Noncollinear Arrangement Research Articles

Terahertz Crystal-Field Transitions and Quasi Ferromagnetic Magnon Excitations in a Noncollinear Magnet for Hybrid Spin-Wave Computation.

The complexity of interactions between the crystal-field and unusual noncollinear spin arrangement in nontrivial magnets demands novel tools to unravel the mystery underneath. In this work, we study such interaction dynamics of crystal-field excitations (CFE) and low-energy magnetic excitations in orthochromite TmCrO3 with controls of temperature and magnetic field using high-resolution magneto-terahertz (THz) time-domain spectroscopy. The THz energy spectrum spanning 0.5-10 meV possesses a low-frequency spin-excitation (magnon) mode and a multitude of CFE modes at 10 K, all of which uniquely embody a range of phenomena. For the magnon mode, a temperature dependence of peak frequency is induced by magnetic interactions between Tm and Cr subsystems. While a change from blue to red shift of peak frequency of this mode marks the magnetization reversal transition, the spin-reorientation temperature and change of magnetic anisotropy are depicted by different features of field and temperature dependent peak frequency dynamics. The modes corresponding to CFE are robust and laden with a multitude of submodes, which are attributes of nontrivial interactions across different transitions. These modes are suppressed only upon substitution of Tb3+ at the Tm3+ site, which suggests a dominant role of single-ion anisotropy in controlling entire THz excitation spectra. Overall, this remarkable range of phenomena seen through the unique lens of all-optical THz tools provides deeper insights into the origin of magnetic phases in systems with complex interactions between rare-earth and transition metal ions and provides a multitude of novel combinations of closely spaced modes for emerging hybrid spin-wave computation.

Exchange bias and topological Hall effect of Fe and Co intercalated NbS2 single crystals

In recent years, the topological Hall effect generated by noncoplanar magnetic structures has been studied extensively. Some two-dimensional chalcogenides with 3d transition metal intercalations also exhibit similar properties. In this study, we investigated the crystalline structure and the magnetic and transport properties of Fe and Co codoped NbS2 single crystals. The structural results indicate disorder between the Fe and Co atoms within the interlayers of NbS2. Magnetic measurements showed that the vertical exchange bias effect appeared below the Néel temperature (TN), with a maximum value of approximately 2.5 mμB/f.u. at 2 K, which can be ascribed to the appearance of a spin-glass state. Additionally, accompanying the antiferromagnetic phase transition, nontrivial electrical transport properties were observed. Below TN, the magnetoresistance became positive and exhibited an initial increase, followed by a decrease with decreasing temperature. The Hall resistivity shows a hump-like curve near TN, indicating a topological Hall effect. This behavior is related to fluctuations in the spin chirality, which affects the scattering of charge carriers. Based on the correlation between the magnetoresistance and Hall resistivity responses, it is believed that the magnetic moments of the doped Fe and Co atoms in a single crystal compete with each other near the Néel temperature, resulting in complex magnetic structures such as noncoplanar and noncollinear arrangements. Such a two-dimensional antiferromagnetic material system provides an ideal platform for studying unconventional transport mechanisms.

Anomalous Nernst effect in the noncollinear antiferromagnet Mn5Si3

Investigating the off-diagonal components of the conductivity and thermoelectric tensor of materials hosting complex antiferromagnetic structures has become a viable method to reveal the effects of topology and chirality on the electronic transport in these systems. In this respect, Mn5Si3 is an interesting metallic compound that exhibits several antiferromagnetic phases below 100 K with different collinear and noncollinear arrangements of Mn magnetic moments determined from neutron scattering. Previous electronic transport measurements have shown that the transitions between the various phases give rise to large changes of the anomalous Hall effect. Here, we report measurements of the anomalous Nernst effect of Mn5Si3 single crystals that also show clear transitions between the different magnetic phases. In the noncollinear phase, we observe an unusual sign change of the zero-field Nernst signal with a concomitant decrease of the Hall signal and a gradual reduction of the remanent magnetization. Furthermore, a symmetry analysis of the proposed magnetic structures shows that both effects should actually vanish. These results indicate a symmetry-breaking modification of the magnetic state with a rearrangement of the magnetic moments at low temperatures, thus questioning the previously reported models for the noncollinear magnetic structure obtained from neutron scattering.

Signatures of polarized chiral spin disproportionation in rare earth nickelates

In rare earth nickelates (RENiO3), electron-lattice coupling drives a concurrent metal-to-insulator and bond disproportionation phase transition whose microscopic origin has long been the subject of active debate. Of several proposed mechanisms, here we test the hypothesis that pairs of self-doped ligand holes spatially condense to provide local spin moments that are antiferromagnetically coupled to Ni spins. These singlet-like states provide a basis for long-range bond and spiral spin order. Using magnetic resonant X-ray scattering on NdNiO3 thin films, we observe the chiral nature of the spin-disproportionated state, with spin spirals propagating along the crystallographic (101)ortho direction. These spin spirals are found to preferentially couple to X-ray helicity, establishing the presence of a hitherto-unobserved macroscopic chirality. The presence of this chiral magnetic configuration suggests a potential multiferroic coupling between the noncollinear magnetic arrangement and improper ferroelectric behavior as observed in prior studies on NdNiO3 (101)ortho films and RENiO3 single crystals. Experimentally-constrained theoretical double-cluster calculations confirm the presence of an energetically stable spin-disproportionated state with Zhang-Rice singlet-like combinations of Ni and ligand moments.

Interfacial layer effect on the enhancement of gilbert damping in RF magnetron sputtered Y3Fe5O12/Gd3Ga5O12 thin films

We report the magnetization dynamics study in Y3Fe5O12 (YIG) film grown by rf magnetron sputtering techniques. The growth-induced interfacial layer is believed to affect the top YIG layer, interrupting the magnetic properties associated with it drastically. The structural data confirmed the epitaxial and strained growth of YIG on a highly matched GGG (100) substrate. The frequency variation of the FMR signal yields various important parameters, such as the line width (ΔH), effective magnetization (4πMeff), and damping constant (α) at 300 K. The significant increase in 4πMeff to 2187.848 Oe reflects the presence of non-collinear or antiparallel arrangement of magnetic moment in YIG thin-film. Apart from this value of α was reported to be 1.5 × 10−3 which is substantially higher than the values reported in the literature for such higher-quality epitaxial thin films. We anticipate that a detailed analysis of these findings will provide excellent speculation in the field of magnonics, advanced spintronics and terahertz frequency-related applications.

Magnetization dynamics in layered systems with coexisting bilinear and biquadratic interlayer exchange coupling

Important aspects of exchange-coupled magnetic layered structures are related to the noncollinear arrangement of sublayer magnetizations which can arise from competition between bilinear (BL) and biquadratic (BQ) interlayer exchange coupling (IEC). In this work, the influence of coexisting BL and BQ IEC of different strengths on magnetization precession in layered systems is investigated both experimentally and theoretically. Laser-induced magnetization precession has been studied in the $\text{Fe/Si}({d}_{\text{Si}}$) multilayers (MLS) as a function of the amplitude ($H$) and orientation angle (${\ensuremath{\theta}}_{H}$) of external magnetic field using time-resolved magneto-optical Kerr (TRMOKE) effect. Strongly changing characters of precession frequency dependencies $\ensuremath{\omega}(H,{\ensuremath{\theta}}_{H})$ for Fe sublayer thickness ${d}_{\text{Fe}}=3$ nm and Si spacer-layer thicknesses (${d}_{\text{Si}}$) varying in the range of 0.9--2.4 nm have been observed. Analytical formulas for acoustic and optic mode dispersion relations with coexisting BL and BQ IEC, scaled by ${J}_{1}$ and ${J}_{2}$ parameters, respectively, for the in-plane effective magnetic anisotropy and arbitrary magnetic field direction were derived, and very good agreement with the experimentally observed frequency dependencies has been obtained. It is shown that BQ coexisting with BL IEC significantly influences on the magnitude and form of dispersion relations. From analytical formula derived, it follows that zero-field optical mode frequency tends to zero as $|{J}_{1}|$ approaches $2{J}_{2}$. The acoustic and optic mode-crossing effect has been observed and it is found that values of crossing fields and frequency gaps strongly increase as ${\ensuremath{\theta}}_{H}$ angles decrease and depend on relative BL and BQ IEC strengths. The BL IEC is of ferromagnetic type with ${J}_{1}\ensuremath{\approx}1.6$ mJ/${\mathrm{m}}^{2}$ for the MLS with ${d}_{\text{Si}}=0.9$ nm, and changes to antiferromagnetic one with ${J}_{1}\ensuremath{\approx}\ensuremath{-}0.9$ mJ/${\mathrm{m}}^{2}$ for the MLS with ${d}_{\text{Si}}=1.4$ nm, while the ${J}_{2}$ parameter of BQ IEC decreases from 1.8 to 1.0 mJ/${\mathrm{m}}^{2}$. The coupling strengths decrease by one to two orders of magnitude for the sample with ${d}_{\text{Si}}=2.4$ nm, but both mode frequencies are still observed and well reproduced by the theory. It is shown that ${J}_{1}$ and ${J}_{2}$ parameters obtained in the TRMOKE experiment coincide within the estimated error bars with the determined from independent measurements of magnetization processes in the static magneto-optical Kerr effect and interpreted with the use of analytical formulas derived. Numerical solutions of coupled Landau-Lifshitz-Gilbert (LLG) equations for acoustic and optic modes, with inclusion of BL IEC, intrinsic Gilbert damping, and spin-pumping damping terms, and extended to include BQ IEC, were performed and fitted to experimental data. It is shown that determined effective damping coefficients on $H$ and ${\ensuremath{\theta}}_{H}$ dependencies for acoustic and optic modes are very well simulated with the use of LLG equation solutions with Gilbert damping, spin-pumping-damping--related effective spin-mixing conductance, and spin-diffusion length parameters included. The dependencies of the parameters on ${d}_{\text{Si}}$ spacer-layer thickness are discussed and compared with available data for other systems.

Chiral antiferromagnetic Josephson junctions as spin-triplet supercurrent spin valves and d.c. SQUIDs

Spin-triplet supercurrent spin valves are of practical importance for the realization of superconducting spintronic logic circuits. In ferromagnetic Josephson junctions, the magnetic-field-controlled non-collinearity between the spin-mixer and spin-rotator magnetizations switches the spin-polarized triplet supercurrents on and off. Here we report an antiferromagnetic equivalent of such spin-triplet supercurrent spin valves in chiral antiferromagnetic Josephson junctions as well as a direct-current superconducting quantum interference device. We employ the topological chiral antiferromagnet Mn3Ge, in which the Berry curvature of the band structure produces fictitious magnetic fields, and the non-collinear atomic-scale spin arrangement accommodates triplet Cooper pairing over long distances (>150 nm). We theoretically verify the observed supercurrent spin-valve behaviours under a small magnetic field of <2 mT for current-biased junctions and the direct-current superconducting quantum interference device functionality. Our calculations reproduce the observed hysteretic field interference of the Josephson critical current and link these to the magnetic-field-modulated antiferromagnetic texture that alters the Berry curvature. Our work employs band topology to control the pairing amplitude of spin-triplet Cooper pairs in a single chiral antiferromagnet.

Non-collinear magnetic structure of the MAX phase Mn2GaC epitaxial films inferred from zero-field NMR study (CE-5:L05)

Zero-field NMR investigations on the 69Ga, 71Ga, and 55Mn nuclei have been performed at 4.2 K on a 100 nm thick epitaxial Mn2GaC(0001) MAX phase film grown on a MgO(111) substrate. This nano-laminated structure consists of ferromagnetic Mn–C–Mn stacks interleaved with monolayers of gallium. A resolved quadrupolar structure of the observed gallium resonances is a fingerprint of a well-defined crystal field confirming high crystal quality. The nuclei of non-magnetic gallium atoms are shown to experience the transferred hyperfine magnetic field of 15.75 T (±0.05 T), which is due to polarization of their 4s electron shell by the magnetic moments of manganese neighbors, evidencing the presence of an uncompensated ferromagnetic moment within the manganese sublattice. The average magnetic moment of manganese was found to be around 2 μB, strongly contrasting with the reported remnant magnetization of only 0.3 μB. Moreover, the 55Mn NMR spectrum indicates the presence of magnetically non-equivalent manganese sites within this structure. The observed features of the 69,71Ga and 55Mn NMR spectra cannot be reconciled with any of the hitherto proposed collinear arrangements of manganese moments and suggest their non-collinear arrangement across a gallium layer. Nevertheless a more advanced study is required to elucidate the detailed nature of magnetic structure in this material.

Magnetic ground states of honeycomb lattice Wigner crystals

Lattice Wigner crystal states stabilized by long-range Coulomb interactions have recently been realized in two-dimensional moiré materials. We employ large-scale unrestricted Hartree-Fock techniques to unveil the magnetic phase diagrams of honeycomb lattice Wigner crystals. For the three lattice filling factors with the largest charge gaps, n=2/3,1/2,1/3, the magnetic phase diagrams contain multiple phases, including ones with non-collinear and non-coplanar spin arrangements. We discuss magnetization evolution with external magnetic field, which has potential as an experimental signature of exotic spin states. Our theoretical results could potentially be validated in moiré materials formed from group VI transition metal dichalcogenide twisted homobilayers.

Orbital Angular Momentum of Magnons in Collinear Magnets.

We study the orbital angular momentum of magnons for collinear ferromagnet (FM) and antiferromagnetic (AF) systems with nontrivial networks of exchange interactions. The orbital angular momentum of magnons for AF and FM zigzag and honeycomb lattices becomes nonzero when the lattice contains two inequivalent sites and is largest at the avoided-crossing points or extremum of the frequency bands. Hence, the arrangement of exchange interactions may play a more important role at producing the orbital angular momentum of magnons than the spin-orbit coupling energy and the resulting noncollinear arrangement of spins.

High-order harmonic generation in three-dimensional Weyl semimetals with broken time-reversal symmetry

In this paper the nonlinear interaction of a Weyl semimetal (WSM) with a strong driving electromagnetic wave field is investigated. In the scope of the structure-gauge-invariant low-energy nonlinear electrodynamic theory, the polarization-resolved high-order harmonic generation spectra in the WSM with broken time-reversal symmetry are analyzed. The results obtained show that the spectra in the WSM are completely different compared to the two-dimensional graphene case. In particular, at the noncollinear arrangement of the electric and Weyl node momentum separation vectors, anomalous harmonics are generated which are polarized perpendicular to the pump wave electric field. The intensities of anomalous harmonics are quadratically dependent on the momentum space separation of the Weyl nodes. If the right and the left Weyl fermions are merged, we have a four-component trivial massless Dirac fermion and, as a consequence, the anomalous harmonics vanish. In contrast to the anomalous harmonics, the intensities of normal harmonics do not depend on the Weyl nodes' momentum separation vector and the harmonics spectra resemble the picture for a massless three-dimensional Dirac fermion.

Implications of electron and hole doping on the magnetic properties of spin–orbit entangled Ca4IrO6 from DFT calculations

We investigate the electronic structure and magnetic properties of a Jeff=1/2 iridate Ca4IrO6 and the implications of doping electrons and holes using ab initio density functional theory. Our calculations considering spin–orbit interaction reveal that although the Mott-insulating parent compound transforms into a conductor upon doping, antiferromagnetism sustains in the doped system, albeit with a grossly noncollinear arrangement of the spins. We find a strong spin–orbit interaction and magneto-crystalline anisotropy, causing frustration in the system, possibly leading to the highly noncollinear arrangement of spins upon non-magnetic doping. Our results may be important from the viewpoint of spintronics using iridates or other 5d materials.

Spatially enhanced electric field induced second harmonic (SEEFISH) generation for measurements of electric field distributions in high-pressure plasmas

The spatial resolution of the ps electric field induced second harmonic (EFISH) generation has been enhanced by using non-collinear pump laser beam arrangements. The pump laser beam (1064 nm, nominal pulse duration 150 ps, pulse energy 20–40 mJ) is separated into two coaxial or crossing beams, overlapping only near the focal point. The spatially enhanced EFISH (SEEFISH) signal is generated over a shorter beam overlap region compared to the collinear beam arrangement. Blocking of either of the two beams results in a complete suppression of the signal. The signal is spatially isolated from the ‘conventional’ EFISH signal and measured by a photomultiplier detector. Measurements of a known Laplacian field generated between two parallel cylinder electrodes in ambient air shows that SEEFISH improves the spatial resolution of the measurements by up to a factor of 2, such that the measurement results agree with the Laplacian field distribution. The spatial resolution is improved further by reducing the focal distance of the lens. The magnitude of the SEEFISH signal is significantly lower compared to that of the single-beam EFISH and decreases rapidly as the beam crossing angle is increased, due to the phase mismatch. This approach has a significant potential for measurements of electric field distributions in high-pressure plasmas, with an additional benefit of removing the stray second harmonic signal from the optical access windows.

Magnetic structure of magnetoelectric multiferroic HoFeWO6

The polar magnetic oxide, HoFeWO6, is synthesized, and its crystal structure, magnetic structure, and thermodynamic properties are investigated. HoFeWO6 forms the polar crystal structure (space group Pna21 (#33)) due to the cation ordering of W6+ and Fe3+. An antiferromagnetic transition at TN = 17 K is accompanied by a significant change in magnetic entropy with a value of ≈ 5 J kg−1 K−1 in a 70 kOe applied field. Temperature dependent neutron diffraction and magnetization data indicate that the Fe sublattice orders in a strongly non-collinear and non-coplanar arrangement below TN. The Fe ordering initially leads to induced ordering of the Ho spins such that the Ho spins also show behavior of long-range ordering that is evident from the neutron diffraction measurements. Below T ≈ 4 K, the Ho spins order independently and pull the Fe spins toward the direction of Ho spins. A comparison with the magnetic structures and corresponding ferroelectric properties of other members of RMWO6 (R = Y, Sm-Tm, M = Cr, Fe, V) family indicate that the spontaneous polarization is due to the magnetic structure specific to the Fe sublattice through magnetoelectric coupling whereas the polarization is independent of the Ho sublattice.

Magnetically Induced Polarization in Centrosymmetric Bonds.

We reveal the microscopic origin of electric polarization P[over →] induced by noncollinear magnetic order. We show that in Mott insulators, such P[over →] is given by all possible combinations of position operators r[over →][over ^]_{ij}=(r[over →]_{ij}^{0},r[over →]_{ij}) and transfer integrals t[over ^]_{ij}=(t_{ij}^{0},t_{ij}) in the bonds, where r[over →]_{ij}^{0} and t_{ij}^{0} are spin-independent contributions in the basis of Kramers doublet states, while r[over →]_{ij} and t_{ij} stem solely from the spin-orbit interaction. Among them, the combination t_{ij}^{0}r[over →]_{ij}, which couples to the spin current, remains finite in the centrosymmetric bonds, thus yielding finite P[over →] in the case of noncollinear arrangement of spins. The form of the magnetoelectric coupling, which is controlled by r[over →]_{ij}, appears to be rich and is not limited to the phenomenological law P[over →]∼ε_{ij}×[e_{i}×e_{j}] with ε_{ij} being the bond vector connecting the spins e_{i} and e_{j}. Using density-functional theory, we illustrate how the proposed mechanism works in the spiral magnets CuCl_{2}, CuBr_{2}, CuO, and α-Li_{2}IrO_{3}, providing a consistent explanation for the available experimental data.

Superconducting Scanning Tunneling Microscope Tip to Reveal Sub-millielectronvolt Magnetic Energy Variations on Surfaces.

Combining the complex ordering ability of molecules with their local magnetic properties is a little-explored technique to tailor spin structures on surfaces. However, revealing the molecular geometry can be demanding. Nickelocene (Nc) molecules present a large spin-flip excitation leading to clear changes of conductance at the excitation-threshold bias. Using a superconducting tip, we have the energy resolution to detect small shifts of the Nc spin-flip excitation thresholds, permitting us to reveal the different individual environments of Nc molecules in an ordered layer. This knowledge allows us to reveal the adsorption configuration of a complex molecular structure formed by Nc molecules in different orientations and positions. As a consequence, we infer that Nc layers present a strong noncollinear magnetic-moment arrangement.

The Influence of Non-Collinear Electrodes Arrangement on a Two-dimensional Resistivity Survey Using Wenner Array

Conventional protocols employed by various multi-electrode resistivity systems are designed with the assumption that the survey lines are straight to ensure collinear electrode pairs. However, as most survey areas are characterized by surface constraints, it is rarely possible to carry out two-dimensional electrical resistivity tomography (2-DERT) measurement on a straight line. Therefore, 2-DERT surveys conducted on a surface constraint field requires shifting of some electrodes off the survey line, which implies a non-collinear electrodes arrangement. Hence, the result of such a survey is prone to false anomalies and in turn, wrong interpretation. This article aims to uncover the potential effect of non-collinear electrodes arrangement on 2-D resistivity survey. To achieve this goal, the data was acquired in four phases using Wenner array with all electrodes inline, one offline, two offline and three offline at stepwise distances, respectively. The inverse resistivity models obtained revealed slight to distinct variation of anomalies as two or more electrodes are offline at a distance >½ the minimum electrode spacing.

Sol-gel derived cobalt containing Ni–Zn ferrite nanoparticles: Dielectric relaxation and enhanced magnetic property study

A systematic study of transitional metal ion doped nickel-zinc ferrite (NZF) nanoparticles with its magnetic properties and conductivity relaxation mechanism are the objectives of this research. We have prepared cobalt doped NZF nanoparticles (NZCo) via a facile chemical route. X-Ray Diffraction (XRD) and Transmission Electron Microscopy (TEM) analyses suggest the formation of single phase nearly spherical nanoparticles around 60 nm in size. UV–Vis study reveals the redshift of the optical band gap for doped samples. Estimation of particle size using the effective mass model agrees well with TEM/XRD results. The electrical modulus spectra have been analyzed using Harvilliak-Negami model function. Migration energy has been found to be the minimum for 10 mol % doped sample. Frequency-dependent modulus spectra have been converted to time domain data and the relaxation process shows Kohlrausch–Williams–Watts (KWW) type behavior. Carrier motion inside the lattice has been found to be strongly correlated. Room temperature magnetization curve shows that very weak AFM/PM contribution and strong FM interaction inside the system as well as non-collinear spin arrangements between interstitial sites. Law of Approach (L.A.) analysis of the AFM/PM part subtracted hysteresis curve delineates the enhanced magnetic properties such as saturation magnetization, anisotropy constant and coercivity. Multi-functional materials of such kind with optimum behavior at specific doping percentages can be fruitful for electronic industries.

Planar Hall effect caused by the memory of antiferromagnetic domain walls in Mn3Ge

In Mn3X (X = Sn, Ge) antiferromagnets, domain walls are thick and remarkably complex because of the non-collinear arrangement of spins in each domain. A planar Hall effect (PHE), an electric field perpendicular to the applied current but parallel to the applied magnetic field, was recently observed inside the hysteresis loop of Mn3Sn. The sign of the PHE displayed a memory tuned by the prior orientation of the magnetic field and its history. We present a study of the PHE in Mn3Ge extended from room temperature down to 2 K and show that this memory effect can be manipulated by either a magnetic field or thermal cycling. We show that the memory can be wiped out if the prior magnetic field exceeds 0.8 T or when the temperature exceeds TN. We also find a detectable difference between the amplitude of the PHE with zero-field and field thermal cycling. The ratio between the PHE and the anomalous Hall effect decreases slightly as temperature is increased from 2 K to TN and tracks the temperature dependence of magnetization. This erasable memory effect may be used for data storage.

Ground state spin structure of GdFeO3: A computational and experimental study

Magnetization studies have been carried out on single-phase, polycrystalline GdFeO3, synthesized using solid-state reaction method. An anti-ferromagnetic transition associated with Gd3+ spin was observed at TN(Gd3+) ~ 2.8 K. The Density Functional Theory (DFT) calculations on the non-collinear spin arrangement in GdFeO3 show a magnetic moment of 0.026µB per Fe3+ ion, consistent with experimentally observed moment of 0.023µB. Further, our results predict that (Gx,Ay,Fz) and Gx spin structures are energetically the most favorable states for Fe3+ and Gd3+ sub-lattices respectively.