Spin Arrangement Research Articles

Observation of collinear antiferromagnetic domains making use of the circular dichroic charge-magnetic interference effect of resonant x-ray diffraction

The circular dichroic charge-magnetic interference effect in resonant x-ray diffraction (RXD) is reported for antiferromagnetic (AFM) materials. The polarization dependence of the scattering cross-section was formulated, and the conditions that the interference gives rise to circular dichroic RXD signals for AFM materials were clarified. By using the interference effect, a pair of AFM domains can be distinguished in certain conditions. We applied this effect to observe collinear chirality AFM domains in a high-temperature magnetoelectric hexaferrite, $\mathrm{B}{\mathrm{a}}_{1.3}\mathrm{S}{\mathrm{r}}_{0.7}\mathrm{CoZnF}{\mathrm{e}}_{11}\mathrm{Al}{\mathrm{O}}_{22}$. Despite its collinear spin arrangement and absence of macroscopic magnetization, the domains are clearly visualized by a circularly polarized x-ray beam. The present result shows that various types of AFM domains including collinear ones can be examined by utilizing the charge-magnetic interference effect, together with the well-established circular dichroism on RXD emerged from pure magnetic scattering.

Two-dimensional triangular-lattice Cu(OH)Cl, belloite, as a magnetodielectric system

Quantum spins on a triangular lattice may bring out intriguing and exotic quantum ground states. Here we report a magnetodielectric system of CuOHCl wherein $S=1/2\mathrm{C}{\mathrm{u}}^{2+}$ spins constitute a two-dimensional triangular lattice with the layers weakly coupled via Cl-H-O bonding. Despite strong magnetic interactions, as expected from the relatively high value of ${\ensuremath{\theta}}_{\mathrm{CW}}=\ensuremath{-}100\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, antiferromagnetic transition occurred at ${T}_{N}=11\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, followed by an uprising turn of the magnetic susceptibility below \ensuremath{\sim}7 K. Neutron-diffraction experiment revealed a coplanar spin structure on the triangular lattice below the ${T}_{N}$, with each spin pointing toward the center of a triangle. Of the three spins on a triangle, two are antiparallel and the third one is angled ${120}^{\ensuremath{\circ}}$ to the antiparallel spins. A concerted effect of geometric frustration in the triangular lattice and superexchange interactions through a zig-zag path via double Cu-O-Cu and double Cu-Cl-Cu bridges counted for this spin arrangement. Further investigation using dielectric constant and heat capacity measurements, as well as a microscopic probe of muon spin rotation, revealed a magnetodielectric effect and the possibility of multiferroic transition at ${T}^{*}\ensuremath{\sim}5\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, which is suspected to be in close relation to geometric frustration in this triangular lattice. The present paper presents a magnetodielectric system on a two-dimensional triangular lattice with chemical stoichiometry. It can also serve as a rare reference to the hotly debated quantum spin-orbital liquid compound $\mathrm{LiNi}{\mathrm{O}}_{2}$.

Synthesis, Structure, and Physical Properties of the Polar Magnet DyCrWO6.

It has recently been reported that the ordered aeschynite-type polar ( Pna21) magnets RFeWO6 (R = Eu, Tb, Dy, Y) exhibit type II multiferroic properties below TN ∼ 15-18 K. Herein, we report a comprehensive investigation of the isostructural oxide DyCrWO6 and compare the results with those of DyFeWO6. The cation-ordered oxide DyCrWO6 crystallizes in the same polar orthorhombic structure and undergoes antiferromagnetic ordering at TN = 25 K. Contrary to DyFeWO6, only a very weak dielectric anomaly and magnetodielectric effects are observed at the Néel temperature and, more importantly, there is no induced polarization at TN. Furthermore, analysis of the low-temperature neutron diffraction data reveals a collinear arrangement of Cr spins but a noncollinear Dy-spin configuration due to single-ion anisotropy. We suggest that the collinear arrangement of Cr spins may be responsible for the absence of electric polarization in DyCrWO6. A temperature-induced magnetization reversal and magnetocaloric effects are observed at low temperatures.

Dependence of characteristic interlayer vibration modes on interlayer spin arrangement in stacked graphene nanofragments

The freedom of interlayer spin arrangement could emerge when assembling small-sized graphene-based nanostructures through stacking. Its possible influence on interlayer vibrations could be significant for developing Raman probes towards small complexes and device design involving intermolecular vibronic process. In this paper, using density-functional-theory calculations on bilayer and trilayer rhombic graphene fragments, we compare finite-size analogues to interlayer shear and breathing modes regarding to ferromagnetic and antiferromagnetic interlayer spin arrangements. For bilayer units, the antiferromagnetic configuration further separate two shear mode components by around 10 cm−1, inducing a further Raman peak splitting. This response is robust regarding to slightly enlarging the fragment and increasing layer number to three. Layer breathing mode is spin-arrangement robust in bilayers but show different arrangement-sensitivity in ABA-like and ABC-like trilayers. Visualization of interface electron density reveals the dependence of anisotropic interface environment to interlayer spin arrangement and unambiguously correlates the arrangement style with shearing responses. Further application of this analysis clarifies the arrangement-based phase-cooperation in trilayer shearing. Results and analysis in this work may contribute to the characterization and design of graphene-based nanostructures as well as understanding the interfacial nature beneath their intermolecular varieties in dynamic processes.

Defect-driven extreme magnetoresistance in an I-Mn-V semiconductor.

The search for appropriate materials for technological applications is challenging, as real materials are subject to uncontrolled doping and thermal effects. Tetragonal NaMnBi of the I-Mn-V class of antiferromagnetic semiconductors with a Néel transition (), above room temperature, can exhibit an extreme magnetoresistance (MR), greater than 10000% at 2K and 600% at room temperature and 9T by quenching disorder into the system. Coupled with the large MR is a re-orientation of the magnetic moment, from a collinear spin arrangement along c to a canted one along the (011) crystallographic axis. The extreme MR is observed in samples with about 15% of Bi vacancies which in turn effectively introduces charge carriers into the lattice, leading to a drastic change in the electronic transport, from semiconducting to metallic, and to the very large MR under the magnetic field. In the absence of Bi defects, the MR is severely suppressed, suggesting that the hybridization of the Mn and Bi orbitals may be key to the field induced large MR. This is the only material of its class that exhibits the extreme MR and may potentially find use in microelectronic devices.

Effective damping enhancement in noncollinear spin structures

Damping mechanisms in magnetic systems determine the lifetime, diffusion and transport properties of magnons, domain walls, magnetic vortices, and skyrmions. Based on the phenomenological Landau-Lifshitz-Gilbert equation, here the effective damping parameter in noncollinear magnetic systems is determined describing the linewidth in resonance experiments or the decay parameter in time-resolved measurements. It is shown how the effective damping can be calculated from the elliptic polarization of magnons, arising due to the noncollinear spin arrangement. It is concluded that the effective damping is larger than the Gilbert damping, and it may significantly differ between excitation modes. Numerical results for the effective damping are presented for the localized magnons in isolated skyrmions, with parameters based on the Pd/Fe/Ir(111) model-type system.

Structural, magnetic, and electron-transport properties of epitaxial Mn2PtSn films

The growth of new magnetic materials on suitable insulating substrates is an important part of the development of spin-electronics devices for memory or information processing. Epitaxial thin films of Mn2PtSn were grown on a MgO [001] substrate by magnetron co-sputtering of the constituents. Structural, magnetic, and electron-transport properties were investigated. The epitaxial Mn2PtSn film has an inverse tetragonal structure with the c-axis aligned in the plane of the MgO substrate. The lattice constants determined using XRD and TEM analysis are c = 6.124 Å and a = b = 4.505 Å. The orientation of Mn2PtSn c-axis which is 45° away from the a-axis of MgO has resulted in a small lattice mismatch of about 2.8%. The measured saturation magnetization is 5.3 μB/f.u., which is smaller than the first-principles calculated value of 6.4 μB/f.u. for ferromagnetic spin arrangement. Magnetization measurements determined the bulk magnetocrystalline anisotropy constant Kv of about 11.3 Merg/cm3 (1.13 MJ/m3). The electron-transport behavior is similar to that of normal magnetic metals. These results indicate that Mn2PtSn may have promising applications in spintronic devices.

Anharmonic Magnon Excitations in Noncollinear and Charge-Ordered RbFe^{2+}Fe^{3+}F_{6}.

RbFe^{2+}Fe^{3+}F_{6} is an example of a charge ordered antiferromagnet where iron sites, with differing valences, are structurally separated into two interpenetrating sublattices. The low temperature magnetically ordered Fe^{2+} (S=2) and Fe^{3+} (S=5/2) moments form a noncollinear orthogonal structure with the Fe^{3+} site displaying a reduced static ordered moment. Neutron spectroscopy on single crystals finds two distinct spin wave branches with a dominant coupling along the Fe^{3+} chain axis (b axis). High resolution spectroscopic measurements find an intense energy and momentum broadened magnetic band of scattering bracketing a momentum-energy region where two magnon processes are kinematically allowed. These anharmonic excitations are enhanced in this noncollinear magnet owing to the orthogonal spin arrangement.

Ferromagnetic resonance in core-shell nanoparticles with multitype exchange anisotropy

A phenomenological model for magnetodynamics of core-shell nanoparticles is presented. The term core-shell implies, prima facie, that the spin structures (phases) of the particle components are different, no matter whether or not they are chemically identical. The model takes in two main assumptions. First, the interphase boundary is a thin (in comparison with the core and shell scales) transition layer with strongly inhomogeneous spin arrangement. Second, the shell is a granular structure consisting of spin-ordered crystallites with a wide spread of internal anisotropy, including a fraction of ones with extremely high coercivity. The framework developed on that basis, despite its simplicity, provides a unified explanation for the major specific properties of magnetic core-shell particles. Namely, (i) the growth of observed anisotropy field with reduction of the particle size, (ii) the presence of fixed unidirectional anisotropy, and (iii) the existence of rotatable anisotropy that emerges in a threshold manner under an external field. For a nanoparticle with the above-described core-shell architecture, a theory of ferromagnetic resonance with allowance for the superparamagnetic effect is worked out, and the ferromagnetic resonance absorption lines of noninteracting ensembles of such particles are presented. It is demonstrated that all the qualitatively different contributions to the core-shell-induced anisotropy could be evaluated from the data on a temperature sweep of the resonance field. Moreover, to do that, it suffices to use just the samples with random orientation of the particle axes. Preliminary assessment shows that a set of measurements for complete evaluation of the exchange-mediated anisotropies is feasible with the aid of a standard $X$-band spectrometer.

Simultaneous Modulation of Magnetic and Dielectric Transition via Spin‐Crossover‐Tuned Spin Arrangement and Charge Distribution

AbstractMagnetic and dielectric properties have been tuned simultaneously by external stimuli with rapid and sensitive response, which is crucial to monitor the magnetic state via capacitive measurement. Herein, positive charged FeII ions were linked via negative charged [(Tp)FeIII(CN)3]− (Tp=hydrotris(pyrazolyl)borate) units to form a neutral chain. The spin‐crossover (SCO) on FeII sites could be sensitively triggered via thermal treatment, light irradiation, and pressure. SCO switched the spin state of the FeII ions and antiferromagnetic interactions between FeIII and FeII ions, resulting in significant change in magnetization. Moreover, SCO induced rotation of negative charged [(Tp)FeIII(CN)3]− units, generating dielectric anomaly due to geometric change of charges distribution. This work provides a rational way to manipulate simultaneous variations in magnetic and dielectric properties utilizing SCO as an actuator to tune spin arrangement, magnetic coupling, and charge distribution.

Simultaneous Modulation of Magnetic and Dielectric Transition via Spin‐Crossover‐Tuned Spin Arrangement and Charge Distribution

Magnetic and dielectric properties have been tuned simultaneously by external stimuli with rapid and sensitive response, which is crucial to monitor the magnetic state via capacitive measurement. Herein, positive charged FeII ions were linked via negative charged [(Tp)FeIII (CN)3 ]- (Tp=hydrotris(pyrazolyl)borate) units to form a neutral chain. The spin-crossover (SCO) on FeII sites could be sensitively triggered via thermal treatment, light irradiation, and pressure. SCO switched the spin state of the FeII ions and antiferromagnetic interactions between FeIII and FeII ions, resulting in significant change in magnetization. Moreover, SCO induced rotation of negative charged [(Tp)FeIII (CN)3 ]- units, generating dielectric anomaly due to geometric change of charges distribution. This work provides a rational way to manipulate simultaneous variations in magnetic and dielectric properties utilizing SCO as an actuator to tune spin arrangement, magnetic coupling, and charge distribution.

Itinerant fermions on a triangular lattice: Unconventional magnetism and other ordered states

We consider a system of 2D fermions on a triangular lattice with well separated electron and hole pockets of similar sizes, centered at certain high-symmetry-points in the Brillouin zone. We first analyze Stoner-type spin-density-wave (SDW) magnetism. We show that SDW order is degenerate at the mean-field level. Beyond mean-field, the degeneracy is lifted and is either $120^{\circ}$ "triangular" order (same as for localized spins), or a collinear order with antiferromagnetic spin arrangement on two-thirds of sites, and non-magnetic on the rest of sites. We also study a time-reversal symmetric directional spin bond order, which emerges when some interactions are repulsive and some are attractive. We show that this order is also degenerate at a mean-field level, but beyond mean-field the degeneracy is again lifted. We next consider the evolution of a magnetic order in a magnetic field starting from an SDW state in zero field. We show that a field gives rise to a canting of an SDW spin configuration. In addition, it necessarily triggers the directional bond order, which, we argue, is linearly coupled to the SDW order in a finite field. We derive the corresponding term in the Free energy. Finally, we consider the interplay between an SDW order and superconductivity and charge order. For this, we analyze the flow of the couplings within parquet renormalization group (pRG) scheme. We show that magnetism wins if all interactions are repulsive and there is little energy space for pRG to develop. However, if system parameters are such that pRG runs over a wide range of energies, the system may develop either superconductivity or an unconventional charge order, which breaks time-reversal symmetry.

Magnetophononics: Ultrafast spin control through the lattice

Using a combination of first-principles and magnetization-dynamics calculations, we study the effect of the intense optical excitation of phonons on the magnetic behavior in insulating magnetic materials. Taking the prototypical magnetoelectric \CrO\ as our model system, we show that excitation of a polar mode at 17 THz causes a pronounced modification of the magnetic exchange interactions through a change in the average Cr-Cr distance. In particular, the quasi-static deformation induced by nonlinear phononic coupling yields a structure with a modified magnetic state, which persists for the duration of the phonon excitation. In addition, our time-dependent magnetization dynamics computations show that systematic modulation of the magnetic exchange interaction by the phonon excitation modifies the magnetization dynamics. This temporal modulation of the magnetic exchange interaction strengths using phonons provides a new route to creating non-equilibrium magnetic states and suggests new avenues for fast manipulation of spin arrangements and dynamics.

Tailoring the structural and magnetic properties of Co-Zn nanosized ferrites for hyperthermia applications

A comparative study of the magnetic properties (magnetic moment, magnetocrystalline anisotropy) and hyperthermia response in Co-Zn spinel nanoparticles is presented. The CoxZn1−xFe2O4 nanoparticles (x = 1, 0.5, 0.4, 0.3, 0.2 and 0.1) were synthesized by co-precipitated method and the morphology and mean crystallite size (around 10 nm) of the nanoparticles were analysed by TEM Microscopy. Regarding the magnetic characterization (SQUID magnetometry), Co-Zn nanoparticles display at room temperature anhysteretic magnetization curves, characteristic of the superparamagnetic behavior. A decrease in the blocking temperature, TB, with Zn content is experimentally detected that can be ascribed to the reduction in the mean nanoparticle size as x decreases. Furthermore, the reduction in the magnetocrystalline anisotropy with Zn inclusion is confirmed through the analysis of TB versus the mean volume of the nanoparticles and the law of approach to saturation. Maximum magnetization is achieved for x = 0.5 as a result of the cation distribution between octahedral and tetrahedral spinel sites, analysed by neutron diffraction studies. The occurrence of a canted spin arrangement (Yafet-Kittel angle) is introduced to properly fit the magnetic spinel structures. Finally, the heating capacity of these spinel ferrites is analyzed under ac magnetic field (magnetic hyperthermia). Maximum SAR (Specific Absorption Rate) values are achieved for x = 0.5 that should be correlated to the maximum magnetic moment of this composition.

Surface anisotropy induced magnetism in BaTiO3-CoFe2O4 (BTO-CFO) nanocomposite

Nanocomposite of BaTiO3 (BTO) and CoFe2O4 (CFO) exhibits magnetism which can be explained by assuming the surface interaction between BTO and CFO. The crystal phase of the nanocomposite has been studied by the X-ray diffraction (XRD) technique which has been supported by the Raman spectra analysis. Surface morphology has been studied using SEM (scanning electron microscopy) and TEM (Transmission electron microscopy). The ball milling has transformed diamagnetic microcrystalline of BTO to nanocrystal ferromagnetic BTO which could be due to oxygen vacancies at the surface of BTO. Thus there has been ferromagnetic exchange interaction between nanocrystalline BTO and CFO at their interfaces which ultimately affect the spin arrangement at the surface of CFO. This interaction leads to high saturation magnetization. A hump in the M–H loop at around ±4000 Oe has been observed for the BTO-CFO composites. It changes its shape with the increase in concentration of CFO. It is probably due to increase of superexchange interaction between CFO and BTO at the interface.

Spontaneous symmetry breaking and electronic and dielectric properties in commensurate La7/4Sr1/4CuO4 and La5/3Sr1/3NiO4

Complex ordered phases involving spin and charge degrees of freedom in condensed matter, such as layered cuprates and nickelates, are exciting but not well understood solid-state phenomena. The rich underlying physics of the overdoped high-temperature superconductor $\mathrm{L}{\mathrm{a}}_{7/4}\mathrm{S}{\mathrm{r}}_{1/4}\mathrm{Cu}{\mathrm{O}}_{4}$ and colossal dielectric constant insulator $\mathrm{L}{\mathrm{a}}_{5/3}\mathrm{S}{\mathrm{r}}_{1/3}\mathrm{Ni}{\mathrm{O}}_{4}$ is studied from first principles within density functional (perturbation) theory, including an effective Hubbard potential $U$ for the exchange and correlation of $d$ orbitals. Charge density wave (CDW) and spin density wave (SDW) orders are found in both materials, where the stripes are commensurate with the lattice. The SDWs are accompanied by complex antiferromagnetic spin arrangements along the stripes. The first series of conduction bands related to the pseudogap observed in the cuprate are found to be directly related to CDW order, while the colossal dielectric constant in the nickelate is demonstrated to be a result of vibronic coupling with CDW order. Differences between the two oxides are related to how the stripes fill with carriers.

Crystal and Magnetic Structures of the Chain Antiferromagnet CaFe4Al8.

The crystal structure of CaFe4Al8 was studied by X-ray single crystal and powder diffraction as well as high-resolution neutron powder diffraction. CaFe4Al8 crystallizes with a tetragonal CeMn4Al8-type structure, an ordered variant of the ThMn12-type (Pearson symbol tI26, space group I4/ mmm, a = 8.777(1), c = 5.077(1) Å). Similarly to the well-known A15-type superconductors, the structure of CaFe4Al8 contains one-dimensional chains of d-metal atoms, which are parallel to the crystallographic fourfold axis. CaFe4Al8 is paramagnetic at room temperature and exhibits long-range antiferromagnetic ordering at about 180 K, combined with a short-range ordered spin arrangement. The magnetic structure, determined by powder neutron diffraction at 4 K, shows that the magnetic moments on the Fe atoms form mirror-inverted chains along the c-direction and are slightly canted from the axis.

Zeeman-magnetic-field–induced magnetic phase transition in doped armchair boron-nitride nanoribbons

In this work, the magneto-charge structure factor (CSF) of hexagonal doped armchair boron-nitride nanoribbons (ABNNRs) has been addressed using the tight-binding Hamiltonian model and the Green's function technique. In particular, we study the charge static susceptibility in the presence of the Zeeman magnetic field. The calculations of the correlation function of charge densities lead to magnetic phase transitions, which are explained by the temperature-dependent magneto-CSF. We have observed different width-dependent CSF treatments in the presence and absence of magnetic field for both undoped and doped ABNNRs. Depending on the magnetic field strength, transitions from antiferromagnetic to the ferromagnetic (paramagnetic) arrangement of spins has been established for undoped (doped) ABNNRs. We have found that, furthermore, in addition to the magnetic field, the magnetic phase can be controlled by the concentration and incoming momentum of electronic dopants. These results have direct implications for the control of the dopant and magnetic field for the practical realization of boron-nitride nanoribbons-based spintronic applications.

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

The cyclisation of a short chain into a ring provides fascinating scenarios in terms of transforming a finite array of spins into a quasi-infinite structure. If frustration is present, theory predicts interesting quantum critical points, where the ground state and thus low-temperature properties of a material change drastically upon even a small variation of appropriate external parameters. This can be visualised as achieving a very high and pointed summit where the way down has an infinity of possibilities, which by any parameter change will be rapidly chosen, in order to reach the final ground state. Here we report a mixed 3d/4f cyclic coordination cluster that turns out to be very near or even at such a quantum critical point. It has a ground state spin of S = 60, the largest ever observed for a molecule (120 times that of a single electron). [Fe10Gd10(Me-tea)10(Me-teaH)10(NO3)10]·20MeCN forms a nano-torus with alternating gadolinium and iron ions with a nearest neighbour Fe–Gd coupling and a frustrating next-nearest neighbour Fe–Fe coupling. Such a spin arrangement corresponds to a cyclic delta or saw-tooth chain, which can exhibit unusual frustration effects. In the present case, the quantum critical point bears a ‘flatland’ of tens of thousands of energetically degenerate states between which transitions are possible at no energy costs with profound caloric consequences. Entropy-wise the energy flatland translates into the pointed summit overlooking the entropy landscape. Going downhill several target states can be reached depending on the applied physical procedure which offers new prospects for addressability.

Ab initio calculation of structural, electronic and magnetic properties and hyperfine parameters at the Fe sites of pristine ZnFe2O4

In this work we present an ab initio study of structural, electronic, magnetic and hyperfine properties of pristine Zn-ferrite (ZnFe2O4, ZFO). Density Functional Theory calculations were performed using the Full-Potential Linearized Augmented Plane Waves (FPLAPW) method in the framework of the Generalized Gradient (GGA) and the GGA+U approximations. In order to discuss the magnetic ordering and the electronic structure of the system we considered different spin arrangements. We found that ZFO presents an energy landscape characterized by a large number of metastable states separated by an energy barrier of about KBTF, being KB the Boltzmann constant and TF the freezing temperature, indicating that ZFO can be described as an spin-glass system at low temperature (<10.5 K). Our calculations also support the picture that below 10.5 K small ferromagnetic spin-clusters (short-range interactions) surrounded by similar spin-clusters with opposite spin orientations (long-range interactions) coexist. Finally, our calculations predict a band gap of normal ZFO of 2.2 eV and successfully describe the hyperfine properties (isomer shift, magnetic hyperfine field and electric field gradient tensor) at the Fe sites that are seen by Mössbauer Spectroscopy (MS) at 4.2 and 300 K. This comparison enables us to characterize the local spin structure around Fe atoms and to explain the origin of the two hyperfine interactions experimentally observed, giving support to the coexistence of short- and a long-range order below 10.5 K.