Antiferromagnetic Resonance in LaMnO3

The external magnetic field and temperature dependencies of the magnetic structure and antiferromagnetic resonance frequencies in LaMnO₃ are studied. A recently developed model which includes orbitally dependent superexchange and single-ion anisotropy interactions is used. The temperature dependence is described in the mean-field approximation in good agreement with experiments. H–T phase diagrams in the main field directions (a, b, c) are drawn. The problem of the origin of weak noncollinearity of Mn³⁺ spins is solved in our work. Also an optimal method for obtaining an expression of the magnetic free energy is represented. Authors' address: Alexey A. Mozhegorov, Physics Department, Urals State University, Lenin ulitsa 51, Yekaterinburg 620083, Russian Federation     

Antiferromagnetic resonance and high magnetic field properties of NaNiO2

Magnetisation measurements up to 23 T and submillimeter wave ESR in the frequency region 48-380 GHz have been performed on NaNiO₂ powders at low temperature. Also typical spectra above the Néel temperature are shown. At 4 K the magnetisation shows a spin-flop transition at 1.8 T and saturation at 10 T. /Ni confirms the low spin state of the Ni³⁺ ions. The susceptibility exhibits a maximum at K with and K. NaNiO₂ is an A-type antiferromagnet: we derive K and K for the interactions between Ni ions within and between adjacent layers, respectively. The AFMR spectra yield an energy gap of 52.5 GHz, in agreement with the spin-flop value derived from the magnetisation. The anisotropy of the g factor observed at 100 K with can be attributed to the Jahn-Teller effect for Ni³⁺ ions in the low spin state, which stabilises the occupation. We finally comment on the isomorphic controversial Li_1-xNi_1+xO₂ compound. Received 9 March 2000 and Received in final form 13 July 2000.     

Magnetic structure and antiferromagnetic resonance spectrum in manganites: The effect of orbital structure

This paper presents an investigation into the temperature dependence of magnetic structure and antiferromagnetic resonance frequencies. Taking into account the crystal and orbital structures of pure lanthanum manganite, it is shown that the orbital structure plays a crucial role in forming the magnetic structure. The H-T phase diagrams for the magnetic structure are drawn.     

Antiferromagnetic resonance studies in molecular magnetic materials

EPR spectroscopy has become an increasingly powerful tool to examine the spin states and dynamics of single-molecule magnets, but has not been exploited to probe bulk magnetically ordered phases of molecular magnets. In this article, we review the EPR spectra of antiferromagnets and canted antiferromagnets below T_N with particular reference to our own studies on the canted antiferromagnet, p-NCC₆F₄CNSSN (T_N=36 K). The antiferromagnetic resonance experiment allows the saturation of the sublattice magnetisation to be probed. In addition, the exchange and anisotropy fields (H_e and H_a), the spin-flop field (H_sf) and for canted antiferromagnets, the Dzyaloshinskii-Moriya field (H_DM), which gives rise to the spontaneous moment, can be determined.     

Photoemission spectra of LaMnO3 controlled by orbital excitations

We investigate the spectral function of a hole moving in the orbital-ordered ferromagnetic planes of LaMnO3, and show that it depends critically on the type of orbital ordering. While the hole does not couple to the spin excitations, it interacts strongly with the excitations of e(g) orbitals (orbitons), leading to a new type of quasiparticle with a dispersion on the orbiton energy scale and with strongly enhanced mass and reduced weight. Therefore we predict a large redistribution of spectral weight with respect to the bands found in local density approximation (LDA) or in LDA+U.     

Lattice dynamics of LaMnO3: Coupling of the lattice and orbital degrees of freedom

The lattice dynamics of regular LaMnO₃ is calculated within a shell model with pairwise interionic interaction potentials and with a Jahn-Teller (JT) contribution included into the energy and dynamic matrix of the crystal. A correlation is made between Raman spectral lines and lattice vibrations. The positions of some lines in the Raman spectrum are found to depend heavily on the linear JT coupling constant V _e . The effect of the JT coupling on the phonon density of states of LaMnO₃ is investigated.     

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.     

Fine structure in the proton magnetic resonance spectrum of solid benzene and solid benzene-cyclohexane mixtures

The PMR spectrum of solid benzene in the vicinity of the melting point consists of broad and narrow lines. New narrow lines in the spectrum of benzene containing some impurity appear at the top of the broad line. Intensities of narrow lines increase with rising of temperature. The temperature dependence of line width and relaxation timesT ₁ andT ₂ have been measured in pure solid benzene an benzene-cyclohexane mixtures. It is assumed that narrow lines in spectra of pure benzene and its mixtures are caused by appearance of a phase with mobile molecules located in the crystallite joint or on its surface. The spectrum of imperfect monocrystalline benzene have been studied also. The narrow line of this sample is split into several narrow components. This is explained by demagnetization fields the distribution of which has a discrete character,     

Nuclear magnetic resonance investigations of the structure and magnetic properties of metallic multilayers and nanocomposites

As a probe of the short-range chemical and topological order, nuclear magnetic resonance (NMR) has proved useful to investigate the nanostructure of magnetic multilayers or granular systems and, in particular, to evaluate the nature, sharp or diffuse, of interfaces in such nanocomposites. These structural aspects are shortly reviewed in the paper. A larger emphasis is given to the magnetic properties that are accessed by the technique. As a first output of an NMR experiment in ferromagnets, the hyperfine field gives a direct insight on the local magnetization. Hence, for example, one can estimate the magnetization profile at a diffuse interface between a magnetic and nonmagnetic phase. In addition, NMR can probe selectively the magnetic anisotropy or exchange energy in different parts of a composite sample. Therefore NMR is a unique tool to investigate the correlation, at a local scale, between the nanostructure and the magnetic properties of a sample. For example, one can evidence the different magnetic hardness of the interface and bulk moments in multilayers, or of the magnetic clusters and alloyed regions in nanogranular alloys. Some relevant results are presented, which have been obtained in the course of investigations of Co-based multilayers, ultrathin films and granular systems.     

Antiferromagnetic resonance and dielectric properties of rare-earth ferroborates in the submillimeter frequency range

The magnetoresonance and dielectric properties of a number of crystals of a new family of multiferroics, namely, rare-earth ferroborates RFe₃(BO₃)₄ (R = Y, Eu, Pr, Tb, Tb_0.25Er_0.75), are studied in the sub-millimeter frequency range (ν = 3–20 cm⁻¹). Ferroborates with R = Y, Tb, and Eu exhibit permittivity jumps at temperatures of 375, 198, and 58 K, respectively, which are caused by the R32 → P3₁21 phase transition. Antiferromagnetic resonance (AFMR) modes in the subsystem of Fe³⁺ ions are detected in the range of anti-ferromagnetic ordering (T < T _N = 30–40 K) in all ferroborates that have either an easy-plane (Y, Eu) or easy-axis (Pr, Tb, Tb_0.25Er_0.75) magnetic structure. The AFMR frequencies are found to depend strongly on the magnetic anisotropy of a rare-earth ion and its exchange interaction with the Fe subsystem, which determine the type of magnetic structure and the sign and magnitude of an effective anisotropy constant. The basic parameters of the magnetic interactions in these ferroborates are found, and the magnetoelectric contribution to AFMR is analyzed.     

Orbital ordering in LaMnO3 investigated by resonance Raman spectroscopy

Orbital ordering leads to an unconventional excitation spectrum that we investigate by resonance Raman scattering using incident photon energies between 1.7 and 5.0 eV. We use spectral ellipsometry to determine the corresponding dielectric function. Our results show resonant behavior of the phonon Raman cross section when the laser frequency is close to the orbiton-excitation energy of 2 eV in LaMnO3. We show an excellent agreement between theoretical calculations based on the Franck-Condon mechanism activating multiphonon Raman scattering in first order of the electron-phonon coupling and the experimental data of phonons with different symmetries.     

Interrelation of the magnetic structure and the band insulating state in doped manganites

The interrelation between the magnetic structure and the band insulating state in doped La_{1 − x} Ca _x MnO₃ manganites has been discussed. An analysis of various zigzag chains has revealed that, in the one-dimensional spectrum of e _g electrons of these compounds, there always appear a number of band gaps, which at certain electron concentrations x support the formation of an insulating state in the corresponding three-dimensional antiferromagnetic structures. Apart from the well-known spectra of chains of the type (1 × 1) (magnetic E-structure) and (2 × 2) (magnetic CE-structure), we have obtained for the first time the spectrum of a (3 × 3) zigzag chain, whose three-dimensional unit cell contains 24 manganese atoms and provides a qualitatively correct fit to the magnetic structure of the La_1/3Ca_2/3MnO₃ manganite. As follows from our analysis, the formation of a magnetic structure in this manganite should also be accompanied by the generation of a spontaneous magnetic moment.     

Preparation and magnetic properties of LaMnO3 + δ (0 ≤ δ ≤ 0.154)

The structural, electrical, and magnetic properties of ceramic perovskite manganites LaMnO_{3 + δ} (δ = 0–0.154) are investigated. It is found that, in a weak magnetic field (B = 2 G), the LaMnO_{3 + δ} manganite with δ = 0.065 at temperatures below the Curie temperature T _C of the paramagnet-ferromagnet phase transition has a mixed (spin glass + ferromagnet) phase. In LaMnO_{3 + δ} manganites with the parameter δ = 0.100–0.154, this phase transforms into a frustrated ferromagnetic phase. A similar transformation was observed previously in La_1?x Ca_xMnO₃ compounds at calcium contents in the range 0 ≤ x ≤ 0.3. This similarity is explained by the fact that, in both materials, the Mn⁴⁺ concentration and, accordingly, the hole concentration c change equally in the concentration range from ～0.13 to 0.34 with an increase in x or δ. However, the magnetic irreversibility, the concentration dependences of the Curie temperature T _C(c) and the magnetic susceptibility X(c), and the critical behavior of the temperature dependence of the susceptibility X(T) in the vicinity of the Curie temperature T _C differ substantially for these two materials. The observed differences are associated with the distortion of the cubic perovskite structure, the decrease in the degree of lattice disorder, and a more uniform distribution of holes in the LaMnO_{3 + δ} manganites as compared to the La_{1 ? x} Ca_xMnO₃ compounds.     

The role of orbital ordering in the formation of electron structure in undoped LaMnO3 manganites in the regime of strong electron correlations

The electron structure of undoped LaMnO₃ and slightly doped La_1?x Sr_xMnO₃ manganites has been calculated within the framework of a generalized tight binding method with explicit allowance for strong intraatomic electron correlations. According to the results of these calculations, the ground state in orbitally disordered undoped LaMnO₃ ferromagnets would be metallic despite the Mott-Hubbard correlation gap in the spectrum of quasiparticles. Owing to the orbital ordering, the insulating state is stabilized in both antiferromagnetic and paramagnetic phases. In-gap states of a polaron nature with a spectral weight proportional to the dopant concentration have been found near the top of the valence band in La_1?x Sr_xMnO₃. As the doping level increases, a metal state appears in the ferromagnetic phase, which has a metallic character for one spin subband and an insulating character for the other subband (representing the so-called half-metallic state).     

Antiferromagnetic resonance and magnetic anisotropy in single crystals of the YFe3(BO3)4-GdFe3(BO3)4 system

The antiferromagnetic resonance in single crystals of the YFe₃(BO₃)₄-GdFe₃(BO₃)₄ system is studied in the frequency range 25–140 GHz and the temperature range 4.2–50.0 K. It is established that the YFe₃(BO₃)₄ crystal containing only the magnetic subsystem of Fe³⁺ ions is an antiferromagnet with an easy anisotropy plane. The temperature dependences of the gaps in the antiferromagnetic resonance spectra of GdFe₃(BO₃)₄ and Y _x Gd_{1 ? x} Fe₃(BO₃)₄ are used to calculate the contributions of the Fe³⁺ and Gd³⁺ subsystems to the magnetic anisotropy of these crystals. The contributions are found to be close in magnitude and have opposite signs. This leads to a relatively weak uniaxial anisotropy field in the crystals under investigation. Since the exchange interaction between the Gd³⁺ and Fe³⁺ ions magnetizes the magnetic subsystem of gadolinium, both subsystems start to contribute simultaneously at the Néel temperature of the iron subsystem.     

Interrelation between the real structure and the magnetic properties of Fe1−xS1−ySey solid solutions

The paper investigates the influence of the concentration and the mode of distribution of cation vacancies in the metal sublattice on the magnetic properties of iron sulfide and quasibinary Fe_1–xS_1–ySe_y solid solutions. A correlation is established between the distinctive features of changes in the real structure and magnetic transformations. A schematic diagram is constructed for the structural and magnetic states of Fe_1–xS and Fe_1–xS_1–ySe_y.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 3, pp. 71–75, March, 1982.     

Charge segregation and a nonuniform magnetic state in donor-and acceptor-doped LaMnO3

A coordinated study of the magnetic, electrical, optical, and EPR properties of LaMnO₃ single crystals doped by donors (7 at. % Ce) and acceptors (7 at. % Sr) revealed that in all cases, except undoped LaMnO₃, charge segregation associated with large-scale crystal-field fluctuations occurs and the magnetic properties originate from the existence of ferromagnetic phase inclusions and localized ferrons in the matrix with a canted magnetic structure.     

Metal-insulator transition and its relation to magnetic structure in (LaMnO3)2n/(SrMnO3)n superlattices

Superlattices of (LaMnO3){2n}/(SrMnO3){n} (1or=3. Measurements of transport, magnetization, and polarized neutron reflectivity reveal that the ferromagnetism is relatively uniform in the metallic state, and is strongly modulated in the insulating state, being high in LaMnO3 and suppressed in SrMnO3. The modulation is consistent with a Mott transition driven by the proximity between the (LaMnO3)/(SrMnO3) interfaces. The insulating state for n>or=3 obeys variable range hopping at low temperatures. We suggest that this is due to states at the Fermi level that emerge at the (LaMnO3)/(SrMnO3) interfaces and are localized by disorder.