Unusual Magnetic Behavior Research Articles

Unusual Optical, Electric, and Magnetic Behaviors of OLEDs due to Exothermic/Endothermic Dexter-Energy-Transfer and Fusion Channels of Hot/Cold Triplet Excitons

Unusual Optical, Electric, and Magnetic Behaviors of OLEDs due to Exothermic/Endothermic Dexter-Energy-Transfer and Fusion Channels of Hot/Cold Triplet Excitons

Unusual magnetic behavior in Dy-doped LuFe0.5Cr0·5O3 perovskite ceramics

In this paper, polycrystalline Lu1-xDyxFe0.5Cr0·5O3 (0≤x≤0.15) perovskite ceramics were synthesized via a conventional solid-state-reaction technique. Structural and magnetic properties of the samples were experimentally studied. The cell volume of the lattice expands with the rise in Dy3+ amount. The measuring of magnetic properties shows that the undoped sample exhibits a negative magnetization effect with a compensation temperature of 231.1 K, while the Dy-doped samples display negative magnetization effects between two compensation temperatures. The magnetic switch experiment demonstrates the significant potential for practical applications through stable and repeatable switching of magnetization state by adjusting the external magnetic field between 50 Oe and 300 Oe. Besides, the presence of two compensation temperatures which can be regulated by changing the doping content or external magnetic field provides more possibilities for application. Moreover, based on the comprehensive analysis of the experimental results, it is believed that the negative magnetization effect originates from the competition of magnetic moments in different directions. Meanwhile, the second compensation temperature occurs in low temperature region might be attributed to the additional positive magnetic moment contributed by the paramagnetic Dy3+ ions.

Unusual magnetic behavior of cubic double perovskite Ba2YIrO6 with Ir5+(5d 4) ions

Using density functional calculations, we investigate the electronic structure and magnetism of double-perovskite Ba2YIrO6 to explore the origin of its unusual magnetic behavior. Our results show that the breakdown of expected j = 0 nonmagnetic state of Ir5+(5d 4) in Ba2YIrO6 is induced by both bandwidth and exchange interaction. In addition, the bandwidth effect makes the system behave like metal, while the antiferromagnetic interaction between Ir ions should be responsible for the insulator behavior. Moreover, the strong geometrical frustration in Ir triangular unit prevents the formation of long-range magnetic order.

Field induced metamagnetic transition and mixed charge transfer Mott-Hubbard character in nanocrystalline FeCo2O4 spinel oxide: A combined study using experimental and first principles techniques

Unusual magnetic behavior of nanocrystalline FeCo2O4 (FCO) has been observed at different annealing temperatures. FCO nanoparticles have been prepared by co-precipitation method and the prepared sample annealed at different temperatures to vary its crystallite size. The powder x-ray diffraction analysis confirms the presence of pure spinel phase in the samples annealed at 900 ℃ and 1000℃. The increase in particle size with annealing temperature has been confirmed by field emission scanning electron microscopy (FESEM) analysis. High resolution x-ray photoelectron spectroscopy (HRXPS) analysis reveals the presence of mixed oxidation states of Fe+2/ Fe+3 and Co+3/Co+2 in the sample annealed at 900℃. The as-synthesized sample at 80 °C shows strong antiferromagnetic behavior due to their smaller particle size, but all the annealed samples have strong ferromagnetic behavior with large coercive field and remanence due to their larger particle size. We have observed a sharp rise in magnetization near small field values in the virgin curve and also the presence of virgin curve completely outside the main hysteresis loop in the M(H) curves measured at 5 K for the samples annealed at and above 1000 ℃ reveal the characteristic of first order nature of field induced metamagnetic transition. Structural parameters obtained after Rietveld refinement of powder x-ray diffraction pattern for sample annealed at 900 ℃ have been used for investigating the magnetic properties using first principles density functional theory. Our calculations using hybrid exchange-correlation functional, HSE06 captures the correct insulating ferromagnetic ground state and band gap for inverse spinel structure in broad agreement with our experimental results while calculations within GGA+U leads to a wrong half metallic ferromagnetic ground state. The partial density of states obtained for inverse spinel structure with HSE06 functional suggests a mixed charge transfer and Mott-Hubbard character in our system. We have explored the interplay among structural, magnetic and transport properties of FCO using experiment as well as first principles density functional theory.

Paramagnetic two-dimensional silicon-oxide from natural silicates

Silicon dioxide’s potential for having magnetic properties is fascinating, as combining its electronic capabilities with magnetic response seems promising for spintronics. In this work, the mechanisms that drive the change from diamagnetic behavior in pure silicates like SiO2 to paramagnetic behavior in transition metal-doped silicates like Rhodonite silicate (CaMn3Mn(Si5O15)) are explored. This naturally occurring Rhodonite (R)-silicate was thinned down while retaining its magnetic properties by liquid-phase scalable exfoliation. Exfoliating R-silicate into the two-dimensional (2D) structure by LPE increases magnetic coercivity, and the internal resistance to demagnetization (ΔHc) up to ∼23.95 Oe compared to 7.08 Oe for its bulk phase. DFT spin-polarized calculations corroborate those findings and explain that the origin of the magnetic moment comes mainly from the Mn in the doped 2D silicate due to the asymmetrical components of the Mn d and Si p states in the valence band. This result is further illustrated by the spin component differential charge densities showing that Mn and Si atoms display a residual up spin charge. Rhodonite’s unusual magnetic behavior has considerable potential for spintronics, data storage, and sensing technologies. Understanding the complex relationships between the structural, magnetic, and electronic properties of silicates is essential for developing new materials and composites as well as for driving future research.

Erbium-Excess Gallium Garnets.

A series of garnets of formula Er3+xGa5-xO12 are described, for which we report the crystal structures for both polycrystalline and single-crystal samples. The x limit in the garnet phase is between 0.5 and 0.6 under our conditions, with the Er fully occupying the dodecahedral (24c) garnet site plus some of the octahedral site (16a) in place of the Ga normally present. Long-range antiferromagnetic order with spin-ice-like frustration is suggested by the transition temperature (TN ≈ 0.8 K) being lower than the Curie-Weiss theta. The magnetic ordering temperature does not depend on the Er excess, but there is increasing residual entropy as the Er excess is increased, highlighting the potential for unusual magnetic behavior in this system. The field-dependent magnetic entropy trend is consistent with the reported behavior for frustrated triangular magnetic systems: an increasing transition temperature with a broader hump as the applied field increases [Xing, J.; Phys. Rev. Mater. 2019, 3(11), 114413;Filippi, J.; Solid State Commun. 1977, 23(9), 613-616; Bloxsom, J. A. Thermal and Magnetic Studies of Spin Ice Compounds. University College London, 2016].

Evidence of an unusual magnetic behavior at the morphotropic phase boundary of La doped BiFeO3 ceramics

In this paper, Bi(1-x)LaxFeO3 ceramics were processed considering two compositions inside (Bi0.85La0.15FeO3) and outside (Bi0.95La0.05FeO3) the morphotropic phase boundary that separates the rhombohedral and orthorhombic phases. An unusual magnetic behavior, characterized by a double hysteresis loop, was observed at room temperature for the Bi0.85La0.15FeO3 sample. Langevin analyses revealed that this behavior is related to both the linear and non-linear components of the magnetization, indicating possible changes of the magnetic phase with doping.

Magnetization reversal modes and coercive field dependence on perpendicular magnetic anisotropy in FePt thin films

The competition between shape and perpendicular magnetic anisotropies in magnetic thin films gives rise to unusual magnetic behaviors. In ferromagnetic thin films, the presence of an out-of-plane component of the magnetic anisotropy may induce a transition from planar to stripe-like magnetic domains above a critical thickness, . In this article, we present a detailed study of the magnetization switching mechanism in FePt thin films, where this phenomenon is observed. Using micromagnetic simulations and experiments, we found that below the reversal mechanism is well described by the two-phase model while above this thickness the magnetization within each stripe reverses by coherent rotation. We also analyzed the out-of-plane component of the magnetic anisotropy and its temperature dependence, probing that substrate-induced strains are responsible for the abnormal coercive field behavior observed for FePt films with .

Enhancing the Squareness and Bi-Phase Magnetic Switching of Co2FeSi Microwires for Sensing Application.

In the current study we have obtained Co2FeSi glass-coated microwires with different geometrical aspect ratios, ρ = d/Dtot (diameter of metallic nucleus, d and total diameter, Dtot). The structure and magnetic properties are investigated at a wide range of temperatures. XRD analysis illustrates a notable change in the microstructure by increasing the aspect ratio of Co2FeSi-glass-coated microwires. The amorphous structure is detected for the sample with the lowest aspect ratio (ρ = 0.23), whereas a growth of crystalline structure is observed in the other samples (aspect ratio ρ = 0.30 and 0.43). This change in the microstructure properties correlates with dramatic changing in magnetic properties. For the sample with the lowest ρ-ratio, non-perfect square loops are obtained with low normalized remanent magnetization. A notable enhancement in the squareness and coercivity are obtained by increasing ρ-ratio. Changing the internal stresses strongly affects the microstructure, resulting in a complex magnetic reversal process. The thermomagnetic curves show large irreversibility for the Co2FeSi with low ρ-ratio. Meanwhile, if we increase the ρ-ratio, the sample shows perfect ferromagnetic behavior without irreversibility. The current result illustrates the ability to control the microstructure and magnetic properties of Co2FeSi glass-coated microwires by changing only their geometric properties without performing any additional heat treatment. The modification of geometric parameters of Co2FeSi glass-coated microwires allows to obtain microwires that exhibit an unusual magnetization behavior that offers opportunities to understand the phenomena of various types of magnetic domain structures, which is essentially helpful for designing sensing devices based on thermal magnetization switching.

Ni3InSb: Synthesis, Crystal Structure, Electronic Structure, and Magnetic Properties

The ternary phase with the composition Ni3InSb has been synthesized by high-temperature synthesis and structurally characterized by a combination of X-ray analysis, neutron diffraction analysis, and theoretical calculations. The structure of Ni3InSb crystallizes in the orthorhombic space group Pnma with lattice constants a = 7.111(3) Å, b = 5.193(3) Å, and c = 8.2113(2) Å. The crystal structure contains ∼20 atoms in its unit cell, which are distributed over four crystallographically independent positions (two Ni, one In, and one Sb). The crystal structure can be considered as a ternary substitutional variant of Ni3Sn2 (Pnma, no. 62), where a trivalent In and a pentavalent Sb orderly occupy two tetravalent Sn sites of Ni3Sn2. This site decoration pattern of two neighboring elements, In and Sb, is unique and confirmed by first principles total energy calculations. The crystal structure can be described by two building units: Ni2Sb (building unit of Ni2In) and NiIn (NiAs-type). They alternate in the crystal structure and form infinite ac-slabs (puckered), and the slabs are stacked along [010]. A triangular lattice formed by Ni atoms indicates the existence of a geometrically frustrated structure. The calculated density of states and crystal orbital Hamilton population enlighten the stability and bonding characteristics of the structure. The temperature-dependent neutron diffraction study down to 5 K reveals that the crystal structure remains in the same orthorhombic symmetry with a weak anomaly in the lattice parameters at ∼100 K. Detailed temperature- and magnetic field-dependent magnetic properties of the title phase Ni3InSb show spin-glass- or spin-disorder-like behaviors below ∼300 K with an unusual magnetic behavior below 100 K, where an enhancement of magnetization with a decrease of the coercive field has been found.

Formula omitted]-antisite disorder driven exchange bias effect and Griffiths-like phase in 25% Sr-doped [formula omitted

The unusual magnetic behaviour and multiple magnetic phases in double perovskite systems mainly originate from B-antisite disorder and various exchange couplings. Here we report the detailed exchange bias study in the hole doped Sm1.5Sr0.5CoMnO6 double perovskite system. The existence of structural antisite-disorder (Co-O-Co-O-Mn or Mn-O-Mn-O-Co) in the system is revealed. The ordering of Co2+ and Mn4+ gives rise to two ferromagnetic transitions, Tc1∼133 K and Tc2∼114 K. A Griffiths-like phase at ∼153 K is identified by the dc magnetization data above the ferromagnetic ordering temperature. The isothermal magnetization measurements further probe the exhibition of the conventional exchange bias effect and training effect phenomena in our sample. Maximum field shift ∼3.43 kOe in exchange bias effect is observed owing to the exchange couplings at the interfaces of FM/AFM at low temperature induced by B-antisite-disorder. In the 64–300 K temperature range, this disordered double perovskite exhibits insulating characteristics with a variable range hopping type of conduction mechanism. We also notice a negative magnetoresistance of −2.74% at 64 K and 60 kOe magnetic field.

Effect of Annealing on the Magnetic Properties of Co2MnSi-Based Heusler Alloy Glass-Coated Microwires

In the current study, we concentrated on the influence of annealing on the magnetic behavior of Co2MnSi-based Heusler microwires. We set the annealing temperature at 1023 K for 2 h, as the sample did not show any significant changes in the magnetic properties at lower temperatures, while annealing at temperatures above 1023 K damages the glass coating. Strong in-plane magnetocrystalline anisotropy parallel to the microwire axis was evident in the magnetic behavior at room temperature for as-prepared and annealed samples. The coercivity of the annealed sample was four times higher than that of the as-prepared sample across a wide range of measuring temperatures. Both annealed and as-prepared samples exhibit quite stable coercivity behavior with temperature, which may have interesting applications. The an nealed sample did not exhibit magnetic saturation for M-H loops measured below 50 K. Sharp irreversible magnetic behavior has been detected for annealed samples at a blocking temperature of 220 K; at the same time, the blocking temperature for the as-prepared sample was 150 K. The strong internal mechanical stress induced during the fabrication of Co2MnSi microwires in addition to the internal stress relaxation caused by the annealing induced the onset of magnetic phases resulting in unusual and irreversible magnetic behavior.

High-field EPR of copper(II)-nitroxide compound exhibiting three-step phase transition: structural insights from the field-induced sample orientation.

Copper(II)-nitroxide based Cu(hfac)2LR compounds exhibit unusual magnetic behavior that can be induced by various stimuli. In many aspects, the magnetic phenomena observed in Cu(hfac)2LR are similar to classical spin-crossover behavior. However, these phenomena originate from polynuclear exchange-coupled spin clusters Cu2+-O˙-N< or >N-˙O-Cu2+-O˙-N<. Such peculiarities may result in additional multifunctionality of Cu(hfac)2LR compounds, making them promising materials for spintronic applications. Herein, we investigate the Cu(hfac)2LMeMe material, which demonstrates a three-step temperature-induced magnetostructural transition between high-temperature, low-temperature, and intermediate states, as revealed by magnetometry. Two main steps were resolved using variable-temperature Fourier-transform infrared and Q-band electron paramagnetic resonance (EPR) spectroscopies. The intermediate-temperature states (∼40-90 K) are characterized by the coexistence of two types of copper(II)-nitroxide clusters, corresponding to the low-temperature and high-temperature phases. High-field EPR experiments revealed the effect of partial alignment of Cu(hfac)2LMeMe microcrystals in a strong (>20 T) magnetic field. This effect was used to unveil the structural features of the low-temperature phase of Cu(hfac)2LMeMe, which were inaccessible using single-crystal X-ray diffraction (XRD) technique. In particular, high-field EPR allowed us to determine the relative direction of the Jahn-Teller axes in CuO6 and CuO4N2 units.

Consistent Evaluation of Magnetic Exchange Couplings in Multicenter Compounds in KS-DFT: The Recomposition Method.

The use of broken-symmetry calculations in Kohn-Sham density functional theory has offered an affordable route to study magnetic exchange couplings in transition-metal-based compounds. However, computing this property in compounds exhibiting several couplings is still challenging and especially due to the difficulties to overcome the well-known problem of spin contamination. Here, we present a new and general method to compute magnetic exchange couplings in systems featuring several spin sites. To provide a consistent spin decontamination of J values, our strategy exploits the decomposition method of the magnetic exchange coupling proposed by Coulaud et al. and generalizes our previous work on diradical compounds where the overall magnetic exchange coupling is defined as the sum of its three main and properly extracted physical contributions (direct exchange, kinetic exchange, and spin polarization). In this aim, the generalized extraction of all contributions is presented to systems with multiple spin sites bearing one unpaired electron. This is done by proposing a new paradigm to treat the kinetic exchange contribution, which proceeds through monorelaxations of the magnetic orbitals. This method, so-called the recomposition method, is applied to a compound featuring three Cu(II) ions with a linear arrangement and to a recently synthesized complex containing a Cu4O4 cubane unit presenting an unusual magnetic behavior.

Correlation driven near-flat band Stoner excitations in a Kagome magnet

Among condensed matter systems, Mott insulators exhibit diverse properties that emerge from electronic correlations. In itinerant metals, correlations are usually weak, but can also be enhanced via geometrical confinement of electrons, that manifest as ‘flat’ dispersionless electronic bands. In the fast developing field of topological materials, which includes Dirac and Weyl semimetals, flat bands are one of the important components that can result in unusual magnetic and transport behaviour. To date, characterisation of flat bands and their magnetism is scarce, hindering the design of novel materials. Here, we investigate the ferromagnetic Kagomé semimetal Co3Sn2S2 using resonant inelastic X-ray scattering. Remarkably, nearly non-dispersive Stoner spin excitation peaks are observed, sharply contrasting with the featureless Stoner continuum expected in conventional ferromagnetic metals. Our band structure and dynamic spin susceptibility calculations, and thermal evolution of the excitations, confirm the nearly non-dispersive Stoner excitations as unique signatures of correlations and spin-polarized electronic flat bands in Co3Sn2S2. These observations serve as a cornerstone for further exploration of band-induced symmetry-breaking orders in topological materials.

Anomalous magnetic behavior in half-metallic Heusler Co2FeSi alloy glass-coated microwires with high Curie temperature

In the current study, we have succeeded to fabricate Co2FeSi Heusler alloy glass-covered microwires with magnetic core nucleus diameter d = 4.36 µm and total diameter D = 17.55 µm, with high Curie temperature (Tc>1100 K) and well-defined magnetic anisotropy for high temperature spintronic devices application. The magnetic properties of as-prepared and annealed at different temperature (873 K, 973 K and 1073 K for 1 h) of Co2FeSi Heusler alloy glass-covered microwires have been investigated. Strong dependence of the magnetic properties on the annealing conditions has been indicated. Anomalous magnetic behavior for annealed samples at 873 K and 973 K has been found and structural properties of such samples have been analyzed. Critical temperatures 155 K and 250 K have been detected for annealed samples at 873 K and 973 K, respectively, where the behavior of M-H loops and coercivity changed. Below the critical point the M-H curve shows “kink or wasp-waisted” magnetic behavior and complex magnetic reversal mechanism is supposed. The anomalous magnetic behavior is due to the martensitic phases induced by annealing conditions below the room temperature. This unusual magnetization behavior provides opportunities to understand the phenomena of different types of magnetic domain structures in the preferred crystallographically oriented Co2FeSi Heusler alloy glass-coated micro-wires, essentially helpful for designing the devices based on magnetization switching.

Violation of the rule of parsimony: Mixed local moment and itinerant Fe magnetism in Fe3GeN

Ternary iron nitrides are of considerable interest due to their diverse magnetic properties. We find, based on first principles calculations, that the relatively minor structural distortion from the cubic antiperovskite structure in Fe$_3$GeN leads to unusual magnetic behavior. In particular, there is a separation into Fe sites with very different magnetic behaviors, specifically a site with Fe atoms having a stable local moment and a site where the Fe shows characteristics of much more itinerant behavior. This shows a remarkable flexibility of the Fe magnetic behavior in these nitrides and points towards the possibility of systems where minor structural and chemical changes can lead to dramatic changes in magnetic properties. The results suggest that, analogously to oxide perovskite materials, modulation of magnetic properties via chemical or strain control of octahedral rotation may be feasible. This may then lead to approaches for tuning magnetism to realize properties of interest, for example tuning magnetic transitions to quantum critical regimes or to proximity to metamagnetic transitions of interest for devices.

On Some Ground State and Finite Temperature Properties of Mixed-Valence Compounds Induced by Next to Next-Nearest-Neighbor (NNNN) Hopping

In the present study, effects of next to next-nearest-neighbor (NNNN) hopping of delectrons in the crystal of mixed valence compounds has been discussed. For convenient theoretical calculation and computer simulation within exact diagonalization method, a small cluster of eight lattice sites is considered here to investigate the valence transition through the study of the inter-site and on-site f-d correlation functions. Unusual magnetic behavior of mixed valence compounds has also been examined. Antiferromagnetic (AF) order has been developed in the compounds of rare earth elements with the addition of NNNN hopping interaction within the extended Falicov-Kimball model. The extrapolation of the curves of the reciprocal susceptibility (χ−1) intercept at a negative temperature which confirms AF order in the system.

BaNa2Co7Te3O18 with a distorted 2-uniform lattice (T13) showing unusual magnetic behaviors.

Search for transition-metal compounds with unique spin lattices is a great challenge. Herein, we report on a successful exploration of a new compound BaNa2Co7Te3O18, featuring a unique spin network of (36; 34, 6)2-like lattice (T13), which is a typical example with distorted 2-uniform lattices. Magnetic measurements show that this compound has large magnetic anisotropy with an easy magnetization c-axis, while an unusually large magnetization loop can be observed in the magnetization curve. Furthermore, no λ-like peaks are observed in the heat capacity data, showing partial long-range order in the system, which is in good agreement with the theoretical prediction.

Ferromagnetic metallic Sr-rich Ln1/2A1/2CoO3 cobaltites with spontaneous spin rotation

The Pr$_{0.50}$Sr$_{0.5}$0CoO$_3$ perovskite exhibits unique magnetostructural properties among the rest of ferromagnetic/metallic Ln$_{0.50}$Sr$_{0.50}$CoO$_3$ compounds. The sudden orthorhombic-tetragonal (Imma $\to$ I4/mcm) structural transition produces an unusual magnetic behavior versus temperature and external magnetic fields. In particular, the symmetry change is responsible for a spontaneous spin rotation in this metallic oxide. We have studied half-doped Ln$_{0.50}$(Sr$_{1-x}$A$_x$)$_{0.50}$CoO$_3$ cobaltites varying the ionic radius rA of A-site cations (divalent cations and lanthanides) in order to complete the T-rA phase diagram. The influence of the structural distortion and the A-cations size for the occurrence of a spontaneous spin reorientation in the metallic state has been investigated. As the reorientation of the magnetization is driven by the temperature induced collapse of the orthorhombic distortion, a careful investigation of the structural symmetry is presented varying the structural distortion of the Sr-rich half-doped cobaltites by means of both compositional and temperature changes. The region in the phase diagram of these perovskites where the phase of magnetic symmetry Fm'm'm replaces that of Im'm'a symmetry was determined in this family of ferromagnetic/metallic cobaltites. In that region the magnetization direction has rotated 45 degrees within the a-b plane with respect to the second.