Magnetic Order Research Articles

Lattice dynamics of 119Sn impurity in a bcc-Cr crystal

The chromium crystal doped with119Sn isotope was studied using the nuclear resonance inelastic x-ray scattering and first principles calculations. The Sn partial phonon density of states (PDOS) was obtained for three temperatures that correspond to different magnetic states of Cr. At all temperatures, the energy spectrum consists of a broad band around 18 meV and a narrow peak at 43 meV. The additional peak around 39 meV is observed only in the magnetically ordered phases, indicating the influence of magnetic order in chromium on lattice dynamics. The partial PDOS calculated with the antiferromagnetic order on Cr atoms show a very good agreement with the experimental data. It is revealed that the high-energy peak is lying above the phonon spectra of the pure bcc-Cr crystal. These are the local modes with the increased energies due to a strongly reduced distance between Sn and the nearest-neighbor Cr atoms.

Entropy-stabilized materials as a platform to explore terbium-based pyrochlore frustrated magnets

Two decades of work have shown that the physics of Tb-based pyrochlores is controlled by a subtle equilibrium between quadrupole-quadrupole and dipolar-dipolar magnetic interactions, as exemplified by the ordered spin ice Tb2Sn2O7 and the quantum spin liquid candidate Tb2Ti2O7. The high-entropy approach is thus quite promising, as it offers the possibility of a delicate tuning of chemical disorder. In this work, we investigate the entropy-stabilized pyrochlore compound Tb2(TiZrHfGeSn)2O7. We report the lack of long range magnetic order, yet the observed magnetic diffuse scattering is characteristic of antiferromagnetic first-neighbor correlations. The crystal field excitation spectrum, with broaden levels, visibly reflects the smooth environmental disorder of the Tb environment. The low energy dynamics are characterized by a narrow mode at about 0.4 meV, consistent with specific heat. Remarkably, as illustrated by a model of random isotropic shifts of oxygen atoms around Tb ions, the spectral weight of this mode is a direct consequence of deviations from the D3d symmetry at Tb sites. In the light of these results, quadrupolar interactions are also discussed.

High Entropy Protected Sharp Magnetic Transitions in Highly Disordered Spinel Ferrites.

How disorder affects magnetic ordering is always an intriguing question, and it becomes even more interesting in the recently rising high entropy oxides due to the extremely high disorder density. However, due to the lack of high-quality single crystal samples, the strong compositional disorder effect on magnetic transition has not been deeply investigated. In this work, we have successfully synthesized high-quality single crystalline high entropy spinel ferrites (Mg0.2Mn0.2Fe0.2Co0.2Ni0.2)xFe3-xO4. Our findings from high-temperature magnetization and neutron diffraction experiments showed ferrimagnetic transitions at 748, 694, and 674 K for x values of 1, 1.5, and 1.8, respectively. Notably, the magnetic transition almost showed no broadening for x values of 1 and 1.5, compared to Fe3O4. Extended X-ray absorption fine structure measurements provided insights into the elemental distribution among the octahedral and tetrahedral sites. The random distribution of elements across these sites reduced the formation of local clusters and short-range orders, enhancing sample homogeneity and preserving the sharpness of the magnetic transition, despite bond length variation. Our study not only marks the first successful synthesis of an HEO bulk single crystal exhibiting long-range magnetic order but also sheds light on the interaction between high configurational entropy and magnetic orderings. This opens new avenues for future research and applications of magnetic high entropy oxides.

Magnetism of pseudospin-1/2 pyrochlore antiferromagnet Na3Co(CO3)2Cl.

Pyrochlore magnets have attracted interest as systems for realizing critical phenomena, rich magnetic structures, associated topological band structures, and nontrivial quantum phases. Na3Co(CO3)2Cl is a pseudospin-1/2 antiferromagnet in which the Co2+ions form a pyrochlore network. Its structural and magnetic properties were investigated using magnetization, heat capacity, ESR, single-crystal X-ray diffraction, powder neutron diffraction and powder inelastic neutron scattering. Magnetization and heat capacity measurements indicated a ground-state doublet, which is regarded as pseudospin 1/2, dominated the magnetic properties at low temperatures, with a magnetic exchange of 9.6 K. As the temperature decreases, a magnetic transition is observed at 1.6 K, which is confirmed to be an all-in-all-out magnetic order. The crystal field excitations observed by inelastic neutron scattering experiments indicated the Ising nature of the ground-state doublet. This thorough study revealed that Na3Co(CO3)2Cl can be regarded as a pseudospin-1/2 pyrochlore lattice antiferromagnet with dominant Ising-type interactions.

Static magnetic order with strong quantum fluctuations in spin-1/2 honeycomb magnet Na2Co2TeO6

Kitaev interactions, arising from the interplay of frustration and bond anisotropy, can lead to strong quantum fluctuations and, in an ideal case, to a quantum-spin-liquid state. However, in many nonideal materials, spurious non-Kitaev interactions typically promote a zigzag antiferromagnetic order in the d-orbital transition-metal compounds. Here, by combining neutron scattering with muon-spin rotation and relaxation techniques, we provide mechanism insights into the exotic properties of Na2Co2TeO6, a candidate material of the Kitaev model. Below TN, the zero-field muon-spin relaxation rate becomes almost constant (~0.45 μs−1). We attribute this temperature-independent relaxation rate to the strong quantum fluctuations, as well as to the frustrated Kitaev interactions. As the magnetic field increases, neutron scattering data indicate a broader spin-wave excitation at the K-point. Therefore, quantum fluctuations seem not only robust but are even enhanced by the applied magnetic field. Our findings provide valuable hints for understanding the onset of the quantum-spin-liquid state in Kitaev materials.

Manipulating Photogalvanic Effects in Two-Dimensional Multiferroic Breathing Kagome Materials.

Multiferroic materials, known for their multiple tunable orders, present an exceptional opportunity to manipulate nonlinear optical responses that are sensitive to symmetry. In this study, we propose leveraging electric and magnetic fields to selectively control and switch specific types of photogalvanic effects in two-dimensional multiferroic breathing kagome materials. Taking monolayer Nb3I8 as an example, we demonstrate that the shift current, characterized by the real-space shift of electrons and holes, is predominantly unaffected by magnetic order. In contrast, injection current, featured by quantum metric dipole in momentum space, is closely related to valley polarization, which can be controlled by a magnetic field. Furthermore, both photocurrents can be reversed by an out-of-plane electric field via lattice breathing. Our findings reveal the potential of multiferroic breathing kagome structures for multifunctional optoelectronic applications and sensors.

Real-Space Imaging of Intrinsic Symmetry-Breaking Spin Textures in a Kagome Lattice.

The electronic orders in kagome materials have emerged as a fertile platform for studying exotic quantum states, and their intertwining with the unique kagome lattice geometry remains elusive. While various unconventional charge orders with broken symmetry is observed, the influence of kagome symmetry on magnetic order has so far not been directly observed. Here, using a high-resolution magnetic force microscopy, it is, for the first time, observed a new lattice form of noncollinear spin textures in the kagome ferromagnet in zero magnetic field. Under the influence of the sixfold rotational symmetry of the kagome lattice, the spin textures are hexagonal in shape and can further form a honeycomb lattice structure. Subsequent thermal cycling measurements reveal that these spin textures transform into a non-uniform in-plane ferromagnetic ground state at low temperatures and can fully rebuild at elevated temperatures, showing a strong second-order phase transition feature. Moreover, some out-of-plane magnetic moments persist at low temperatures, supporting the Kane-Mele scenario in explaining the emergence of the Dirac gap. The observations establish that the electronic properties, including both charge and spin orders, are strongly coupled with the kagome lattices.

Spin-Peierls instability of the U(1) Dirac spin liquid

Quantum fluctuations can inhibit long-range ordering in frustrated magnets and potentially lead to quantum spin liquid (QSL) phases. A prime example are gapless QSLs with emergent U(1) gauge fields, which have been understood to be described in terms of quantum electrodynamics in 2+1 dimension (QED3). Despite several promising candidate materials, however, a complicating factor for their realisation is the presence of other degrees of freedom. In particular lattice distortions can act to relieve magnetic frustration, precipitating conventionally ordered states. In this work, we use field-theoretic arguments as well as extensive numerical simulations to show that the U(1) Dirac QSL on the triangular and kagome lattices exhibits a weak-coupling instability due to the coupling of monopoles of the emergent gauge field to lattice distortions, leading to valence-bond solid ordering. This generalises the spin-Peierls instability of one-dimensional quantum critical spin chains to two-dimensional algebraic QSLs. We study static distortions as well as quantum-mechanical phonons. Even in regimes where the QSL is stable, the singular spin-lattice coupling leads to marked temperature-dependent corrections to the phonon spectrum, which provide salient experimental signatures of spin fractionalisation. We discuss the coupling of QSLs to the lattice as a general tool for their discovery and characterisation.

Antiferromagnetic coupling in ferrimagnetic Mn4N-based bilayer structures

Mn4N/(Mn,Cu)4N epitaxial bilayer structures with (Mn,Cu)4N compositions below and above the magnetization compensation composition were prepared on SrTiO3(001) substrates by molecular beam epitaxy. The thickness of the (Mn,Cu)4N layer was fixed at approximately 20 nm, while that of the Mn4N layer was changed from 7.5 to 19.6 nm. Cross-sectional elemental mapping proved that the diffusion of Cu from the (Mn,Cu)4N layer to the Mn4N layer was negligible. The magnetization curves showed that the magnetic moments of Mn4N and (Mn,Cu)4N were antiferromagnetically coupled, independent of the Mn4N film thickness, indicating a synthetic ferrimagnetic structure. The dependence of magnetic order on Mn4N film thickness was confirmed by surface-sensitive measurements using polar magneto-optical Kerr effect and x-ray magnetic circular dichroism. This is due to the change in the layer with dominant magnetization and the strength of the antiferromagnetic coupling. The temperature dependence of the anomalous Hall effect showed that the antiferromagnetic coupling was retained in the Mn4N(7.5 nm)/(Mn,Cu)4N(22.4 nm) structure over a wide temperature range of 10–350 K.

Reconstructing the spatial structure of quantum correlations in materials

Quantum correlations are a fundamental property of quantum many-body states. Yet they remain experimentally elusive, hindering certification of genuine quantum behavior, especially in quantum materials. Here we show that the momentum-dependent dynamical susceptibility measured via inelastic neutron scattering enables the systematic reconstruction of a general family of quantum correlation functions, which express the degree of quantum coherence in the fluctuations of two spins at an arbitrary mutual distance. Using neutron scattering data for the compound KCuF3—a system of weakly coupled S=1/2 Heisenberg chains—and numerically exact quantum Monte Carlo data, we show that quantum correlations possess a radically different spatial structure with respect to conventional correlations. Indeed, they exhibit a different emergent length scale—the quantum coherence length—which is finite at any finite temperature (including when long-range magnetic order develops). Moreover, we show theoretically that coupled Heisenberg spin chains exhibit a form of quantum monogamy, with a trade-off between quantum correlations along and transverse to the spin chains. These results highlight real-space quantum correlators as an informative, model-independent means of probing the underlying quantum state of real quantum materials. Published by the American Physical Society 2024

Ce2Ir3Ga5 : A new locally noncentrosymmetric heavy fermion system

Recently, a new type of unconventional superconductivity with a field-induced transition between two different superconducting (SC) states was discovered in the heavy fermion system CeRh2As2. This unusual SC state was proposed to be based on specific symmetries of the underlying structure, i.e., a globally centrosymmetric layered structure, but where the Ce layers themselves lack inversion symmetry. This new type of SC state has attracted strong interest, prompting the search for further heavy fermion systems crystallizing in structures with appropriate symmetries. We report the discovery and the study of a new Ce-based heavy fermion system with a globally centrosymmetric structure but without inversion symmetry on the Ce-site, Ce2Ir3Ga5. A single crystal x-ray diffraction study revealed an orthorhombic U2Co3Si5 type structure. Resistivity, specific heat, and magnetization measurements indicate a moderate-heavy fermion behavior with a Kondo energy scale of the order of 40 K. Most experimental results suggest the absence of magnetic order, but a tiny anomaly in the specific heat opens the possibility for a very weak, itinerant type of ordering. Published by the American Physical Society 2024

SYNTHESIS STRUCTURAL AND MAGNETIC PROPERTIES OF TITANIUM DOPED MAGNESIUM ZINC FERRITE

Magnetic ceramics or ferrites are very well established group of magnetic materials which exhibits ferrimagnetism. It possess high electrical resistivity, low eddy current and dielectric loss which makes it superior than the other ordinary magnetic oxides that contain the ferric oxide (Fe₂O₃) as their basic magnetic compounds. The ceramic magnets are widely used in high frequency transformer application. [(Mg, Mn, F12o4)] spinels are used in square-loop application. Ceramic materials found application in nuclear physics. In nuclear reactors ceramics are used as core components. The studies include the preparation and analysis of Titanium doped Magnesium zinc ferrite. Here, Titanium doped magnesium zinc ferrite nanoparticles (NPS) were synthesized using solid state reaction method. Titanium doping can enhance the magnetic properties of magnesium zinc ferrite in several ways these can contribute to improved magnetic properties , such as increased magnetic moment, saturation magnetization, and magnetic ordering , making titanium – doped magnesium zinc ferrite a promising material for various applications including magnetic storage, sensors, and spintronics. According to the stoichiometric equation [Mg0.9Zn 0.1TixFe2-xO4] at different values of x, (x=0.1, 0.3) are synthesised. Calcination and sintering of the samples is made by high temperature PID controlled muffle furnace which can go up to 1000°C. The structural and magnetic properties are examined using XRD, FTIR and Curie temperature analysis. From the XRD analysis it revels the phase structure and lattice parameters of the samples. XRD analysis gives maximum intensity of (h k l) values as (3 1 1) in both cases. It also reveals that no secondary phases are produced during growth. That means the specimens FCC stacking. FTIR analysis of the samples done using Fourier transformer infrared spectroscopy. From this analysis it revels the detailed atomic structure and bonding of the samples. The bands obtained reveal spinal ferrite structure. Curie temperature of the specimens is determined by Curie temperature apparatus for the study of magnetic properties of the specimens.

Magnetoelectric effect in multiferroic nickelate perovskite YNiO3

The interaction of magnetic order and spontaneous polarization is a fundamental coupling with the prospect for the control of electronic properties and magnetism. The connection among magnetic order, charge localization and associated metal-insulator transition (MIT) are cornerstones for materials control. Materials that combine both effects are therefore of great interest for testing models that claim the occurrence of spontaneous polarization from magnetic and charge order. One class of materials proposed to combine these functionalities is the family of RNiO3 (R: Lanthanide or Yttrium), whose members show a clear MIT and an antiferromagnetic ground state and for which an electric polarization has been predicted. Here, using resonant magnetic x-ray scattering with circular polarization and an applied electric field we show that YNiO3 possess a magnetic structure containing domains of spin-rotations that are consistent with an electric polarization. We show a reversal of the magnetic structure with the applied electric field confirming that charge ordered RNiO3 are magnetoelectric type II multiferroics with a MIT.

Contrasting Magnetic Characteristics of Disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 and 112-Type Ordered NdBaMnFeO6-δ Perovskites.

The magnetic properties of disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 and ordered NdBaMnFeO6-δ perovskites were investigated through temperature- and field-dependent DC-magnetization measurements. The temperature dependence of magnetic susceptibilities revealed that antiferromagnetic ordering occurs at temperatures below 185 K for the disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 sample, whereas the ordered NdBaMnFeO6-δ perovskite exhibited a paramagnetic state throughout the entire temperature range examined. Notably, the disordered sample exhibited a glassy state, even at room temperature, which transformed into an antiferromagnetic state under higher applied magnetic fields. The magnetic ordering in the disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 perovskite and the magnetic-disordering state in the structurally ordered NdBaMnFeO6-δ perovskite could be attributed to the alteration of the oxidation state of Mn.

Measurement of the magnetic octupole susceptibility of PrV2Al20

Revealing the presence of magnetic octupole order and associated octupole fluctuations in solids is a highly challenging task due to the lack of simple external fields that can couple to magnetic octupoles. Here, we demonstrate a methodology for probing the magnetic octupole susceptibility of a candidate material, PrV2Al20, using a product of magnetic field Hi and shear strain ϵjk as a composite effective field, while employing an adiabatic elastocaloric effect to probe the response. We observe Curie-Weiss behavior in the obtained octupolar susceptibility down to approximately 3 K. Although octupole order does not appear to be the leading multipolar channel in PrV2Al20, our results nevertheless reveal the presence of strong magnetic octupole fluctuations and hence demonstrate that octupole order is at least a competing state. More broadly, our results highlight how anisotropic strain can be combined with magnetic fields to probe elusive ‘hidden’ electronic orders.

Anisotropic magnetoresistance in altermagnetic MnTe

Recently, MnTe was established as an altermagnetic material that hosts spin-polarized electronic bands as well as anomalous transport effects like the anomalous Hall effect. In addition to these effects arising from altermagnetism, MnTe also hosts other magnetoresistance effects. Here, we study the manipulation of the magnetic order by an applied magnetic field and its impact on the electrical resistivity. In particular, we establish which components of anisotropic magnetoresistance are present when the magnetic order is rotated within the hexagonal basal plane. Our experimental results, which are in agreement with our symmetry analysis of the magnetotransport components, showcase the existence of an anisotropic magnetoresistance linked to both the relative orientation of current and magnetic order, as well as crystal and magnetic order. Altermagnetism is manifested as a three-fold component in the transverse magnetoresistance which arises due to the anomalous Hall effect.

Magnetic properties and large low-field magnetocaloric effect of RFe2Si2 (R = Ho, Tm) compounds

Nowadays, magnetic refrigerant technology has drawn much attention for its environmental friendliness. Those magnetic materials possessing giant low-field magnetocaloric effect (MCE) performance are of great importance for practical applications, especially at low temperatures. Herein, we present a detailed study on polycrystalline magnetocaloric compounds HoFe2Si2 and TmFe2Si2. HoFe2Si2 exhibits a transition from antiferromagnetic to paramagnetic phase at 2.2 K, while no long-range magnetic ordering is observed in TmFe2Si2 even temperature down to 2 K. For both compounds, they showed large low-field magnetic entropy change (−ΔSM) with the peak values of 10.6 and 7.9 J kg−1 K−1 under field change of 0–2 T for HoFe2Si2 and TmFe2Si2, respectively, which is comparable or even larger than some low-temperature magnetocaloric materials. In addition, the characteristic of second-order magnetic transitions of both compounds were confirmed on basis of Arrott plots and mean-field theory criterion. The low magnetic ordering temperatures, large low-field MCE performance along with the feature of second order phase transition for HoFe2Si2 and TmFe2Si2 indicate that both compounds are promising candidate for magnetic refrigerant materials at liquid helium temperature.

Triplon analysis of magnetic disorder and order in maple-leaf Heisenberg magnet

The nearest-neighbor spin-1/2 Heisenberg model on the maple-leaf lattice formed by hexagons (couplingJh), triangles (couplingJt), and dimers (couplingJd), is investigated in a parameter regime whereJh>0andJt,Jd<0. This investigation aims to identify regions hosting exotic valence-bond solid states. Two potential magnetically disordered ground states are identified, and their stability is assessed through plaquette-triplon mean-field analyses. The resulting quantum phase diagram reveals that at large|Jt|and|Jd|, the system adopts a magnetically disordered dimerized VBS state, while for small|Jd|, it stabilizes a Néel state. A second-order phase transition from the dimerized phase to a Néel phase is observed, which, being Landau-forbidden, suggests the potential presence of exotic phenomena such as a deconfined quantum critical point or the appearance of a quantum spin liquid. This work provides insights into the phase diagram of the nearest-neighbor spin-1/2 Heisenberg model on the maple-leaf lattice and lays the groundwork for further investigations into its intriguing physics.

Self-Stacked 1T-1H Layers in 6R-NbSeTe and the Emergence of Charge and Magnetic Correlations Due to Ligand Disorder.

The emergence of correlated phenomena arising from the combination of 1T and 1H van der Waals layers is the focus of intense research. Here, we synthesize a self-stacked 6R phase in NbSeTe, showing perfect alternating 1T and 1H layers that grow coherently along the c-direction, as revealed by scanning transmission electron microscopy. Angle-resolved photoemission spectroscopy shows a mixed contribution of the trigonal and octahedral Nb bands to the Fermi level. Diffuse scattering reveals temperature-independent short-range charge fluctuations with propagation vector qCO = (0.25 0), derived from the condensation of a longitudinal mode in the 1T layer, while the long-range charge density wave is quenched by ligand disorder. Magnetization measurements suggest the presence of an inhomogeneous, short-range magnetic order, further supported by the absence of a clear phase transition in the specific heat. These experimental analyses in combination with ab initio calculations indicate that the ground state of 6R-NbSeTe is described by a statistical distribution of short-range charge-modulated and spin-correlated regions driven by ligand disorder. Our results demonstrate how natural 1T-1H self-stacked bulk heterostructures can be used to engineer emergent phases of matter.

A complex magnetic study: evidence of spin-glass transition below long-range magnetic ordering and its correlation with renormalization of phonon modes

In this paper, we report a complex magnetic behavior arising due to the interplay of three active magnetic cations (Nd/Sm, Co and Ir), forming 3d-5d-4f magnetic sublattices. The B-site ordered double perovskites Nd2CoIrO6and Sm2CoIrO6were successfully prepared by conventional solid-state method. Detailed structural analysis revealed that both samples crystallized in monoclinic structure with P21/n (No.-14) space group. X-ray photoelectron spectroscopy analysis confirms the presence of multiple oxidation states of Ir (i.e. Ir4+and Ir5+). Both samples show a paramagnetic-ferrimagnetic (TFiM) transition around 100 K, additionally, a low temperature transition is observed at around 10 K in the SCIO sample. This FM-like behavior of the samples is attributed to the antiparallel alignment of the Co2+and Ir4+spins, resulting in FiM ordering. The ac susceptibility analysis confirms a spin glass type transition just below the long-range ordering temperature in NCIO sample, The obtained characteristic flipping time of a single spin from both the law (Power law and Vogel-Fulcher law) and nonzero Vogel-Fulcher temperature (T0≃ 89.1 K) further verified the existence of cluster spin-glass behavior below the ordering temperature. The temperature evolution of phonon modes (up to 4 K) suggests that the phonon mode above the magnetic ordering temperature is mainly governed by the lattice degrees of freedom; notable renormalization of the mode frequency below the ordering temperature is due to the coupling of lattice with the underlying magnetic degrees of freedom.