Neutron diffraction studies of Tb2Rh3Si5 compound

In this work neutron diffraction studies of Tb₂Rh₃Si₅ compound are reported. The compound crystallizes in the monoclinic crystal structure of Lu₂Co₃Si₅-type. At 1.5 K an antiferromagnetic ordering with a propagation vector k=(1/2;1/2;1/2) was observed. The Tb magnetic moments of 9.8(2) μ_B form a non-collinear magnetic structure. In the vicinity of Néel temperature of 8 K a change of the magnetic ordering is evidenced. The change seems to be connected with phase transition from commensurate to incommensurate sine-wave modulation of the Tb magnetic moments.     

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.     

Crystal structure and the magnetic properties of CeTiGe3

The crystal structure of the RTiGe₃ compounds (R=La, Ce and Pr) has been studied by X-ray powder diffraction methods; Rietveld refinement has been carried out on the La homologue. These compounds crystallise in the BaNiO₃ prototype structure, hP10-P6₃/mmc, also called the hexagonal perovskite (a=6.300(1), c=5.915(1) Å for LaTiGe₃). This seems to be the first example in which an intermetallic phase adopts such a structure type which can be considered as derived from the Ni₃Sn type (anti) by a distortion of the lattice and the occupation of the quasi-octahedral 2a site at the origin of the cell (0, 0, 0) by Ti. The composition, also confirmed by microprobe analyses, was found to be strictly 1:1:3 indicating that these are line compounds, forming very likely by a peritectoid reaction. The existence of homologous compounds has been established for the lighter rare earths La, Ce and Pr. Heat capacity and magnetisation data show that CeTiGe₃ orders ferromagnetically with a Curie temperature of nearly 14 K. On the other hand a−ln T variation of the magnetic part of the resistivity below 300 K is consistent with that expected for single impurity Kondo behaviour. CeTiGe₃ is thus an uncommon example of a ferromagnetic dense Kondo lattice.     

Neutron diffraction study of the magnetic ordering in the series R 2 BaNiO 5 (R = Rare Earth)

A neutron diffraction study, as a function of temperature, of the title compounds is presented. The whole family (space group Immm, a ≈ 3.8?, b ≈ 5.8?, c ≈ 11.3?) is structurally characterised by the presence of flattened NiO₆ octahedra that form chains along the a-axis, giving rise to a strong Ni-O-Ni antiferromagnetic interaction. Whereas for Y-compound only strong 1D correlations exist above 1.5 K, presenting the Haldane gap characteristic of 1D AF chain with integer spin, 3D AF ordering is established simultaneously for both R and Ni sublattices at temperatures depending on the rare earth size and magnetic moment. The magnetic structures of R₂BaNiO₅ ( R = Nd, Tb, Dy, Ho, Er and Tm) have been determined and refined as a function of temperature. The whole family orders with a magnetic structure characterised by the temperature-independent propagation vector = (1/2, 0, 1/2). At 1.5 K the directions of the magnetic moments differ because of the different anisotropy of the rare earth ions. Except for Tm and Yb (which does not order above 1.5 K), the magnetic moment of the R³⁺ cations are close to the free-ion value. The magnetic moment of Ni²⁺ is around 1.4 , the strong reduction with respect to the free-ion value is probably due to a combination of low-dimensional quantum effects and covalency. The thermal evolution of the magnetic structures from T _N down to 1.5 K is studied in detail. A smooth re-orientation, governed by the magnetic anisotropy of R³⁺, seems to occur below and very close to T _N in some of these compounds: the Ni moment rotates from nearly parallel to the a-axis toward the c-axis following the R moments. We demonstrate that for setting up the 3D magnetic ordering the R-R exchange interactions cannot be neglected. Received 19 July 2001     

Crystal and magnetic structure of Ho2NiGe6

The crystal and magnetic structure of Ho₂NiGe₆ was studied by powder neutron diffraction. The paramagnetic neutron diffraction data confirmed the Ce₂CuGe₆-type crystal structure reported earlier for this compound. Below the Néel temperature equal to 11 K the Ho magnetic moments form a uniaxial antiferromagnetic ordering. The Ho magnetic moments equal to 8.16(7)μ_B at 1.5 K are parallel to the b-axis. The data are compared with those published for HoNi_0.46(6)Ge₂.     

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.     

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.     

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.     

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.     

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.     

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 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.     

Neutron powder diffraction study on the structures of LaNi5−xAlxDy compounds

The structures of LaNi_5−xAl_xD_y (x=0.75,0.25,y=1.01, 1.10, 1.91 and 3.1) were systematically investigated by neutron and X-ray diffraction. D atoms are found to enter the 6m site of the α-phase but not the reported 12n site, while the 6m and 12n sites of the β-phase. In the case of LaNi_4.75Al_0.25D_y with lower Al content and symmetry, D atoms do not enter the α-phase but occupy the 4h site besides the 6m and 12n sites of the β-phase. The relationship between structures and properties is also discussed.     

Simulation of magnetic properties of the two-dimensional magnetic with anisotropic antiferromagnetic interactions and cluster ordering by quantum Monte Carlo

Magnetic with anisotropic antiferromagnetic exchange interactions and special topology of coupling in the square lattice with spins pairs ordering is studied by quantum Monte Carlo method. The antiferromagnetic order is found to be more stable as compared to spin liquid state. Exchange interactions and wave vector of structure modulation for Cu₃B₂O₆ is estimated. Neel temperature versus strength of exchange in spin pair is calculated. Plateau and modulation of magnetic structure in field magnetization dependence is revealed.     

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     

Neutron powder diffraction study of methane deuterohydrate by the maximum entropy method

To examine the nature of thermal motions of the CH₄ molecules in the methane deuterohydrate (8CH₄·46D₂O), the scattering length density distribution was observed by the maximum entropy method (MEM) using neutron powder diffraction data measured in the temperature range of 7-185 K. We drew the scattering-length density distribution as three dimensional graphic images and used the same isosurface level for all temperatures. The negative scattering length density, corresponding to the H atoms of CH₄, was observed only in the large cage. The positive scattering length density attributed to the C atom of CH₄ was observed at the center of each cage. With an increase in temperature, the negative and positive scattering length densities in the large cage disappear. The positive scattering length density remains at the center of the small cage regardless of temperature. These results strongly indicate that the motions of CH₄ depend on the cage size and geometry.     

Electron-phonon coupling and longitudinal sound velocity of La0.5Ca0.5MnO3

In this paper, the microscopic theory of the relative change in velocity of sound with temperature of La_0.5Ca_0.5MnO₃ is reported. The phonon Green function is calculated using the Green function technique of Zubarev in the limit of zero wave vector and low temperature. The lattice model electronic Hamiltonian in the presence of the phonon interaction with hybridization between the conduction electrons and the l-electrons is used. The relative change in velocity of sound at various temperatures is studied for different model parameters, namely the position of the l-level, the effective phonon coupling strength and hybridization strength. The phonon anomalies observed experimentally at different temperatures are explained theoretically. An abrupt change in velocity at Neel temperature (T_N) is observed clearly. It is observed that different parameters influence the velocity of sound.