Spin Arrangement Research Articles

Orbital dependent band degeneracy and edge states in single layer and AA bilayer honeycomb lattice systems with p orbital degeneracy

We have investigated band structure and edge states of single and AA bilayer honeycomb lattice systems with p orbital degeneracy which would be relevant for relatively heavy metals such as Pb and Bi. The p electrons, which are triply degenerate in the atomic limit, form quadruple degeneracy at K point in a single layer honeycomb lattice. The spin-orbit interaction splits the quartet at K point into two singlets and one doublet which are mixtures of p x , p y and p z orbitals. In the AA bilayer honeycomb lattice, the Dirac node at K point is deformed into circular line node around it. With the intermediate interlayer coupling, there is a degenerate point along Γ-K with p z character. A p x /p y type degenerate point exists under the strong interlayer coupling. This degenerate point is robust against the spin-orbit interaction and the antiferromagnetic spin arrangement only along the intralayer bonds. Without SOI, localized edge states with p x /p y or p z character are created at the zigzag edges both in the single and AA bilayer systems. In the AA bilayer system with SOI, only the p x /p y edge states exhibit the Dirac-like dispersion.

Enhanced Alkaline Oxygen Evolution Using Spin Polarization and Magnetic Heating Effects under an AC Magnetic Field.

Renewable electricity from splitting water to produce hydrogen is a favorable technology to achieve carbon neutrality, but slow anodic oxygen evolution reaction (OER) kinetics limits its large-scale commercialization. Electron spin polarization and increasing the reaction temperature are considered as potential ways to promote alkaline OER. Here, it is reported that in the alkaline OER process under an AC magnetic field, a ferromagnetic ordered electrocatalyst can simultaneously act as a heater and a spin polarizer to achieve significant OER enhancement at a low current density. Moreover, its effect obviously precedes antiferromagnetic, ferrimagnetic, and diamagnetic electrocatalysts. In particular, the noncorrected overpotential of the ferromagnetic electrocatalyst Co at 10 mA cm-2 is reduced by a maximum of 36.6% to 243 mV at 4.320 mT. It is found that the magnetic heating effect is immediate, and more importantly, it is localized and hardly affects the temperature of the entire electrolytic cell. In addition, the spin pinning effect established on the ferromagnetic/paramagnetic interface generated during the reconstruction of the ferromagnetic electrocatalyst expands the ferromagnetic order of the paramagnetic layer. Also, the introduction of an external magnetic field further increases the orderly arrangement of spins, thereby promoting OER. This work provides a reference for the design of high-performance OER electrocatalysts under a magnetic field.

Insight into ground-state spin arrangement and bipartite entanglement of the polymeric coordination compound [Dy[formula omitted]Cu[formula omitted]][formula omitted] through the symmetric spin-1/2 Ising–Heisenberg orthogonal-dimer chain

The ground-state spin arrangement and the bipartite entanglement within Cu2+-Cu2+ dimers across the magnetization process of the 4f-3d heterometallic coordination polymer [Dy(hfac)2(CH3OH)2Cu(dmg)(Hdmg)2]n (H2dmg = dimethylglyoxime, Hhfac = 1,1,1,5,5,5-hexafluoropentane-2,4-dione) are theoretically examined using the symmetric isotropic spin-1/2 Ising–Heisenberg orthogonal-dimer chain. The numerical results point to five possible ground states of the compound with three different degrees of the quantum entanglement within Cu2+-Cu2+. Besides the standard ferrimagnetic and saturated phases without quantum entanglement of Cu2+ ions, which are manifested in low-temperature magnetization curve as wide plateaus at the non-saturated magnetization 16.26μB and at the saturation value 20.82μB, respectively, one also finds an intriguing singlet-like phase with just partial entanglement within Cu2+-Cu2+ and two singlet phases with fully entangled Cu2+-Cu2+ dimers. The former quantum phase can be identified in the low-temperature magnetization process as very narrow intermediate plateau at the magnetization 9.27μB per unit cell, while the latter ones as zero magnetization plateau and intermediate plateau at the magnetization 18.54μB. Non-monotonous temperature variations of the concurrence, through which the entanglement within cooper dimers is quantified, point to the possible temporary thermal activation of the entangled states of Cu2+-Cu2+ also above non-entangled ferrimagnetic and saturated phases.

Role of External Stimuli in Engineering Magnetic Phases and Real-Time Spin Dynamics of Co/Mn Oxides.

Magnetism in atomically thin two-dimensional (2D) materials can be easily manipulated by alloying, functionalization, external ultrafast laser pulse, strain, electric field, etc. In this work, we have performed a series of spin-resolved density functional theory calculations on 2D magnetic hexagonal transition-metal oxide alloys, CoMnO4. We have explored different alloy patterns and found the most stable magnetic phases in each pattern, resulting in a stable ferromagnetic (FM) ground state depending upon the pattern. We have used Janus functionalization in these materials to tune the magnetic nature of the system from FM to antiferromagnetic (AFM) states. To further control the spin dynamics, we have applied an ultrafast laser pulse to the Janus systems to explore an AFM-to-FM transition process. Finally, applying strain and electric field to the Janus alloys allows us to tune the structure-property relationship in the 2D layers to obtain desirable spin arrangements.

Giant exchange bias in antiferromagnetic Pr2CoFe0.5Mn0.5O6: a structural and magnetic properties study

Antiferromagnetic (AFM) materials with a colossal exchange bias (EB) effect find applications as high-density spintronic devices. We report structural (geometrical and electronic) and magnetic studies in the polycrystalline Pr2CoFe0.5Mn0.5O6 double perovskite system. The observed lack of training effect suggests the existence of robust EB. In addition, the detailed magnetic studies and Raman studies unravel the Griffith-like phase along with the spin-phonon coupling in the present system. The x-ray photoemission spectroscopy (XPS) analysis supports more than one valence state of B-site elements, which is accountable for the competition between ferromagnetic (FM) and AFM interactions in addition to the anti-site disorder in the system. The neutron measurement confirms the G-type AFM spin arrangement, accredited by the DFT calculation. The magnetic studies have correlated with the electronic structure, neutron study, and theoretical first principle calculations.

Magnetic order and disorder environments in superantiferromagnetic hbox {NdCu}_{mathbf{2}} nanoparticles

Magnetic nanoparticles exhibit two different local symmetry environments, one ascribed to the core and one corresponding to the nanoparticle surface. This implies the existence of a dual spin dynamics, leading to the presence of two different magnetic arrangements governed by different correlation lengths. In this work, two ensembles of hbox {NdCu}_{2} nanoparticles with mean sizes of 18 nm and 13 nm have been produced to unravel the magnetic couplings established among the magnetic moments located within the core and at the nanoparticle surface. To this end, we have combined neutron diffraction measurements, appropriate to investigate magnetically-ordered spin arrangements, with time-dependent macroscopic AC susceptibility measurements to reveal memory and aging effects. The observation of the latter phenomena are indicative of magnetically-frustrated states. The obtained results indicate that, while the hbox {Nd}^{3{+}} magnetic moments located within the nanoparticle core keep the bulk antiferromagnetic commensurate structure in the whole magnetic state, the correlations among the surface spins give rise to a collective frustrated spin-glass phase. The interpretation of the magnetic structure of the nanoparticles is complemented by specific-heat measurements, which further support the lack of incommensurability in the nanoparticle state.

Real-Time Observation of Magnetic Domain Structure Changes with Increasing Temperature for Z-Type Hexagonal Ferrite.

Z-type hexagonal ferrites have recently received attention for their room-temperature magnetoelectric (ME), which is activated when the temperature at which the transverse-conical spin-state transitions to a ferrimagnetic state is increased. The changes in the magnetic domain structure at the transition have been well-documented; however, they are still not understood in detail. In the present study, Lorentz transmission electron microscopy (TEM) analysis combined with an in situ heating experiment was conducted to demonstrate the shift in magnetic domain structure during the transition from the transverse-conical spin arrangement to a ferrimagnetic spin order. The dynamics of the magnetic domain structure changes with the increasing temperature were acquired in real-time. At 490 K, the magnetization transition from the transverse-conical spin state to the ferromagnetic state was demonstrated. Cross-tie domain walls formed during the magnetic transition process. The increased effect of the demagnetizing field applied to the 180° magnetic domains was caused by a lower magnetocrystalline anisotropy (MCA) at the easy axis of magnetization.

Enhanced magnetism and suppressed magnetoelastic coupling induced by electron doping in Ca1− x Y x MnReO6

The Ca2MnReO6 double perovskite is a spin–orbit-assisted Mott insulator with exotic magnetic properties, including a largely non-collinear Mn2+ spin arrangement and nearly orthogonal coupling between such spins and the much smaller Re 5d magnetic moments. Here, the electron-doped compound Ca1−x Y x MnReO6 (x = 0.1, 0.2 and 0.3) is reported and a detailed investigation is conducted for x = 0.3. Neutron and x-ray powder diffraction confirm that nearly full chemical order is maintained at the Mn and Re sites under the Y substitution at the Ca site. X-ray absorption measurements and an analysis of the Mn–O/Re–O bond distances show that the Mn oxidation state remains stable at +2 whereas Re is reduced upon doping. The electron doping increases the magnetic ordering temperature from T c = 121 to 150 K and also enhances significantly the ferromagnetic component of the Mn spins at the expense of the antiferromagnetic component at the base temperature (T = 3 K). The lattice parameter anomalies at T c observed in the parent compound are suppressed by the electron doping. The possible reasons for the enhanced magnetism and the suppressed magnetoelastic coupling in Ca1.7Y0.3MnReO6 are discussed.

Revisiting the antiferromagnetic structure of Tb14Ag51: the importance of distinguishing alternative symmetries for a multidimensional order parameter

The antiferromagnetic structure of Tb14Ag51 with the propagation vector [1/3, 1/3, 0] and the parent space group P6/m is revisited using both magnetic symmetry and irreducible representation arguments. A new magnetic structure under the hexagonal Shubnikov magnetic space group P 6′ which fits much better the experimental data is found. This new solution was obtained by constraining the spin arrangement to one of the three possible magnetic space groups of maximal symmetry that can be realized by a magnetic ordering transforming according to the four-dimensional physically irreducible representation that is known to be relevant in this magnetic phase. The refined model, parameterized under P 6′, implicitly includes the presence of a third harmonic with the propagation vector at the gamma point [0, 0, 0], which has an important weight in the final result. The structure consists of 13 symmetry-independent Tb magnetic moments with the same size of 8.48 (2) μB, propagating cycloidally in the ab plane. The modulation has a substantial deviation from being purely sinusoidal due to the contribution of the mentioned third harmonic.

Electron density distribution influencing the electrical and magnetic properties of polycrystalline Bi0.9Sm0.1FeO3 ceramics

Abstract This article reports the structural properties that influence the electrical and magnetic behaviours of polycrystalline Bi1−x Sm x FeO3 (x = 0, 0.1) ceramics. The samples are synthesized by a two-step solid state reaction. X-ray diffraction patterns expose two characteristic peaks corresponding to (104) and (110) planes around 31°. Bi1−x Sm x FeO3 (x = 0, 0.1) samples crystalize primarily in the R3c phase along with the traces of secondary phases. The Rietveld refinement analysis reveals that the tilt angle of Bi0.9Sm0.1FeO3 reduces due to the twisting of FeO6 octahedra compared to pristine BiFeO3. The electron density distribution and type of bonding are analyzed using the maximum entropy method. The microstructural analysis reveals that the Bi0.9Sm0.1FeO3 sample has a reduced average particle size compared to pristine BiFeO3. The influence of samarium ions in the bismuth site deviates the canting angle of the modulated spiral spin arrangement and the charge density distribution of the Bi0.9Sm0.1FeO3 sample as a result, the electrical and magnetic behaviours are improved compared with bare BiFeO3.

Spin coupling in Ag film growth on Sn/Ge(111)-[formula omitted

Silver has been deposited on the Sn/Ge(111)-(3×3)-R30° surface at room temperature. The Ag growth and resulting surface morphology have been investigated using scanning tunneling microscopy. The first layer of silver forms an interface with domains of two different phases. One structure consists of short atomic rows with three-fold symmetry, oriented in the directions of the 3×3 surface. These rows are separated by a distance equal to 3 and are found to fit a 23×3 unit cell. The other phase is a 3×3 honeycomb structure, oriented in the Ge(111) 1 × 1 directions. Atomic structural models for the two interface phases are proposed, based on two different spin arrangements of the Sn/Ge(111)-3×3 surface. The results highlight the topological coupling of the two interface faces. Both interface structures are preserved with additional silver deposition. The second layer of Ag grows with a bulk-like lattice thickness on top of both interfaces. Low-energy electron diffraction on a mostly two layer Ag film reveals that it consists of domains where Ag grows in different orientations. These domains are rotated 30° with respect to each other, and thus mirror the symmetry directions of the two interfacial phases.

Magnetism of two-dimensional honeycomb layered Na2Ni2TeO6 driven by intermediate Na-layer crystal structure

The microscopic spin-spin correlations in the 2D layered spin-1 honeycomb lattice compound Na2Ni2TeO6 have been investigated by neutron diffraction and inelastic neutron scattering. The honeycomb lattice of spin-1 Ni2+ ions, within the crystallographic ab planes, are well separated along the c axis by an intermediate Na layer whose crystal structure contains chiral nuclear density distributions of Na ions. The chirality of the alternating Na layers is opposite. Such alternating chirality of the Na layer dictates the magnetic periodicity along the c axis where an up-up-down-down spin arrangement of the in-plane zigzag AFM structure is found. Besides, the above described commensurate (CM) zigzag AFM order state is found to coexist with an incommensurate (ICM) AFM state below the TN ~ 27.5 K. The ICM state is found to appear at much higher temperature ~ 50 K and persists down to lowest measured temperature of 1.7 K. Our reverse Monte Carlo (RMC) analysis divulges a two dimensional (2D) magnetic correlations (within the ab plane) of the ICM AFM state over the entire temperature range 1.7-50 K. Further, the spin-Hamiltonian has been determined by carrying out inelastic neutron scattering experiments and subsequent linear spin-wave theory analysis which reveals the presence of competing inplane exchange interactions up to 3 rd nearest neighbours consistent with the zigzag AFM ground state, and weak interplanar interaction as well as a weak single-ion-anisotropy. The values of the exchange constants yield that Na2Ni2TeO6 is situated well inside the zigzag AFM phase (spans over a wide ranges of J2/J1 and J3/J1 values) in the theoretical phase diagram. The present study, thus, provides a detailed microscopic understanding of the magnetic correlations and divulges the intertwining magneto-structural correlations.

Mixed magnetic edge states in graphene quantum dots

Graphene quantum dots (GQDs) exhibit abundant magnetic edge states with promising applications in spintronics. Hexagonal zigzag GQDs possess a ground state with an antiferromagnetic (AFM) inter-edge coupling, followed by a metastable state with ferromagnetic (FM) inter-edge coupling. By analyzing the Hubbard model and performing large-scale spin-polarized density functional theory calculations containing thousands of atoms, we predict a series of new mixed magnetic edge states of GQDs arising from the size effect, namely mix-n, where n is the number of spin arrangement parts at each edge, with parallel spin in the same part and anti-parallel spin between adjacent parts. In particular, we demonstrate that the mix-2 state of bare GQDs (C) appears when and the mix-3 state appears when , where N is the number of six-membered-ring at each edge, while the mix-2 and mix-3 magnetic states appear in the hydrogenated GQDs with N = 13 and N = 15, respectively.

Observation of a 1/3 magnetization plateau in Pb2Cu10O4(SeO3)4Cl7 arising from (Cu2+)7 clusters of corner-sharing (Cu2+)4 tetrahedra.

A mixed-valence compound Pb2Cu10O4(SeO3)4Cl7 has a complex structure consisting of one nonmagnetic Cu+ (S = 0) ion and four nonequivalent magnetic Cu2+ (S = 1/2) ions. It exhibits antiferromagnetic ordering at TN = 10.2 K. At a temperature below TN, a sequence of spin-flop transition at Bspin-flop = 1.3 T and 1/3 plateau formation at Bspin-flip = 4.4 K is observed in the magnetization curve M(B). The 1/3 magnetization plateau persists at least up to 53.5 T. The spin exchanges of Pb2Cu10O4(SeO3)4Cl7 evaluated by performing energy-mapping analysis based on DFT+U calculations show that the magnetic properties of Pb2Cu10O4(SeO3)4Cl7 are described by the (Cu2+)7 cluster of corner-sharing (Cu2+)4 tetrahedra, and that each (Cu2+)7 cluster has a S = 3/2 spin arrangement in the ground state. The 1/3 magnetization plateau observed for Pb2Cu10O4(SeO3)4Cl7 is explained by the field-induced flip of every second (Cu2+)7 cluster within a unit cell.

Edge-state-induced magnetism in two-dimensional hematene

The row-wise spin arrangement and edge state make hematene ribbons with width of odd numbers of atoms show magnetic order near room temperature.

Insight into Ground-State Spin Arrangement and Bipartite Entanglement of the Polymeric Coordination Compound [Dy2cu2]N Through the Symmetric Spin-1/2 Ising-Heisenberg Orthogonal-Dimer Chain

Insight into Ground-State Spin Arrangement and Bipartite Entanglement of the Polymeric Coordination Compound [Dy2cu2]N Through the Symmetric Spin-1/2 Ising-Heisenberg Orthogonal-Dimer Chain

Ground State, Magnetization Process and Bipartite Quantum Entanglement of a Spin-1/2 Ising-Heisenberg Model on Planar Lattices of Interconnected Trigonal Bipyramids.

The ground state, magnetization scenario and the local bipartite quantum entanglement of a mixed spin- Ising–Heisenberg model in a magnetic field on planar lattices formed by identical corner-sharing bipyramidal plaquettes is examined by combining the exact analytical concept of generalized decoration-iteration mapping transformations with Monte Carlo simulations utilizing the Metropolis algorithm. The ground-state phase diagram of the model involves six different phases, namely, the standard ferrimagnetic phase, fully saturated phase, two unique quantum ferrimagnetic phases, and two macroscopically degenerate quantum ferrimagnetic phases with two chiral degrees of freedom of the Heisenberg triangular clusters. The diversity of ground-state spin arrangement is manifested themselves in seven different magnetization scenarios with one, two or three fractional plateaus whose values are determined by the number of corner-sharing plaquettes. The low-temperature values of the concurrence demonstrate that the bipartite quantum entanglement of the Heisenberg spins in quantum ferrimagnetic phases is field independent, but twice as strong if the Heisenberg spin arrangement is unique as it is two-fold degenerate.

Suppression of the Cycloidal Spin Arrangement in BiFeO3 Caused by the Mechanically Induced Structural Distortion and Its Effect on Magnetism

Bismuth ferrite (BiFeO3) particles are prepared by a combined mechanochemical−thermal processing of a Bi2O3 + α-Fe2O3 mixture. Structural, magnetic, hyperfine, morphological and chemical properties of the as-prepared BiFeO3 are studied using X-ray diffraction (Rietveld refinement), 57Fe Mössbauer spectroscopy, SQUID magnetometry, electron microscopy and energy dispersive X-ray spectroscopy. It is revealed that the structure of the ferrite exhibits the long-range distortion (significantly tilted FeO6 octahedra) and the short-range disorder (deformed FeO6 octahedra). Consequently, these structural features result in the suppression of a space modulated cycloidal spin arrangement in the material. The latter manifests itself by the appearance of only single spectral component in the 57Fe Mössbauer spectrum of BiFeO3. The macroscopic magnetic behavior of the material is interpreted as a superposition of ferromagnetic and antiferromagnetic contributions with a large coercive field and remanent magnetization. Taking into account the average particle size of the as-prepared BiFeO3 particles (∼98 nm), exceeding the typical period length of cycloid (∼62 nm), both the suppression of the spiral spin structure in the material and its partly ferromagnetic behavior are attributed to the crystal lattice distortion caused by mechanical stress during the preparation procedure.

Magnetic properties of the intercalated compoundLu2Fe3O7

Complex spin and charge order in the frustrated Fe/O bilayers of rare-earth ferrites $R$Fe${}_{2}$O${}_{4}$ and proposed multiferroicity for $R$ = Lu have attracted a lot of interest. The authors focus on $i\phantom{\rule{0}{0ex}}n\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}e\phantom{\rule{0}{0ex}}r\phantom{\rule{0}{0ex}}c\phantom{\rule{0}{0ex}}a\phantom{\rule{0}{0ex}}l\phantom{\rule{0}{0ex}}a\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}e\phantom{\rule{0}{0ex}}d$ Lu${}_{2}$Fe${}_{3}$O${}_{7}$, with additional Fe/O single layers inserted between the bilayers. Macroscopic magnetization measurements, polarized neutron scattering, and x-ray magnetic circular dichroism indicate that spin-charge coupling and the local spin arrangement in each individual bilayer is the same as in the nonintercalated compound, with the Fe spins in the single layers giving rise to an additional paramagneticlike contribution.

Structural, electronic and magnetic properties of weakly correlated metal Sr2CrTiO6: a first principles study

Structural, electronic and magnetic behaviour of a less-explored material Sr2CrTiO6 has been investigated using ab initio calculations with generalized gradient approximation (GGA) and GGA + U methods, where U is the Hubbard parameter. For each of the three possible Cr/Ti cationic arrangements in the unit cell, considered in this work, the non-magnetic band structure shows distinct traits with significant flat-band regions leading to large t 2g density of states around the Fermi energy. The Cr4+ ion in Sr2CrTiO6, which is a d 2 system, shows a reverse splitting of the t 2g orbitals. The calculated hopping matrix contains non-zero off-diagonal elements between the d xz and d yz orbitals, while the d xy orbitals remain largely unmixed. A minimal tight binding model successfully reproduces the six t 2g bands around the Fermi energy. The Fermi surface shows a two-dimensional nesting feature for the layered arrangement of Cr and Ti atoms. Fixed spin moment studies suggest that the magnetism in this compound cannot be explained by Stoner’s criterion of an itinerant band ferromagnet. In the absence of Hubbard U term, the ground state is a half-metallic ferromagnet. Calculations for the anti-ferromagnetic spin arrangement show re-arrangement of orbital character resulting in (a) narrow d xz /d yz bands and sharp peaks in the density of states at the Fermi energy and (b) highly dispersive d xy bands with a broader density of states around the Fermi energy. The metallicity persists even with increasing U for both the spin arrangements, thus suggesting that Sr2CrTiO6 belongs to the class of weakly correlated metals, while the shifting of O 2p states towards the Fermi energy with U indicates a negative charge-transfer character in Sr2CrTiO6.