High magnetic field properties and ESR of the compounds

compounds have a layered structure made of alternating Ni-O and Li-O slabs. An amount z of extra divalent Ni ions is always present in the Li-O layers. We show, using high field magnetisation, static and dynamic susceptibility and high frequency ESR, that the magnetic properties are driven by the z parameter. The compounds can be described as ferromagnetic Ni-O layers, bridged by clusters possessing a net ferromagnetic moment. Received: 24 July 1998 / Revised and Accepted: 23 September 1998     

Study on the spin-states of cobalt-based double-layer perovskite Sr<Subscript>2</Subscript>Y<Subscript>0.5</Subscript>Ca<Subscript>0.5</Subscript>Co<Subscript>2</Subscript>O<Subscript>7</Subscript>

The spin-states of cobalt based perovskite compounds depend sensitively on the valence state and local crystal environment of Co ions and the rich physical properties arise from strong coupling among charge, spin, and orbital degrees of freedom. While extensive studies have been carried out in the past, most of them concentrated on the isotropic compound LaCoO₃. In this paper, using the unrestricted Hartree-Fock approximation and the real-space recursion method, we have investigated the competition of various magnetically ordered spin-states of anisotropic double-layered perovskite Sr₂Y_0.5Ca_0.5Co₂O₇. The energy comparison among these states shows that the nearest-neighbor high-spin-intermediate-spin ferromagnetically ordered state is the relevant magnetic ground state of the compound. The magnetic structure and sizes of magnetic moments are consistent with the recent experimental observation.     

Pressure-induced modifications of crystal and magnetic structure of oxygen deficient La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3-d</Subscript> manganites

The crystal and magnetic structures of the oxygen deficient manganites La_0.7Sr_0.3MnO_3-d (d = 0.15, 0.20) have been studied by means of powder neutron diffraction over the 0–5.2 GPa pressure and 10–290 K temperature ranges. La_0.7Sr_0.3MnO_2.85 exhibits a coexistence of rhombohedral and tetragonal (I4/mcm) crystal structures and below T_g ~ 50 K a spin glass state is formed. La_0.7Sr_0.3MnO_2.80 exhibits a tetragonal (I4/mcm) crystal structure. Below T_g ~ 50 K a phase separated magnetic state is formed, involving coexistence of C-type AFM domains with spin glass domains. In both compounds the crystal structure and magnetic states remain stable upon compression. The factors leading to the formation of different magnetic states in La_0.7Sr_0.3MnO_3-d (d = 0.15, 0.20) and their specific high pressure behavior, contrasting with that of the stoichiometric A_0.5Ba_0.5MnO₃ (A = Nd, Sm) compounds showing pressure-induced suppression of the spin glass state and the appearance of the FM state, are analysed.     

Phase transition in YbAl<Subscript>3</Subscript>C<Subscript>3</Subscript>

¹⁷⁰Yb M?ssbauer spectroscopy, temperature dependent X-ray, magnetisation and specific heat data are presented in the hexagonal intermetallic YbAl₃C₃, in order to shed light on the isostructural transition occurring near 80 K and to investigate the electronic state of the Yb ion above and below the transition. In the low temperature phase, we find that there occurs an atomic rearrangement in the hexagonal unit cell, leading to a strong symmetry lowering at the Yb site. We show that no magnetic ordering of the Yb³⁺ moments occurs down to 0.04 K, and we discuss this finding in terms of 4f-conduction electron hybridisation and geometric frustration.     

Quantum spin dynamics of the bilayer ferromagnet La Sr Mn O

We construct a theory of spin wave excitations in the bilayer manganite La_1.2Sr_1.8Mn₂O₇ based on the simplest possible double-exchange model, but including leading quantum corrections to the spin wave dispersion and damping. Comparison is made with recent inelastic neutron scattering experiments. We find that quantum effects account for some part of the measured damping of spin waves, but cannot by themselves explain the observed softening of spin waves at the zone boundary. Furthermore a doping dependence of the total spin wave dispersion and the optical spin wave gap is predicted. Received 15 January 2002 Published online 6 June 2002     

Electronic structure and properties of strontium ferrite Sr3Fe2O6

The electronic structure of strontium ferrite Sr₃Fe₂O₆ was calculated using the tight-binding linear muffin-tin orbital method (TB LMTO) in the local spin density approximation of density functional theory with Coulomb correlations correction (LSDA+U). The semiconducting character of the spectrum with charge transfer energy gap of 1.82 eV was obtained in reasonably good agreement with experimental data. The iron ions are found to be in the high spin state. The calculated value of the local spin magnetic moment of Fe³⁺ ion is 3.94 μ_B which is not typical for trivalent iron ion in the high spin state. It is shown that the strong hybridization between Fe3d and O2p orbitals favors the d⁶ L configuration of Fe³⁺ ion, where L is a hole in the oxygen p shell. The mechanism of oxygen transport in ferrite is discussed basing on the total energy calculations of the different spatial configurations of oxygen vacancies.     

Jahn-Teller distortion and magnetoresistance in electron doped Sr1-xCexMnO3 (x = 0.1, 0.2, 0.3 and 0.4)

Neutron and electron diffraction, electrical transport and magnetic measurements have been carried out on a newly synthesized electron doped Sr_1-xCe _x MnO₃ (x = 0.1, 0.2, 0.3 and 0.4) system. For x=0.1, while cooling, it undergoes a first-order metal-insulator transition at 315 K which is associated with a structural transition from cubic (Pm3m) to tetragonal (I4/mcm) due to Jahn-Teller ordering () which stabilizes a chain like (C-type) antiferromagnetic ground state with . The antiferromagnetic insulator state is insensitive to an applied magnetic field of 7 T. With increase of x, while the nuclear structure at room temperature for x=0.2 and 0.3 remains tetragonal, for x=0.4 it becomes orthorhombic (Imma) where the doping electrons seem to occupy mainly the d _x2-y2 symmetry. Further, the JT distortion and the antiferromagnetic interactions decrease with doping and a small negative magnetoresistance appears for . Magnetic measurements show that the dilution of antiferromagnetic interaction results into a spin glass like behaviour at low temperature for the samples with x=0.3 and 0.4. This behaviour is in contrast with the CMR properties of calcium based electron doped systems and hole doped manganites. The stability of C-type antiferromagnetic ordering in the electron doped system with large A-site cationic size may be responsible for the absence of double exchange ferromagnetism and CMR effect. Received 10 September 1999     

Spin-spin correlations in the insulating and metallic phases of the Mott system V 2 O 3

The magnetic response in V ₂ O ₃ has been investigated using polarised neutron scattering with polarisation analysis. Measurements were carried out at three temperatures corresponding to the antiferromagnetic insulating ground state, the metallic phase and the high temperature metallic phase. At the first order metal insulator transition there is a dramatic change in the magnetic response with the metallic and high temperature metallic phases being characterised by ferromagnetic spatial correlations of the paramagnetic response. The establishment of ferromagnetic correlations at the metal insulator transition accounts for the abrupt jump in the uniform susceptibility. It is proposed that the differentiation of the V-V distances across the edges of VO ₆ octahedra is of critical importance for the change in electronic conductivity but also for the establishment of the spatial correlations. The gradual high temperature evolution of the conductivity then occurs by the reduction in the vanadium d overlap brought about by thermal expansion. The first order reduction in atomic volume which occurs on the establishment of the metallic phase results from an instability of the vanadium local moment arising from the change in electronic structure. Received 7 April 1999     

Form-factor measurements on chromium with high-energy synchrotron radiation

Results of high-energy magnetic X-ray diffraction on pure antiferromagnetic chromium are presented. The temperature dependence of the propagation vector of the spin-density wave (SDW) and the strain-wave (SW) could be reproduced. The temperature dependence of the magnetic integrated intensity could be measured in the transversally as well as in the longitudinally polarised SDW phase. The magnetic form-factor has been determined in the transversally polarised SDW phase with five magnetic satellites. For the first time a spin-orbit separation has been performed by comparing X-ray to neutron data. The small orbital contribution to the magnetisation density turns out to be negligible, in agreement to our relativistic band-structure calculations. In addition, measurements of strain-wave reflections have been undertaken, and the results complement previous studies. Received 17 August 1998 and Received in final form 10 August 1999     

Coulomb correlations do not fill the e<Superscript>′</Superscript><Subscript>g</Subscript> hole pockets in Na<Subscript>0.3</Subscript>CoO<Subscript>2</Subscript>

There exists presently considerable debate over the question whether local Coulomb interactions can explain the absence of the small e^′ _g Fermi surface hole pockets in photoemission studies of Na_0.3CoO₂. By comparing dynamical mean field results for different single particle Hamiltonians and exact diagonalization as well as quantum Monte Carlo treatments, we show that, for realistic values of the Coulomb energy U and Hund exchange J, the e^′ _g pockets can be slightly enhanced or reduced compared to band structure predictions, but they do not disappear.     

X-ray detected ferromagnetic resonance in thin films

We discuss the physical content of X-ray Detected Magnetic Resonance (XDMR), i.e. a novel spectroscopy which uses XMCD to probe the resonant precession of the local magnetization in a strong microwave pump field. We focus on the simplest case of a steady-state precession of elemental moments in the non-linear regime of angular foldover. Like XMCD, XDMR is element and edge selective and could become a unique tool to investigate how precessional dynamics can locally affect the spin and orbital magnetization of p- or d-projected DOS. This should be possible only in the limit where there is no overdamping due to ultrafast orbit-lattice relaxation.     

Spontaneous surface magnetisation of single crystal MnF2 in the antiferromagnetic state

Spontaneous magnetisation of (100) and (010) surfaces of single crystal MnF₂ in the antiferromagnetic state has been discovered. The sign of the surface magnetisation is determined by the difference in dielectric constants of MnF₂ and ambient matter: magnetisation is directed to the substance with smaller . Received 28 August 1998 and Received in final form 15 December 1998     

The chromium spin density wave: magnetic X-ray scattering studies with polarisation analysis

We report on X-ray magnetic diffraction studies of the spin density wave antiferromagnetism formed in the conduction electron band of chromium. Non-resonant X-ray magnetic scattering was used to directly determine that chromium has zero orbital magnetisation. Furthermore, the azimuthal dependence of this scattering provides unique evidence that chromium forms a linearly polarised wave. In the vicinity of the K absorption edge, resonant X-ray magnetic scattering was observed. A consistent model of the magnetic scattering has been derived from the resonant and non-resonant magnetic amplitudes. The enhancement of the magnetic intensity arises primarily from dipole transitions from the core 1s level to 4p states. Quadrupole transitions to the magnetic 3d states are essentially non-existent due to their sensitivity to (and the absence of) orbital moment. This effect is predicted from atomic considerations of the 3d⁵ ( = 0) transition metal ions. Received 22 September 2000     

Magnetic ordering in Dy<Subscript>1-x</Subscript>Ca<Subscript>x</Subscript>BaCo<Subscript>2</Subscript>O<Subscript>5.5</Subscript> for x = 0.0 and 0.1

The crystal and magnetic structures of Dy_1-xCa_xBaCo₂O_5.5 for x = 0.0 and 0.1 have been studied by neutron powder diffraction and the crystal structures of both compounds were found to be best described in space group Pmmm with a a_p × 2a_p × 2a_p unit cells where a_p is the lattice parameter of the cubic perovskite unit cell. The a- and b-axes were found to decrease and increase abruptly between 315 and 350 K as the temperature increases and the unit cell volumes exhibit signs of excess thermal expansion in the temperature range from 260 to 315 K. Dy_0.9Ca_0.1BaCo₂O_5.5 orders antiferromagnetically for T ≤ 305 K into a G-type magnetic structure with a 2a_p × 2a_p × 2a_p magnetic unit cell. DyBaCo₂O_5.5 exhibits two magnetically ordered phases and a G-type magnetic structure was observed at the investigated temperatures 260 and 290 K. A 2a_p × 2a_p × 4a_p magnetic unit cell was needed for indexing of the magnetic reflections observed for T ≤ 230 K. The low temperature magnetic structure of DyBaCo₂O_5.5 is different from the observed magnetic structures of TbBaCo₂O_5.5 and HoBaCo₂O_5.5 despite the proximity of Tb, Dy and Ho in the periodic table. It is a relatively complex antiferromagnetic structure with both pyramidally and octahedrally coordinated Co ions in the intermediate spin state. It contains both ferro- and antiferromagnetic interactions and the magnetic moments are canted in the a, b-plane. The canting angles between the magnetic moments and the b-axis are 6.6 and 50.0° at 20 K for the pyramidally and octahedrally coordinated Co ions, respectively. The high and low temperature magnetic phases were found to coexist at 230 K.     

Spin correlations in the two-dimensional spin-5/2 Heisenberg antiferromagnet

We report a neutron scattering study of the instantaneous spin correlations in the two-dimensional spin S =5/2 square-lattice Heisenberg antiferromagnet Rb₂MnF₄. The measured correlation lengths are quantitatively described, with no adjustable parameters, by high-temperature series expansion results and by a theory based on the quantum self-consistent harmonic approximation. Conversely, we find that the data, which cover the range from about 1 to 50 lattice constants, are outside of the regime corresponding to renormalized classical behavior of the quantum non-linear model. In addition, we observe a crossover from Heisenberg to Ising critical behavior near the Néel temperature; this crossover is well described by a mean-field model with no adjustable parameters. Received: 3 March 1998 / Received in final form: 4 May 1998 / Accepted: 19 May 1998     

Chromium doped manganites: evidence for electronically phase-separated systems

X-ray absorption spectroscopy (XAS) and soft-X-ray magnetic circular dichroism (SXMCD) at the Mn L_2,3-, Cr L_2,3- and O-K edges of Sm_0.5Ca_0.5Mn_1-xCr_xO₃ () bulk polycrystalline samples have been performed at T=20 K below the ferromagnetic Curie temperature. We show the existence of a magnetic sublattice on each of the probed cations. Considering an electronically phase-separated system, results are compared with magnetization and resistivity measurements and a tentative correlation with magnetoresistance properties on such doped compounds is discussed. Received 7 January 2000     

Neutron scattering on the strongly correlated electron CeNi Cu system: from non-magnetic behaviour to long-range magnetic order

The ground state of the strongly correlated electron CeNi_1-xCu_x compounds has been investigated by means of neutron scattering experiments. Thus, magnetic diffraction was performed for compounds showing long-range magnetic order (x > 0.2). An evolution from a collinear ferromagnetic structure for x =0.6 to a simple antiferromagnetic one for CeCu takes place through some more complex magnetic structures for intermediate compositions. The magnetic moments are continuously reduced when the Ni content increases reflecting the progressive enhancement of the Kondo screening. The large reduction found for x =0.6 compound is discussed and the existence of a spin glass like component of the magnetic moment cannot be discarded. From the quasielastic spectra, we have obtained the Kondo temperatures which are close to the magnetic ordering ones. The quasielastic line-width evolves from a linear temperature dependence to a T ^1/2 behaviour when approaching the non-magnetic limit. Then, this system provides an interesting example for the evolution of unstable 4 f shell relaxation regimes when modifying the hybridisation strength. Received 22 May 2000     

Canted antiferromagnetism and magnetoelastic coupling in metallic Ho0.1Ca0.9MnO3

Ho0.1Ca0.9MnO3 is a canted antiferromagnet with the magnetic space group Pn ' ma '. The magnetic structure is a superposition C x F y A z of the three types of order allowed in Pn ' ma '. In the Ca-rich corner of the system Ho _1-x Ca x MnO ₃ the title compound has a strong magnetoelastic distortion , the highest metallic conductivity and a ferromagnetic component F y close to the maximum in the series. Among the areas ab, bc, ca calculated from the lattice constants only ca shows a strong magnetoelastic effect below T N = 106 K. The x-, y-, z-spin components depend differently on the temperature. This gives rise to spin rotation which is particularly strong close to T N. MnO ₆ octahedra have short bond lengths with a temperature independent average . They are practically regular at room temperature and show a Jahn-Teller distortion of 3.5% in the magnetically ordered state. Above T N we find small polaron conductivity. The presence of the Jahn-Teller distortion due to the only small abundance (10%) of Mn ³⁺ in the t _2g ³ e g configuration is attributed to delocalised e g electrons. In the magnetically ordered state the averaged magnetic moment of Mn is reduced appreciably from the paramagnetic value due to spin disorder. Received 21 January 1999     

Magnetic properties of LaNi <Emphasis Type="Bold">1-</Emphasis><Emphasis Type="Bold">x</Emphasis>Mn <Emphasis Type="Bold">x</Emphasis>O <Emphasis Type="Bold">3+δ</Emphasis> perovskites

Magnetic measurements have been carried out in different LaNi_1-xMn_xO _{3 + δ} samples with 0.1 ⩽ x ⩽ 0.9. All these samples show two magnetic anomalies, one at relatively high temperature characteristic of a ferromagnetic ordering and the other at low temperature, typical of magnetic relaxation phenomena. Neutron diffraction patterns indicate that long-range ferromagnetic ordering is only achieved for x ≥ 0.5. Neutron patterns of LaNi_0.5Mn_0.5O _{3 + δ} samples show an ordered arrangement of Ni and Mn atoms in the perovskite lattice. LaNi_0.5Mn_0.5O _{3 + δ} is then, a double perovskite A₂BB'O₆ whereas Ni and Mn atoms are randomly distributed for the rest of the samples. X-ray magnetic circular dichroism experiments confirm the presence of collinear ferromagnetism in LaNi_0.5Mn_0.5O _{3 + δ} . The role of competitive magnetic interactions, structural disorder, magnetic anisotropy and magnetic disaccommodation is also discussed Received 19 July 2002 / Received in final form 23 October 2002 Published online 31 December 2002     

Induced ferromagnetism and colossal magnetoresistance by Ir-doping in Pr 1 - x Ca x MnO 3

The doping of the manganese site by iridium (up to 15%) in the small A cation manganites Pr_1-xCa_xMnO₃ ( 0.4 ? x ? 0.8), has been investigated as a new method to suppress charge-ordering and induce CMR effects. Ir doping leads to ferromagnetism and to insulator to metal transitions, with high transition temperatures reaching 180 K and CMR ratio in 7 T as large as 10⁴. The efficiency with which iridium induces ferromagnetism and CMR is compared to previous results obtained with other substitutions (Ru, Rh, Ni, Cr...). The ionic radius of the foreign cations and their mixed-valencies are found to be the main parameters governing the ability to collapse the charge-ordered state. Received 14 May 2001 and Received in final form 2 July 2001