Antiferromagnetic-resonance spectrum in charge-ordered R<Subscript>0.5</Subscript>Ca<Subscript>0.5</Subscript>MnO<Subscript>3</Subscript> manganites (R=La,Pr, Tb): The effect of orbital and charge structures

A theoretical study is made into the effect of the crystal, orbital, and charge structures on the magnetic structure and spin-wave spectra and on the antiferromagnetic resonance (AFMR) for R_0.5Ca_0.5MnO₃ crystals of monoclinic structure. The model assumes fixed crystal, charge, and orbital structures and enables one to determine the orbitally dependent exchange interaction and single-ion anisotropy for R = La, Pr, Tb. A 16-sublattice weakly noncollinear magnetic CE-structure without a ferromagnetic component is obtained. The behavior of magnetic structure in an external magnetic field is simulated, and the values of fields of spin-flop-transition for different Rs are obtained. The law of spin-wave dispersion and the field dependence of the antiferromagnetic-resonance spectrum are calculated.     

The influence of nonlinear vibronic interaction on the BiMnO3 orbital and magnetic structures

Theoretical principles of the formation of an orbital structure in a strongly distorted Jahn-Teller BiMnO₃ crystal are considered. The way by which the orbital state in different sublattices of the magnetic manganese ion can change the type of magnetic ordering of the crystal in the presence of magnetic frustration is studied.     

Atomic disorder and magnetism in Fe2TiSn alloy

An effect of local atomic disorder on the electronic structure and magnetic moments in Fe₂TiSn is studied. The band structure is calculated by the spin-polarised tight-binding linearised muffin tin orbital (TB LMTO). We found that the Fe₂TiSn alloy in which Fe occupy two FCC sublattices in L2₁-type structure is paramagnetic. The substitution of Fe atoms onto titanium or tin positions leads to an increase of the magnetic moment.     

Correlations induced orbital ordering and cooperative Jahn–Teller distortion in the paramagnetic insulator KCrF<Subscript>3</Subscript>

We investigate the origin of the orbital ordering in the paramagnetic phase of KCrF₃. All previous studies described structural parameters of the paramagnetic phase using a magnetic ordering in the compound. Our simulations of real paramagnetic KCrF₃ were performed within an approach combining density functional theory and dynamical mean field theory (DFT+DMFT). As a result, it was found that the experimentally observed cooperative Jahn–Teller effect is successfully described in a lattice relaxation calculation for structure without any long-range magnetic ordering. It is established that the existence of the orbital ordering even in undistorted perovskite structure clearly confirms the electronic origin of the orbital ordering in KCrF₃.     

Antiferromagnetic resonance spectrum in LaMnO3: Interrelation of the orbital structure and the magnetic properties

The relation between the orbital ordering and magnetic structure of the crystal LaMnO₃ is investigated. The dependence of the exchange parameters on the angle Φ of the orbital structure is determined. When the isotropic exchange interaction and the single-ion anisotropy, which depends on the angle Φ and the rotational distortions, are introduced into the spin Hamiltonian, a four-sublattice structure (A _X, F _Y, G _Z) is obtained with orientation of the magnetic moments of the sublattices near the long axis of the orthorhombic cell of the crystal in the basal plane of the crystal (A _X ? G _Z, F _Y). The effect of a magnetic field on the magnetic structure and the antiferromagnetic resonance spectrum are investigated taking account of the nonequivalent, anisotropic, orbitally-dependent g tensors. The spin-flop and spin-flip transition fields are calculated.     

Hyperfine interactions in titanates: Study of orbital ordering and local magnetic properties

Hyperfine magnetic fields induced on the nuclei of nonmagnetic ions ¹³⁹La and ⁸⁹Y in LaTiO₃ and YTiO₃, respectively, have been microscopically calculated. The dependence of the hyperfine fields on the orbital and magnetic structures of the compounds under study has been analyzed. The comparative analysis of the calculated and known experimental data confirms the existence of the static orbital structure in lanthanum and yttrium titanates.     

Interrelation of the spin,orbital, and charge degrees of freedom in half-doped manganites

Based on the double-exchange model in the tight-binding approximation, self-consistent energy-band-structure calculations are carried out for the first time for the orbital and charge ordering in La_0.5Ca_0.5MnO₃-type manganites with 16 Mn ions in the unit cell under the assumption of a linear dependence of the Jahn-Teller splitting of the e _g level on the occupancy of each ion. The equilibrium magnetic and orbital configurations are determined by minimizing the total energy with respect to the direction of the local magnetic moments and the orbital states of the Mn ions. The dependence of the splitting on the occupancy favors the stabilization of phases with charge separation. This separation is an important factor determining the magnetic structure of the ground state. The ground state can be an insulating antiferromagnetic structure of the CE or G type or a new ferrimagnetic structure with a magnetization lower than that of a saturated ferromagnet by a factor of 2. The existence and the width of the bandgap in the electronic energy spectrum of the CE phase depend on the ratio between the values of the Hund exchange and the splitting. When the splitting is sufficiently large, the Jahn-Teller effect stabilizes the insulating state. The finite value of the Hund coupling also favors the stabilization of the CE phase for the realistic values of the interionic exchange and the hopping integral of itinerant electrons.     

Theoretical study of the magnetic moments and anisotropy energy of CoRh nanoparticles

The role of size, structure and chemical order on the magnetic moments and magnetic anisotropy energy (MAE) of CoRh nanoparticles are studied in the framework of a self-consistent real-space tight-binding method. Our results show that a Rh core in a geometry having a large surface/volume ratio and with Co–Rh mixing at the interface is the most likely chemical arrangement. A local analysis reveals that the orbital and spin moments at the Co–Rh interface are largely responsible for the increase of the magnetic moments and magnetic anisotropy. Moreover, the local moments induced at the Rh atoms, which amount to about 20% of the moment per Co atom [ μ_Rh = (0.2–0.3) μ_B] and the orbital moments of Co atoms play a crucial role on the interpretation of experiment. The results are discussed in the context of the interplay between chemical order and magnetic properties.     

Orbital correlations in doped manganites

We review our recent X-ray scattering studies of charge and orbital order in doped manganites, with specific emphasis on the role of orbital correlations in Pr_1-xCa_xMnO₃. For x=0.25, we find an orbital structure indistinguishable from the undoped structure and long-range orbital order at low temperatures. For dopings 0.3≤x≤0.5, we find scattering consistent with a charge and orbitally ordered CE-type structure. While in each case the charge order peaks are resolution limited, the orbital order exhibits only short-range correlations. We report the doping dependence of the correlation length and discuss the connection between the orbital correlations and the finite magnetic correlation length observed on the Mn³⁺ sublattice with neutron-scattering techniques. The physical origin of these domains, which appear to be isotropic, remains unclear. We find that weak orbital correlations persist well above the phase transition, with a correlation length of 1–2 lattice constants at high temperatures. Significantly, we observe similar correlations at high temperatures in La_0.7Ca_0.3MnO₃, which does not have an orbitally ordered ground state, and we conclude that such correlations are robust to variations in the relative strength of the electron–phonon coupling. Received: 22 May 2001 / Accepted: 4 July 2001 / Published online: 5 October 2001     

Study of the ferrodistorsive orbital ordering in NaNiO2 by neutron diffraction and submillimeter wave ESR

NaNiO₂ has been studied by neutron-powder diffraction, magnetic susceptibility and submillimeter wave ESR. The monoclinic structure at room temperature is characterised by a ferrodistorsive orbital ordering due to the Jahn-Teller (JT) effect of the Ni³⁺ ions in the low spin state. NaNiO₂ undergoes a structural transition at around 480 K, above which the orbital ordering disappears. The high temperature phase is rhombohedral with the layered -NaFeO₂ structure ( space group). The magnetic susceptibility exhibits hysteresis and we observe a change of the Curie-Weiss law parameters above the JT transition. The anisotropy of the g-factor at 200 K can be attributed to the JT effect which favours the orbital occupation. Finally, the interplay between the magnetic and structural properties of NaNiO₂ and Li_1-xNi_1+xO₂ is discussed. Received 29 May 2000     

Crystal field effects on the magnetic structures of the rare earth compounds with the FeB structure

In order to confirm the role of the crystalline electric potential on the stability of non collinear magnetic structures of the rare earth compounds with the FeB-type structure, the magnetic properties of the (Gd_0.5Y_0.5)Ni compound, where the rare earth orbital moment is nul, are studied. Below its Curie temperature (57 K) the compound is ferromagnetic. The spontaneous magnetization at 0 K reaches 7.05 μ_B per gadolinium atom. Yttrium and nickel atoms being not magnetic the gadolinium moments are parallel and the exchange interactions are positive. Then the non collinear magnetic structures observed when the alloyed rare earths have an orbital moment result from the competition between a multiaxial anisotropy due to the crystal field effects and isotropic exchange interactions of the Heisenberg type.     

Field dependence of spin and orbital moments of Fe in L10 FePt magnetic thin films

The field dependence of spin and orbital magnetic moments of Fe in L1₀ FePt magnetic thin films was investigated using X-ray magnetic circular dichroism (XMCD). The spin and orbital moments were calculated using the sum rules; it was found that the spin and orbital moment of Fe in L1₀ FePt films are ∼2.5 and 0.2 μ_B, respectively. The relative XMCD asymmetry at Fe L₃ peak on the dependence of applied field suggested that the majority magnetic moment of L1₀ FePt films resulted from Fe.     

The electronic structure and the ferromagnetic properties of the organic radical 4-methacryloyloxy-2,2,6,6-tetramethyl-1-piperidinyloxyl (MOTMP)

The ab initio method of the full potential linearized augmented-plane-wave has been used to study the electronic band structure and the ferromagnetic (FM) properties of the organic radical MOTMP. The total and the partial density of states and the atomic spin magnetic moments are calculated. The calculation revealed that MOTMP has a stable ferromagnetic ground state and the spin magnetic moment is 1.0 μ_B per molecule, which is in good agreement with the experimental value. It is found that the unpaired electrons in this compound are localized in a molecular orbital constituted primarily of π*(NO) orbital and the main contribution of the spin magnetic moment comes from the NO free radical. It is also found that there exists ferromagnetic intermolecular interaction in the compound.     

Structural and magnetic properties of Fe<Subscript>7−<Emphasis Type="Italic">n</Emphasis></Subscript>Pt<Subscript><Emphasis Type="Italic">n</Emphasis></Subscript> with <Emphasis Type="Italic">n</Emphasis> = 0, 1, 2, . . . 7, bimetallic clusters

An exhaustive study of the structural and magnetic properties of Fe_7?n Pt _n with n = 0, 1, 2, …7, bimetallic clusters is presented. Based on ab initio density functional theory that includes spin-orbit coupling (SOC) and graph theory, the ground state geometry, the local chemical order, and the orbital and spin magnetic moments are calculated. We show how the systems evolves from the 3-d Fe to the quasi-planar Pt clusters. These calculations show that SOC are necessary to describe correctly the composition dependence of the binding energy of these nanoalloys. We observe that the ground state geometries on the Fe rich side resemble the fcc structure adopted by bulk samples. Furthermore, we observe how the spin and orbital magnetic moments depend on the chemical concentration and chemical order. Based on these results, we estimated the magnetic anisotropy energy and found that the largest values correspond to some of the most symmetric structures, Fe₅Pt₂ and FePt₆. To determine the degree of non-collinearity, we define an index that shows that in FePt₆ the total magnetic moments, on each atom, are the less collinear.     

Spin re-orientation in FeCr2S4

The spinel FeCr₂S₄has been studied intensely for its peculiar magnetic and local structural changes which are sensitively influenced by the Jahn?CTeller properties of Fe^2?+?in tetrahedral sulfur coordination. Recent muon spin rotation data give strong evidence that the commonly assumed collinear magnetic structure of this compound is only found between the Curie temperature T_C = 165 K and 50 K. For lower temperatures a helical structure has been proposed. We present new Mössbauer spectroscopic data taken on the same sample as used for muon spin rotation. Also the hyperfine spectra revealing non-equivalent iron sites support the appearance of a spin re-orientation around 50 K which may be related to the onset of short-range orbital order. Below 20 K severe dynamic broadenings are found which may indicate orbital fluctuations. Orbital order occurs around 11 K accompanied by severe changes in the crystalline electric field ground state as traced from quadrupole interaction.     

Electronic structure,electron density,electric field gradient-, magnetic susceptability- and G-tensor of K3Fe(CN)6

Molecular orbital calculations are presented for the electronic structure of K₃Fe(CN)₆ based on clusters of formula K₈Fe(CN)⁵⁺₆, using a semi-empirical molecular orbital method including mixing of low-lying electronic configurations and spin-orbit coupling. The energy splittings obtained are in qualitative agreement with ligand field studies from several workers, excluding those of Merrithew and Modestino. While other authors interpret either Mössbauer data, or ESR results, or susceptibility values only, we obtain from the electron structure calculations charge densities at the iron nucleus, and electric field gradient, magnetic susceptibility and gyromagnetic tensors, which consistently interpret experimental Mössbauer-, EST- and magnetic anisotropy results. From the electronic structure calculations as well as from the reanalysis of experimental quadrupole line intensities (obtained by Oosterhuis and Lang) we derive that orthorhombic polytypism of K₃Fe(CN)₆ has to be considered for a consistent interpretation of the experimental data. The successful correlation between calculation and experiment in an energy range of about 300 K above the electronic groundstate is a measure for the adequacy of our electronic structure calculations in this low-energy range.     

Magnetism of mass-filtered nanoparticles on ferromagnetic supports

The magnetic properties of 3d-metal clusters significantly differ from bulk behavior and, for small clusters, strongly depend on the number of atoms within each cluster. Such phenomena are caused by a narrowing of electronic states and the high ratio of surface to volume atoms giving rise to enhanced magnetic orbital moments. However, even large Fe nanoparticles (6–12 nm) deposited onto ferromagnetic surfaces show enhanced orbital moments. At a low coverage large iron clusters on a cobalt film exhibit a nearly doubled value for the orbital moments when compared to bulk behaviour. With increasing coverage, the orbital moment is clearly reduced. Additionally, the spin and orbital moments of iron and cobalt in Fe₅₀Co₅₀ alloy clusters with a size of 7.5 nm on a nickel substrate have been investigated. FeCo alloys are known to exhibit very high magnetic moments for soft magnetic materials. PACS 73.22.-f; 75.75.+a; 81.07.-b     

Effect of orbital ordering on the magnetic-structure formation in the LaMnO3 Jahn-Teller magnet

A study is reported on the relation between orbital ordering and the magnetic structure of an LaMnO₃ crystal. The dependence of the exchange parameters on the orbital-structure angle Φ has been determined. Inclusion into the spin Hamiltonian of isotropic exchange interaction and single-ion anisotropy, which depends on the angle Φ and rotational distortions, results in a four-sublattice structure (A _X , F _Y , G _Z ), with the sublattice magnetic moments oriented close to the long axis of the orthorhombic cell in the basal plane of the crystal . The effect of the rare-earth-ion size in RMnO₃ manganites on the orbital and magnetic structures is considered.