealed very strong antiferromagnetic Cu^II-Cu^II exchange interactions, which were supported by magneto-structural correlation and DFT calculations conducted within a broken symmetry (BS) framework. Complexes K1 and K2 exhibited luminescent properties that may be of great importance in the search for new OLEDs. Both K1 and K2 complexes showed emissions in the range of 392–424 nm in solutions at various polarities. Thin materials of the studied compounds were deposited on Si(111) by the spin-coating method or by thermal vapor deposition and studied by scanning electron microscopy (SEM/EDS), atomic force microscopy (AFM), and fluorescence spectroscopy. The thermally deposited K1 and K2 materials showed high fluorescence intensity in the range of 318–531 nm for K1/Si and 326–472 nm for the K2/Si material, indicating that they could be used in optical devices. Full article

Haldane conjectures the fundamental difference in the energy spectrum of the Heisenberg antiferromagnetic (HAF) of the spin S chain is that the half-integer and the integer S chain have gapless and gapped energy spectrums, respectively. The ground state (gs) of the HAF spin-1/2 and spin-1 chains have a quasi-long-range and short-range correlation, respectively. We study the effect of the exchange interaction between an HAF spin-1/2 and an HAF spin-1 chain forming a normal ladder system and its gs properties. The inter-chain exchange interaction $J_{\perp }$ can be either ferromagnetic (FM) or antiferromagnetic (AFM). Using the density matrix renormalization group method, we show that in the weak AFM/FM coupling limit of $J_{\perp }$, the system behaves like two decoupled chains. However, in the large AFM $J_{\perp }$ limit, the whole system can be visualized as weakly coupled spin-1/2 and spin-1 pairs which behave like an effective spin-1/2 HAF chain. In the large FM $J_{\perp }$ limit, coupled spin-1/2 and spin-1 pairs can form pseudo spin-3/2 and the whole system behaves like an effective spin-3/2 HAF chain. We also derive the effective model Hamiltonian in both strong FM and AFM rung exchange coupling limits. Full article

New Gd³⁺- and Mn²⁺-co-doped calcium molybdato-tungstates with the chemical formula of Ca_1−3x−yMn_y▯_xGd_2x(MoO₄)_1−3x(WO₄)_3x (labeled later as CaMnGdMoWO), where ▯ denotes vacant sites in the crystal lattice, 0 < x ≤ 0.2500 and y = 0.0200 as well as 0 < y ≤ 0.0667 and x = 0.1667 were successfully synthesized by high-temperature solid-state reaction method and combustion route. Obtained ceramic materials crystallize in scheelite-type structure with space group I4₁/a. Morphological features and grain sizes of powders under study were investigated by SEM technique. Spectroscopic studies within the UV-vis spectral range were carried out to estimate the direct band gap (E_g) and Urbach energy (E_U) of obtained powders. EPR studies confirmed the existence of two types of magnetic objects, i.e., Mn²⁺ and Gd³⁺ ions, and significant antiferromagnetic (AFM) interactions among them. Full article

In the last decade, Fe₂Mo₃O₈ was recognized for a giant magnetoelectric effect, the origin of which is still not clear. In the present paper, we contribute to the microscopic theory of the magnetoelectric coupling in this compound. Using crystal field theory and the molecular field approximation, we calculated the low-lying energy spectrum for iron ions and their interaction with electric and magnetic fields. Classical ionic contribution to the electric polarization related to the ionic shifts is also estimated. It is found that the electronic and ionic contributions to the electric polarization are comparable and these mechanisms support each other at $T<T_N$. The suggested electronic mechanism provides insight into the nature of huge jumps in polarization upon phase transitions from paramagnetic (PM) to antiferromagnetic (AFM) and then to ferrimagnetic (FRM) states under an applied external magnetic field as well as the large differential magnetoelectric coefficient. Full article