Spin waves and exchange interactions in the antiferromagnetic garnets with Fe3+ in the octahedral sites

The results of an inelastic neutron scattering study of the spin wave spectrum for the garnet Fe₂Ca₃Si₃O₁₂(FeSiG) are presented. We compare the exchange parameters for this garnet and for the Ge-species (Fe₂Ca₃Ge₃O₁₂(feGeG)) having the same magnetic structure. We relate the differences found with structural information from powder neutron diffraction. In this way the super exchange paths viap orbitals of intermediate oxygen atoms can be identified. We discuss the effect of a small number (3.2(5)%) of Mn²⁺ impurities in the 24c sites. These lead to an effective ferromagnetic exchange between the Fe³⁺ ions and drastically renormalize the average exchange constants. An estimate for the Fe³⁺–Mn²⁺ indirect exchange between a and c sites of 6(1) K is obtained. The exchange parameters for the pure FeSiG are found to beJ ₁=1.16(4) K,J ₁=0.96(4K andJ ₂=–1.24(4) K for nearest and next nearest neighbours, respectively. These values apply for a moment of 4.02(4) _B per iron atom as obtained from a structure refinement of powder diffraction data. Finally we present results for FeSiG of a high resolution study of the excitations at the zone centre in an attempt to verify our earlier findings of a quantum spin wave gap for FeGeG. In contrast to the earlier measurements, we could follow the acoustical branch to much lower energies using a timeof-flight spectrometer. We found indications for a crossing of the two low lying spin wave branches, the acoustical one extrapolating to the anisotropy gap of 0.005 THz and the antiphase branch extrapolating to the quantum gap of 0.02 THz.     

Effect of Co-Substitution on Magnetic Properties in Spinels GeNi2O4 Systems

The magnetic properties of spinel GeNi_2-2xCo_2xO₄ systems in the range 0≤x≤1 are studied by mean field theory and high-temperature series expansions. The nearest neighbouring and the next-neighbouring super-exchange interactions J₁ (x) and J₂(x) are evaluated for these systems in the range 0≤x≤1, by using the first theory. The intra-planar and the inter-planar interactions and the exchange energy are deduced. The second theory is applied in the spinel GeNi_2-2xCo_2xO₄ systems, combined with the Padé approximants method, to determine the magnetic phase diagrams (T_N versus dilution x) in the range 0≤x≤1. The obtained theoretical results are in agreement with experimental data obtained by magnetic measurements. The critical exponents associated with the magnetic susceptibility γ and the correlation lengths ν are deduced.     

Zn Doping Effect on Magnetic Properties of Znx Cdl-xCr2S4 Systems by High-Temperature Series Expansions

The effect of Zn doping on the magnetic properties of CdCr2S4 systems is studied by mean field theory and high-temperature series expansion （HTSE）. The nearest neighbouring and the next-neighbouring super-exchange interactions Jl（x） and J2（x） are evaluated for the spinel system Zn, Cd1-xCr2S4 in the range 0 〈 x 〈 1. The intra-planar and the inter-planar interactions are deduced. The HTSE combined with the Padd approximant method （PA） is applied to the spinel system ZnxCdl-,Cr2S4. The magnetic phase diagram, i.e. Tc versus dilution x, is obtained. The critical exponents associated with the magnetic susceptibility 7 and the correlation length u are deduced. The obtained theoretical results are in agreement with the experimental data obtained by magnetic measurements.     

Nuclear and magnetic order in Y(Ni,Mn)O3 manganites by neutron powder diffraction

Neutron powder diffraction experiments performed on two selected compositions of the yttrium-based solid solution YNi_xMn_1−xO₃ clearly reveal a nuclear order between the Ni²⁺ and Mn⁴⁺ ions in the half-substituted compound YNi_0.50Mn_0.50O₃, so that the crystal structure is no longer described in the conventional orthorhombic Pbnm space group, but in the monoclinic P2₁/n, all over the investigated temperature range (1.5-300 K). However, both X-rays diagrams and neutron patterns of the YNi_0.25Mn_0.75O₃ phase are indexed in the Pbnm orthorhombic-like symmetry, indicating that the Mn and Ni ions are randomly distributed on the octahedral sites.In addition, neutron diffraction points out that the nature of the magnetic ordering is strongly connected to the structural properties. Whereas no long-range 3D-magnetic ordering was detected for the Pbnm YNi_0.25Mn_0.75O₃ phase, the YNi_0.50Mn_0.50O₃ compound exhibits a magnetic transition at The magnetic structure consists of two collinear Mn⁴⁺ and Ni²⁺ ferromagnetic layers (F_x0F_z magnetic configurations) with saturated magnetic moment values of 2.25(2) and 1.57(2) μ_B for Mn⁴⁺ and Ni²⁺, respectively, at 1.5 K.     

Magnetic exchange interactions induced by Cr-doping in perovskite manganites

The effect of Cr-doping on the structural, magnetic and transport properties of perovskite manganites La_0.8Ca_0.2Mn_1−xCr_xO₃ (0≤x≤0.7) has been investigated. The Curie temperature (T_C) of the Cr-doped samples is almost unchanged up to 30% of Cr-doping. The Cr-doped samples, however, undergo a transition from the parent metallic state to the insulating state below T_C. The dc and ac magnetization data suggest that ferromagnetic clusters induced by double exchange interaction between Cr³⁺ and Mn³⁺ ions and antiferromagnetic components driven by Cr³⁺/Mn⁴⁺ and Cr³⁺/Cr³⁺ interactions are present in the Cr-doped system, which is supported by comparative studies on magnetic and transport properties of LaMnO_3+δ and LaMn_0.75Cr_0.25O_3+δ.     

Magnetic and transport properties of lanthanum perovskites with B-site half doping

We have synthesized various half doped lanthanum perovskites (BB′=MnV, MnCr, MnCo, MnNi, FeCr, FeMn, FeCo, FeNi) by solid state reaction method. The crystal structure was orthorhombic in all samples, but the magnetic and transport properties showed a large variation with the composition. A ferromagnetic feature was quite strong in the Mn-based perovskites but weak or non-existent in the Fe-based ones. The resistivity of Ni-doped ones was much smaller than those of the others. For all half doped perovskits, remarkably, the temperature dependent transport was well explained by variable range hopping model with different localization lengths.     

Inter-network magnetic interactions in GdMexMn1−xO3 perovskites (Me=transition metal)

The gadolinium-based manganite GdMnO₃ of perovskite structure has been partially substituted at the manganese site by transition metal elements Me like Cu, Ni and Co, leading to a general formula GdMe_xMn_1−xO₃, in which different magnetic entities (e.g., Gd³⁺, Cu²⁺, Ni²⁺, Co²⁺, Co³⁺, Mn³⁺, Mn⁴⁺) can coexist, depending on charge equilibrium conditions. For divalent cations such as Cu²⁺ and Ni²⁺, the solid solution extends from x  (Me)=0–0.5, with O-type orthorhombic symmetry (a<c/√2<b)$\left(a<c/\surd 2<b\right)$. When the substituting element is cobalt, the solid solution extends over the whole range [0?x  ?1], changing from O′-type symmetry (c/√2<a<b)$\left(c/\surd 2<a<b\right)$ to O-type for x>0.5. In this latter case, the synthesis is performed under oxygen flow, which allows the cobalt ion to take a 3+ oxidation state.     

Magnetic phase diagram of the four-sublattice antiferromagnet Tb2O2SO4 for a particular field direction

Tb₂O₂SO₄ orders antiferromagnetically at 3.9 K in a four-sublattice structure with two of the nearest-neighbour moments antiparallel and two almost perpendicular to that of a central ion. Specific-heat and magnetization measurements were carried out and allowed to establish the phase diagram for the external magnetic field along one of the moments' direction. Starting at the Néel temperature, the boundary of the paramagnetic phase is first shifted to lower temperatures for increasing field and then it stays at constant temperature for further increase of field. The shift is caused by the reduction of the staggered field that is existing in the antiferromagnetic phase. The experimental results are corroberated to a large extent by mean-field calculations.     

Magnetic states and exchange interaction in hexagonal MnFeAs: A first principles study

The electronic structure and magnetic states for hexagonal-MnFeAs have been studied by a first-principles density functional theory (DFT) calculation. The ground state is ferromagnetic and the calculated magnetic moments for Fe and Mn are 1.1 and 3.1μ_B, respectively, leading to a total magnetization of 4.1μ_B per formula unit due to the small negative moments of As atoms. The exchange interaction between Fe and Mn layers () is positive and tends to form the ferromagnetic ordering. On the other hand, the exchange interaction at the Fe-As₁ layer () is negative while that at the Mn-As₂ layer () is positive. The field induced first order magnetic transition at T_C is related to the competed exchange interaction in the compound.     

Magnetization reversal in bulk and thin films of the ferrimagnetic ErCo0.50Mn0.50O3 perovskite

We present herein a comparison of the magnetic properties of bulk ceramics and thin films of the ferrimagnetic ErCo_0.50Mn_0.50O₃ compound. Epitaxial thin films were deposited onto (1 0 0) SrTiO₃ substrates by pulsed-laser ablation while bulk ceramics were prepared by solid state reaction. When cooling under low applied fields, a spin reversal is observed in both thin film and bulk due to the competition between two magnetic sublattices (Co/Mn and Er) coupled by a negative exchange interaction. Original features are observed in the M(H) loops for bulk materials: abrupt jumps at 4 T due to a reorientation of domains, while in the low field region, the increasing and decreasing branches of the magnetization intersect each other. In the thin film, the ordering temperature increased from 69 to 75 K, and the ZFC anomaly (AF transition) became sharper, compared to the bulk specimen. The oxygen content and the microstructure are crucial to observe the intersection of the magnetization branches.     

In-Situ Alignment of MnBi Crystals Induced by High Magnetic Field above Curie Temperature

Above Curie temperature, MnBi crystals are aligned in situ along the c-axis in a Bi matrix by a high fabrication magnetic field H f of 10 T. Magnetic testing shows a pronounced anisotropy in magnetization in directions normal and parallel to the fabrication field, resulting from the alignment. The successful alignment m v result from the fact that the easy magnetization direction is along the c-axis of MnBi and the high fabrication field of 10 T is large enough to rotate the ）MnBi crystal to this direction even though the temperature is above the Curie temperature.     

Low-temperature magnetic structures in the DySi FeB-type compound 27.03.09

The low-temperature magnetic ordering of the dimorphic DySi compound has been studied at 1.5 K by neutron diffraction on two polycrystalline samples. The samples comprise various amounts of the two orthorhombic modifications: CrB-type (Cmcm Nr. 63, all atoms at 4c site: (0, y, )) and FeB-type (Pnma Nr. 62, all atoms at 4c site: (x, , z)), both order antiferromagnetically (T_N≈38 K). The CrB-type phase orders with a uniaxial structure with the wave vector q₁=(0, 0, ) requiring a doubling of the c-axis. The Dy moments point along the linear chain with the shortest distance c. At 1.5 K, the ordered moment value is 8.57(1) μ_B/Dy atom.Two symmetry independent wave vectors describe the 1.5 K magnetic ordering of the FeB-type phase: q₂=(0, , ) and q₃=(0, 0.484(1), 0.0892(1)), coexisting in form of domains. In both structures the magnetic moments are confined to the (0 0 1) plane at an angle of 2(2)° and 22(3)° from the shortest axis b, respectively. Both structures correspond to sine wave modulations. The amplitude of the q₂ wave is m_o=7.5(1) μ_B/Dy atom and that of q₃ 8.2(1) μ_B/Dy atom. The wave vector q₂ when referring to the (a, 2b, c) cell and the wave vector q=(0, 0, ) corresponds to a transversal modulation, which by a proper origin choice can be also described as an antiphase domain structure with two amplitudes. The moments point to the b-axis and are stacked in the sequence (+m_o/2, −m_o/2, −m_o, −m_o/2, +m_o/2, +m_o, …) along the c-direction, while t_b acts as an antitranslation. For the q₃ phase, the local moment value depends on the atom position in the wave. We also discuss the case where q₃ and q₂ act simultaneously in physical space.     

Magnetization reversal in Gd0.67Ca0.33MnO3: Comparison between epitaxial thin films and bulk

Rare-earth-based manganites ABO₃ may present interesting properties when the lanthanide (A-site) and/or the manganese (B-site) are partially substituted by divalent elements. Heavy lanthanides are particularly appealing because of the expected interplay between the intrinsic magnetic properties of the rare-earth element (Ln) and those of the ferromagnetic manganese sublattice. As such, a spin reorientation has been observed during magnetization-versus-temperature cycles due to a negative exchange interaction between Mn and Ln. We present herein high-quality epitaxial thin films (∼200 nm thick) of Gd_0.67Ca_0.33MnO₃ deposited onto (1 0 0) SrTiO₃ substrates by pulsed-laser deposition. Enhanced properties were observed in comparison with bulk samples. The magnetic transition temperature T_c of the as-grown films is much higher than the corresponding bulk values. Most interesting, magnetization measurements performed under small applied fields, exhibit magnetization reversals below T_c, no matter whether the film is field-cooled (FC) or zero-field-cooled (ZFC). The reversal mechanism is discussed in terms of a negative exchange f-d interaction and magnetic anisotropy, this latter enhanced by strain effects induced by the lattice mismatch between the film and the substrate.     

Competing magnetic structures in the DySi FeB-type phase diagram

The temperature magnetic phase diagrams, of the dimorphic DySi compound, have been studied in terms of wave vectors in the range 1.5-45 K, by neutron diffraction. The polycrystalline sample consists of 26% of CrB-type (Cmcm no. 63, all atoms at 4c site: (0, y, 1/4)) and of 74% of FeB-type (Pnma no. 62, all atoms at 4c site: (x, 1/4, z)). The CrB-ordering is described by the wave vector: q₁=(0, 0, 1/2) over the entire magnetically ordered regime with a uniaxial magnetic structure along the shortest axis c. The FeB-type magnetic phase diagram reveals three distinct regions of magnetic ordering below T_N and one first order transition at T₂=23.5 K (on heating). The ordering is described by two symmetry independent magnetic vectors q₂=(0, 1/2, 1/6) and q₃=(0, q_3y, q_3z) with a temperature variable length. At 1.5 K q_3y≈1/2 and q_3z≈1/11. The two phases coexist in the form of domains. They differ in the moment orientation of the q₃ phase that deviates by ∼22° from the b-axis in the (0, 0, 1) plane. The low temperature range (LT) 1.5 K—T₂ subdivides into two regions: (i) LT-1, between 1.5 K—T₁ where the relative amount of the two phases remains unchanged and in (ii) LT-2: T₁-T₂ where the amount of the incommensurate q₃ phase increases at the cost of the commensurate q₂ amplitude modulated structure which remains unchanged but fully disappears at the first order transition at T₂=23.5 K. The q₃ phase undergoes minor changes until 22 K and gets destabilised at T₂ where the q_3z component jumps from the LT value q_3z≈1/11 to the HT value ≈1/7 and the q_3y component increases from 0.484(1) to 0.495(1). (iii) The high temperature (HT) range T₂-T_N (T_N=40±1 K) is described by a single wave vector q₃. The disproportionation of the HT magnetic phase q₃ below T₂ into two coexisting distinct phases q₂, q₃ down to 1.5 K is an unusual phenomenon, to our knowledge observed for the first time. Various mechanisms are discussed.     

Magnetic phase transitions and structures of Co3V 2O8

Co₃V ₂O₈ is a spin- 3/2 system on a Kagomé staircase and is known to undergo two magnetic phase transitions between 6 and 11 K. The H-T phase diagram of Co₃V ₂O₈ derived by magnetization measurements on a single crystal is presented. Additionally both ordered magnetic structures were investigated by neutron powder diffraction experiments and solved using Bertaut’s macroscopic theory. For the ferromagnetic phase the magnetic moments of the Co²⁺ ions were found to be 1.5(3)μ_B and 2.7(1)μ_B at 3.5 K along the crystallographic a axis for the (4a) and (8e) sites, respectively. The antiferromagnetic phase exhibits a magnetic cell with a doubled b axis with respect to the nuclear one. The magnetic moments point along the a axis being 1.8(2)μ_B (4a) and 1.8(1)μ_B (8e) at 8 K.     

Magnetic Properties and Spin State Transition of Gallium Doped Perovskite Cobaltite Oxide

A series of Ga doping perovskite cobaltite La2/3Sr1/3 （Co1-y Gay）03 （y = 0, 0.1, 0.2, 0.3 and 0.4） are prepared by the standard solid-state reaction method. Their magnetic properties and Co ions spin state transitions are studied. Upon doping, no appreciable structure changes can be found. However, the corresponding Curie temperature sharply decreases and the magnetization is greatly reduced, indicating that Ga doping destroys the ferromagnetic interaction in the system. In addition, the high temperature magnetization data follow the Curie-Weiss law. At least one kind of Co ions （Co^3＋ or Co^4＋） favours the mixed spin state, and most Co ions are at the lower spin state （low and intermediate state）. With increasing Ga content, more Co ions transit to the higher spin state.     

Phase diagram and magnetic structures of the two-level singlet antiferromagnet Ho2O2SO4

The orthorhombic holmium oxisulphate orders as a two-sublattice antiferromagnet atT=3.5 K. In external fields along the crystallographica- andc-directions with large and medium-sized magnetic moment, respectively, a ferrimagnetic phase with 1/3 of the saturation magnetization is passed before the paramagnetic phase is reached. Calculations in mean-field theory reveal that for thec-direction the ferrimagnetic phase is not stable atT=0, it only exists for finite temperatures. Magnetization and susceptibility contain large contributions of van Vleck paramagnetism which at any rate have to be taken into consideration. The phase diagram for the two field directions and the magnetic structures of the different phases are established.     

Size of the interpolated cation and hole carrier density: two key parameters for the optimisation of colossal magnetoresistive properties of Pr-based manganites

The exploration of the magnetic and transport properties of four series of manganese perovskites, Pr_0.7Ca_0.34−xA_xMnO_3−δ (A=Sr, Ba), Pr_0.7−xLa_xCa_0.3 MnO_3−δ and Pr_0.66Ca_0.34−x Sr_xMnO_3−δ has allowed four phases with colossal magnetoresistive (CMR) properties to be isolated: Pr_0.7Ca_0.25Sr_0.025MnO_3−δ and Pr_0.66Ca_0.26Sr_0.08MnO_3−δ that exhibit a variation of resistance of 2.5. 10⁷% and 10⁹% at μ₀ H=5 T for T=88 K and 50 K respectively, Pr_0.58La_0.12Ca_0.3 MnO_3−δ that exhibits a variation of 6.10⁶% for μ₀ H=5 T at T=80 K and Pr_0.7Ba_0.025Ca_0.275MnO_3−δ for which a resistance variation of 5.10⁹%, at T=50 K, for μ₀ H=5 T is evidenced. for each compound of this series except the barium phase, one observes that the temperature T_max, which corresponds to the resistance maximum on the R(T) curves in zero magnetic field, increases dramatically as the mean size of the interpolated cations increases, and that the CMR effect correlatively decreases dramatically. The comparison of the two series Pr_0.7Ca_0.3−xSr_xMnO_3−δ and Pr_0.66Ca_0.34−xSr_xMnO_3−δ shows also the crucial role of the hole carrier density: for a same mean ionic radius of the interpolated cation T_max is decreased of about 50 K by introducing 0.034 hole per Mn mole.     

Magnetic anisotropy and geometrical frustration in the Ising spin-chain system Sr5Rh4O12

A structural and thermodynamic study of the newly synthesized single crystal Sr₅Rh₄O₁₂ is reported. Sr₅Rh₄O₁₂ consists of a triangular lattice of spin chains running along the c-axis. It is antiferromagnetically ordered below 23 K with the intrachain and interchain coupling being ferromagnetic (FM) and antiferromagnetic (AFM), respectively. There is strong evidence for an Ising character in the interaction and geometrical frustration that causes incomplete long-range AFM order. The isothermal magnetization exhibits two step-like transitions leading to a ferrimagnetic state at 2.4 T and a FM state at 4.8 T, respectively. Sr₅Rh₄O₁₂ is a unique frustrated spin-chain system ever found in 4d and 5d based materials without a presence of an incomplete 3d-electron shell.