Search Results (249)

The reaction of Mn(II) salts in the air with different R-salicylaldehyde oximes and the sodium or cesium salts of 9-anthracenecarboxylato (9-AC) allows for the isolation of new six polynuclear compounds: [Mn₃NaO(salox)₃(9-AC)₂(EtOH)₃H₂O]_n·2EtOH (1), [Mn₃NaO(3-Me-salox)₃(9-AC)₂(EtOH)₃H₂O]_n·EtOH (2), [Mn₆O₂(salox)₆(9-AC)₂(EtOH)₂(H₂O)₂]·3EtOH (3), [Mn₃O(3-Me-salox)₃(9-AC)(EtOH)₃(H₂O)]·1.8EtOH·3H₂O (4), [Mn₆O₂(Me-salox)₆(9-AC)₂(EtOH)₄(H₂O)₂]·0.5H₂O (5), and [Mn₆O₂(Et-salox)₆(9-AC)₂(EtOH)₄(H₂O)₂]·3EtOH (6). H₂salox is a salicylaldehyde oxime, H₂(3-Me-salox) is a 3-methyl-salicylaldehyde oxime, H₂Me-salox is a 1-(2-hydroxyphenyl)ethan-1-one oxime and a H₂-Et-salox is 1-(2-hydroxyphenyl)propan-1-one oxime. Structurally, compounds 1 and 2 consist of chains of trinuclear {Mn^III₃(μ₃-O)(salox)₃}⁺ units connected by Na⁺ ions. Compounds 3, 5, and 6 are hexanuclear units formed by two parallel trinuclear units {Mn^III₃(μ₃-O)(salox)₃}⁺ or {Mn^III₃(μ₃-O)(Me-salox)₃}⁺ planes related through an inversion center. Compound 4 consists of two isolated [Mn₃O(3-Me-salox)₃(9-AC)(EtOH)₃(H₂O)] trinuclear molecules in the unit cell showing crystallographic differences. Magnetic studies reveal a set of antiferromagnetic interactions in compounds 1 and 2 and a combination of antiferromagnetic and ferromagnetic interactions in compounds 3, 5, and 6. In all cases, the magneto-structural correlation between the intramolecular Mn^III-N-O-Mn^III torsion angle and the magnetic exchange within these units have been confirmed. For compounds 5 and 6, ac magnetic measurements reveal the slow relaxation of magnetization with moderate energy barriers of 19.9 cm⁻¹ and 31.1 cm⁻¹, respectively. Absorbance and fluorescence measurements in solution show the transitions of the 9-anthracenecarboxylate chromophore for all the compounds. Full article

Employing the spin-wave formalism within and beyond the harmonic-oscillator approx-imation, we study the dynamic structure factors of spin-${\displaystyle \frac{1}{2}}$ nearest-neighbor quantum Heisenberg antiferromagnets on two-dimensional quasiperiodic lattices with particular emphasis on a mag-netic analog to the well-known confined states of a hopping Hamiltonian for independent electrons on a two-dimensional Penrose lattice. We present comprehensive calculations on the C_5v Penrose tiling in comparison with the C_8v Ammann–Beenker tiling, revealing their decagonal and octagonal antiferromagnetic microstructures. Their dynamic spin structure factors both exhibit linear soft modes emergent at magnetic Bragg wavevectors and have nearly or fairly flat scattering bands, signifying magnetic excitations localized in some way, at several different energies in a self-similar manner. In particular, the lowest-lying highly flat mode is distinctive of the Penrose lattice, which is mediated by its unique antiferromagnons confined within tricoordinated sites only, unlike their itinerant electron counterparts involving pentacoordinated, as well as tricoordinated, sites. Bringing harmonic antiferromagnons into higher-order quantum interaction splits, the lowest-lying nearly flat scattering band in two, each mediated by further confined antiferromagnons, which is fully demonstrated and throughly visualized in the perpendicular as well as real spaces. We disclose superconfined antiferromagnons on the two-dimensional Penrose lattice. Full article

The domain wall energy is calculated by the balance between exchange, magnetocrystalline anisotropy and magnetoelastic energy contributions. The described method is theoretical and is based on experimental measurements of neutron inelastic scattering. The domain wall energy is determined by both finding the minimum of energy and deriving the energy and setting it to zero. The determination was undertaken for the discrete case, and this means that the calculation was performed for each plane or atomic layer. This is in contrast with the Bloch wall, which assumes continuum mean. The energy of the Lilley domain wall was discussed. Most of the energy of the Bloch wall was comprised inside the Lilley distance (above 99.9% of the energy). Antiferromagnetic interactions strongly decreased the domain wall energy. The negative terms due to antiferromagnetism must be considered in the Hamiltonian describing the exchange energy terms. The domain wall energy and width of terbium were reassessed. The values varied between 83.7 and 95.2 Kelvin (10.3 to 11.2 ergs/cm²). The domain width was estimated to be 57 Angstroms. It was found that a significant part of the total domain wall energy was concentrated on the planes at the center of the domain wall. Full article

The hexagonal ferrite h-YbFeO₃ grown on YSZ(111) by pulsed laser deposition is foreseen as a promising single multiferroic candidate where ferroelectricity and antiferromagnetism coexist for future applications at low temperatures. We studied in detail the microstructure as well as the temperature dependence of the magnetic properties of the devices by comparing the heterostructures grown directly on YSZ(111) (i.e., YbPt_Th0nm) with h-YbFeO₃ films deposited on substrates buffered with platinum Pt/YSZ(111) and in dependence on the Pt underlayer film thickness (i.e., YbPt_Th10nm, YbPt_Th40nm, YbPt_Th55nm, and YbPt_Th70nm). The goal was to deeply understand the importance of the crystal quality and morphology of the Pt underlayer for the h-YbFeO₃ layer crystal quality, surface morphology, and the resulting physical properties. We demonstrate the relevance of homogeneity, continuity, and hillock formation of the Pt layer for the h-YbFeO₃ microstructure in terms of crystal structure, mosaicity, grain boundaries, and defect distribution. The findings of transmission electron microscopy and X-ray diffraction reciprocal space mapping characterization enable us to conclude that an optimum film thickness for the Pt bottom electrode is Th_Pt = 70 nm, which improves the crystal quality of h-YbFeO₃ films grown on Pt-buffered YSZ(111) in comparison with h-YbFeO₃ films grown on YSZ(111) (i.e., YbPt_Th0nm). The latter shows a disturbance in the crystal structure, in the up-and-down atomic arrangement of the ferroelectric domains, as well as in the Yb–Fe exchange interactions. Therefore, an enhancement in the remanent and in the total magnetization was obtained at low temperatures below 50 K for h-YbFeO₃ films deposited on Pt-buffered substrates Pt/YSZ(111) when the Pt underlayer reached Th_Pt = 70 nm. Full article

A reaction between copper(II) nitrate and trans-1,4-cyclohexanedicarboxylic acid (H₂chdc) carried out under hydrothermal conditions led to a new metal-organic coordination polymer [Cu₂(Hchdc)₂(chdc)]_n. According to single-crystal XRD data, the compound is based on bi-nuclear paddlewheel-type carboxylate blocks that are joined with polymeric chains due to the (μ₃-κ¹:κ²) coordination of carboxylate groups. The chains are interconnected by chdc²⁻ bridging ligands into layers containing free COOH groups of terminal Hchdc⁻. The neighboring layers adopt a RCOOH···OOCR hydrogen bond-assisted arrangement into a dense-packed structure. Magnetization measurements showed the presence of a strong antiferromagnetic exchange interaction (J/k_B = −495 K) inside the bi-nuclear blocks. At the same time, no significant interaction was found between the {-Cu₂(OOCR)₄-} units in spite of their polymeric in-chain packing. Patterns of magnetic behavior of [Cu₂(Hchdc)₂(chdc)]_n were thoroughly analyzed and explained from a structural point of view. Full article

The structural, electronic, and magnetic properties of a novel two-dimensional monolayer material, TaF₄, are investigated using first-principles calculations. The dynamical and thermal stabilities of two-dimensional monolayer TaF₄ were confirmed using its phonon dispersion spectrum and molecular dynamics calculations. The band structure obtained via the high-accuracy HSE06 (Heyd–Scuseria–Ernzerhof 2006) functional theory revealed that monolayer two-dimensional TaF₄ is an indirect bandgap semiconductor with a bandgap width of 2.58 eV. By extracting the exchange interaction intensities and magnetocrystalline anisotropy energy in a J₁-J₂-J₃-K Heisenberg model, it was found that two-dimensional monolayer TaF₄ possesses a Néel-type antiferromagnetic ground state and has a relatively high Néel temperature (208 K) and strong magnetocrystalline anisotropy energy (2.06 meV). These results are verified via the magnon spectrum. Full article

We studied the noncovalent interactions of gadolinium bisphthalocyanine (GdPc₂) with cluster models for graphene and hexagonal boron nitride (hBN) of variable size by using the PBE functional of the generalized gradient approximation in conjunction with Grimme’s dispersion correction and a DND double numerical basis set (that is, PBE-D2/DND). We found that in terms of the bonding strength, changes in the Gd-N bond lengths, the charge and spin of the Gd central ion, and the spin of the GdPc₂ molecule, the behaviors of the graphene- and hBN-based model systems are rather similar. As expected, when increasing the size of the graphene and hBN cluster models, the strength of the interaction with GdPc₂ increases, in which the bonding with the hBN models is usually stronger by a few kcal/mol. One of the main questions addressed in the present work was whether a change in the antiferromagnetic spin alignment to a ferromagnetic one, which is typical for GdPc₂, is (at least theoretically) possible, as it has been observed previously for a number of graphene models when a smaller basis set DN was employed. We found that the use of a larger DND basis set dramatically reduces the occurrence of ferromagnetic adsorption complexes but does not exclude this possibility completely. 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 the present work, we have synthesized rare-earth ion modified Bi_4−xRE_xTi₂Fe0_.7Co_0.3O_12−δ (RE = Dy, Sm, La) multiferroic compounds by the conventional solid-state route. Analysis of X-ray diffraction by Rietveld refinement confirmed the formation of a polycrystalline orthorhombic phase. The morphological features revealed a non-uniform, randomly oriented, plate-like grain structure. The peaks evident in the Raman spectra closely corresponded to those of orthorhombic Aurivillius phases. Dielectric studies and impedance measurements were carried out. Asymmetric complex impedance spectra suggested the relaxation of charge carriers belonging to the non-Debye type and controlled by a thermally activated process. Temperature-dependent AC conductivity data showed a change of slope in the vicinity of the phase transition temperature of both magnetic and electrical coupling natures. Based on the universal law and its exponent nature, one can suppose that the conduction process is governed by a small polaron hopping mechanism but significant distortion of TiO₆ octahedral. The doping of the A-sites with rare-earth element ions and changes in the concentrations of Fe and Co ions located on the B-sites manifested themselves in saturated magnetic hysteresis loops, indicating competitive interactions between ferroelectric and canted antiferromagnetic spins. The magnetic order in the samples is attributed to pair-wise interactions between adjacent Fe³⁺–O–Fe³⁺, Co^2+/3+–O–Co^3+/2+, and Co^2+/3+–O–Fe³⁺ ions or Dzyaloshinskii–Moriya interactions among magnetic ions in the adjacent sub-lattices. As a result, enhanced magnetoelectric coefficients of 42.4 mV/cm-Oe, 30.3 mV/cm-Oe, and 21.6 mV/cm-Oe for Bi_4−xDy_xTi₂Fe0_.7Co_0.3O_12−δ (DBTFC), Bi_4−xLa_xTi₂Fe0_.7Co_0.3O_12−δ (LBTFC), and Bi_4−xSm_xTi₂Fe0_.7Co_0.3O_12−δ (SBTFC), respectively, have been obtained at lower magnetic fields (<3 kOe). The strong coupling of the Aurivillius compounds observed in this study is beneficial to future multiferroic applications. Full article

The mononuclear and dinuclear ruthenium(III) complexes trans-Ph₄P[Ru^III(acac)₂Cl₂] (1), Ph₄P[{Ru^III(acac)Cl}₂(μ-Cl)₃] (2) and trans-Ph₄P[Ru^III(acac)₂(NCS)₂]·0.5C₆H₁₄ (3·0.5C₆H₁₄) were synthesized. Single crystals of 1, 2·H₂O and 3·CH₃CN suitable for X-ray crystal structure analyses were obtained through recrystallization from DMF for 1 and 2·H₂O and from acetonitrile for 3·CH₃CN. An octahedral Ru with bis-chelate-acac ligands and axial chlorido or κ-N-thiocyanido ligands (for 1 and 3·CH₃CN) and triply µ-chlorido-bridged dinuclear Ru₂ for 2·H₂O were confirmed through the structure analyses. The Ru–Ru distance of 2.6661(2) of 2·H₂O is indicative of the existence of the direct metal–metal interaction. The room temperature magnetic moments (μ_eff) are 2.00 and 1.93 μ_B for 1 and 3·0.5C₆H₁₄, respectively, and 0.66 μ_B for 2. The temperature-dependent (2–300 K) magnetic susceptibility showed that the strong antiferromagnetic interaction (J ≤ −800 cm⁻¹) is operative between the ruthenium(III) ions within the dinuclear core. In the ¹H NMR spectra measured in CDCl₃ at 298 K, the dinuclear complex 2 showed signals for the acac ligand protons at 2.50 and 2.39 ppm (for CH₃) and 5.93 ppm (for CH), respectively, while 1 and 3·0.5C₆H₁₄ showed signals with large paramagnetic shifts; −17.59 ppm (for CH₃) and −57.01 ppm (for CH) for 1 and −16.89 and −17.36 ppm (for CH₃) and −53.67 and −55.53 ppm (for CH) for 3·0.5C₆H₁₄. Cyclic voltammograms in CH₂Cl₂ with an electrolyte of ⁿBu₄N(ClO₄) showed the Ru^III → Ru^IV redox wave at 0.23 V (vs. Fc/Fc⁺) for 1 and the Ru^III → Ru^II waves at −1.39 V for 1 and −1.25 V for 3·0.5C₆H₁₄ and the Ru^III–Ru^III → Ru^III–Ru^IV and Ru^III–Ru^III → Ru^III–Ru^IV waves at 0.91 V and −0.79 V for 2. Full article

Based on the proposed microscopic model, we investigate the multiferroic characteristics of VOX₂ (X = Cl, Br, I) monolayers using a Green’s function method. The dependence of the microscopic parameters of the ferroelectric system (pseudo-spin arrangement and flipping rate) on the magnitude and sign of the exchange magnetic interaction along the b-axis and the value of the Dzyaloshinskii–Moria vector have been investigated and qualitatively explained. The possibility of observing a spin-reorientation transition with a change in the character of spin ordering from antiferromagnetic to ferromagnetic is investigated. It is found that the antisymmetric magnetoelectric interaction may be responsible for the spin-reorientation transition without a change in the ordering of magnetic moments. Changing the sign of the exchange magnetic interaction along the b-axis leads to ferromagnetic ordering without observing a spin-reorientation transition. The dependence of isotropic and antisymmetric magnetic interactions on the microscopic parameters of the ferroelectric system is qualitatively explained. A mechanism for the occurrence of the spin-reorientation transition is presented based on the proposed microscopic model. The obtained results qualitatively coincide with Density Functional Theory calculations. Full article

Using the microscopic s-f model and Green’s function theory, we study the temperature dependence of the band gap energy $E_g$ and the phonon energy $\omega$ and damping $\gamma$ of ferro- and antiferromagnetic semiconductors, i.e., with different signs of the s-f interaction constant I. The band gap is a fundamental quantity which affects various optical, electronic and energy applications of the materials. In the temperature dependence of $E_g$ and the phonon spectrum, there is a kink at the phase transition temperature $T_C$ or $T_N$ due to the anharmonic spin–phonon interaction (SPI) R. Moreover, the effect of the SPI R and electron–phonon interaction (EPI) A on these properties is discussed. For $I>0,R>0$, $E_g$ decreases with increasing SPI and EPI, whereas for $I<0,R>0$, there is a competition; $E_g$ increases with raising the EPI and decreases for enhanced SPI. For $R<0$, in both cases, the SPI and EPI reduce $E_g$. The magnetic field dependence of $E_g$ for the two signs of I and R is discussed. The SPI and EPI lead to reducing the energy of the phonon mode $\omega$ = 445 cm⁻¹ in EuO ($I>0$, $R<0$), whereas $\omega$ = 151 cm⁻¹ in EuSe ($I>0$, $R>0$) is enhanced with increasing EPI and reduced with SPI. Both the SPI and EPI lead to an increasing of the phonon damping in EuO and EuSe. The results are compared with the existing experimental data. Full article

We develop a strong coupling approach towards quantum magnetism in Mott insulators for Wannier-obstructed bands. Despite the lack of Wannier orbitals, electrons can still singly occupy a set of exponentially localized but nonorthogonal orbitals to minimize the repulsive interaction energy. We develop a systematic method to establish an effective spin model from the electron Hamiltonian using a diagrammatic approach. The nonorthogonality of the Mott basis gives rise to multiple new channels of spin-exchange (or permutation) interactions beyond Hartree–Fock and superexchange terms. We apply this approach to a Kagome lattice model of interacting electrons in Wannier-obstructed bands (including both Chern bands and fragile topological bands). Due to the orbital nonorthogonality, as parameterized by the nearest-neighbor orbital overlap g, this model exhibits stable ferromagnetism up to a finite bandwidth $W\sim Ug$, where U is the interaction strength. This provides an explanation for the experimentally observed robust ferromagnetism in Wannier-obstructed bands. The effective spin model constructed through our approach also opens up the possibility for frustrated quantum magnetism around the ferromagnet-antiferromagnet crossover in Wannier-obstructed bands. Full article

The exchange coupling between two ferromagnetic thin films, one with magnetically hard and the other with soft phases, separated by a thin non-magnetic layer, is studied. Nd-Fe-B/Ti/Fe thin film heterostructures were fabricated using DC magnetron sputtering on Si substrates, which were heated in situ at 650 °C using a house-built vacuum-compatible heater. The effect of the thickness of the Ti buffer layer and the annealing temperature on the formation of various phases of Nd-Fe-B was investigated. The effect of the thickness of the non-magnetic Ti spacer layer on the exchange coupling strength between the hard phase Nd-Fe-B ferromagnetic thin layer and the soft phase transition metal Fe layer was experimentally investigated. Hysteresis loops of multilayer thin films indicate an antiferromagnetic coupling was observed when the thickness of the spacer layer was 2 nm. This is within the range of an antiferromagnetic coupling calculation based on RKKY theory predictions. Full article

The t-J model remains an indispensable construct in high-temperature superconductivity research, bridging the gap between charge dynamics and spin interactions within antiferromagnetic matrices. This study employs the multiple Davydov Ansatz method with thermo-field dynamics to dissect the zero-temperature and finite-temperature behaviors. We uncover the nuanced dependence of hole and spin deviation dynamics on the spin–spin coupling parameter J, revealing a thermally-activated landscape where hole mobilities and spin deviations exhibit a distinct temperature-dependent relationship. This numerically accurate thermal perspective augments our understanding of charge and spin dynamics in an antiferromagnet. Full article