Crystal structure and magnetic ordering of RNi Si compounds

The element distributions and the magnetic ordering behaviour of compounds RNi₁₀Si₂ (R = Tb, Dy, Ho, Er, Tm) have been studied by neutron powder diffraction down to temperatures of 1.6 K. The compounds crystallize in an ordered variant of the ThMn₁₂ structure type in the tetragonal space group P4/nmm. An ordered 1:1 distribution of Ni and Si on sites 4d and 4e, respectively, corresponds to a modulation vector [0, 0, 1] with respect to the space group I4/mmm of the ThMn₁₂ structure. TbNi₁₀Si₂ orders antiferromagnetically below T _N = 4.5 K with a magnetic propagation vector of [0, 0, 1/2]. The magnetic Tb moments, 8.97(2) /Tb atom at 1.6 K, are aligned along the c-axis. The Ni sites in TbNi₁₀Si₂ do not carry any ordered magnetic moments. The compounds with R = Dy, Ho, Er, and Tm are paramagnetic down to 1.6 K and 3.0 K, respectively. Received 10 July 2002 / Received in final form 12 September 2002 Published online 29 October 2002     

Triangular antiferromagnetic order in the honeycomb layer lattice of

ErCl₃ crystallizes in the AlCl₃-type layer structure. The crystal structure was refined in the paramagnetic state by powder neutron diffraction. The monoclinic lattice parameters at 1.5 K are a = 6.8040(3)?, b = 11.7456(5)?, c = 6.3187(3)? and . The space group is C2/m. Short-range, predominantly in-plane, magnetic ordering occurs above 350 mK up to several Kelvin. Below mK a three-dimensional antiferromagnetic order with a propagation vector of sets in. The magnetic structure of ErCl₃ was determined by powder and single-crystal neutron diffraction at temperatures down to 45 mK. The Er³⁺ ions are located on two-dimensional honeycomb layers in the a–b plane. There are two antiferromagnetically coupled triangular sublattices which form right- and left-handed helices along the c-axis. The magnetic moments are oriented in the a–b plane and amount to 3.3(1) at saturation. From the temperature dependence of the integrated neutron magnetic peak intensity a critical exponent (2) was derived for the magnetic phase transition. Received 1 December 1999 and Received in final form 21 July 2000     

Crystal and magnetic structures of the oxyphosphates MFePO 5 (M = Fe, Co, Ni, Cu). Analysis of the magnetic ground state in terms of superexchange interactions

We have studied in detail the crystal and magnetic structures of the oxyphosphates MFePO₅ (M: divalent transition metal) using neutron powder diffraction as a function of temperature. All of them are isomorphic to the mixed valence compound α-Fe₂PO₅ with space-group Pnma. No disorder exists between the two metallic sites. The M²⁺O₆ octahedra share edges between them and faces with Fe³⁺O₆ octahedra building zigzag chains running parallel to the b-axis that are connected by PO₄ tetrahedra. The topology of this structure gives rise to a complex pattern of super-exchange interactions responsible of the observed antiferromagnetic order. The magnetic structures are all collinear with the spin directed along the b-axis except for M = Co. The experimental magnetic moments of Cu⁺² and Ni²⁺ correspond to the expected ionic value, on the contrary the magnetic moment of Fe³⁺ is reduced, probably due to covalence effects, and that of Co²⁺ is greater than the spin-only value indicating a non negligible orbital contribution. Using numerical calculations we have established a magnetic phase diagram adapted for this type of crystal structure and determined the constraints to be satisfied by the values of the exchange interactions in order to obtain the observed magnetic structure as the ground state. Received 15 December 2000 and Received in final form 25 June 2001     

Temperature dependence of the YBa2Cu3O7 energy gap in differently oriented tunnel junctions

We have applied the break-junction technique to highly biepitaxial c-axis oriented YBa₂Cu₃O₇ thin films with T _C (ρ=0) = 91 K. Mechanically adjustable junctions with a good stability and tunneling current favored along the ab-planes have been realized. The conductance characteristics of these junctions show the presence of gap related maxima that move towards zero bias for increasing temperatures. Considering the misorientation angle α≈ 45 ^° ± 5 ^° of the junction, a maximum gap value at the Fermi level Δ ≈ 22 meV is inferred at T = 13 K. The temperature dependence of the gap related structures, shows a quasilinear behavior for T > 0.4 T _C similar to that observed in c-axis oriented, S-I-N type YBa₂Cu₃O₇ planar junctions. Received 20 July 2001     

A study of the magnetic susceptibility of R3Au3Sb4 (R = Tb,Ho, Er,Tm)

The magnetic susceptibilities of the new cubic intermetallic compounds R₃Au₃Sb₄ (R = Tb, Ho, Er, and Tm) have been measured between 4 and 300 K. The compounds are paramagnetic down to 4 K. The experimental effective magnetic moment of the erbium compound is in agreement with the free-ion value, whereas the effective moments of the other three compounds are lower than the corresponding free-ion values. This discrepancy is interpreted in terms of quenching by the crystalline electric field.     

Interplay of structural, magnetic and transport properties in thelayered Co-based perovskite LnBaCo 2 O 5 (Ln = Tb, Dy, Ho)

The oxygen deficient cobaltites LnBaCo₂O₅ (Ln = Tb, Dy, Ho) exhibit two successive crystallographic transitions at T _N ∼340 K and at T _CO ∼210 K. Whereas the first transition (P4/mmm to Pmmm) is related to the long-range antiferromagnetic ordering of the Co ions (spin ordering), the second transition (Pmmm to Pmmb) corresponds to the long-range ordering of the Co²⁺ and Co³⁺ species (charge ordering) occurring in 1:1 ratio in the structure. The charge ordered (CO) state was directly evidenced by the observation of additional superstructure peaks using neutron and electron diffraction techniques. The CO state was also confirmed indirectly from refinement of high resolution neutron diffraction data as well as from resistivity and DSC measurements. From the refined saturated magnetic moment values only, ∼3.7 and ∼2.7 , the electronic configuration of the Co ions in LnBaCo₂O₅ remains conjectural. Two pictures, with Co³⁺ ions either in intermediate spin state ( t ⁵ _2g e ¹ _g ) or in high spin state ( t ⁴ _2g e ² _g ), describe equally well our experimental data. In both cases, the observed magnetic structure can be explained using the qualitative Goodenough-Kanamori rules for superexchange. Finally, in contrast to the parent Ln = Y compound [Vogt et al. , Phys. Rev. Lett. 84, 2969 (2000)], we do not report any spin transition in LnBaCo₂O₅ (Ln = Tb, Dy, Ho). Received 13 December 2000     

A quantitative determination of magnetic fluctuations in CuGeO3

A polarised neutron scattering investigation has been carried out on a powder sample of CuGeO₃ within the temperature range of 1.5 K to 600 K. The magnetic scattering has been separated from all other contributions by using polarised neutrons and polarisation analysis and placed onto an absolute scale. At low temperatures the long wavelength components of the paramagnetic response are suppressed consistent with the formation of Cu dimers in which the magnetic moments are correlated antiferromagnetically. This form of the scattering persists to temperatures well above the dimerisation temperature T _sp ∼ 14 K. However as the temperature is raised the intensity of the long wavelength spin fluctuations increases and above ∼150 K they are the dominant feature in the wave vector dependence of the response. At all temperatures the observed scattering extrapolates smoothly to the Q = 0 value given by the uniform susceptibility. Consequently the thermal variation of the uniform susceptibility arises from the evolution of the long wavelength magnetic fluctuations. At large wave vectors the energy dependence of the scattering revealed that the response occurs below 16 meV in agreement with the reported maximum magnetic excitation energy at the zone boundary in the ground state. However the total magnetic scattering is significantly less than that expected for a local moment system suggesting that the spectrum of thermal and quantum fluctuations overlap. Received 30 May 2000 and Received in final form 22 March 2001     

Incommensurate modulated magnetic structure in orthorhombic EuPdSb

Orthorhombic EuPdSb is known to undergo two magnetic transitions, at 12 K and at T _N≃ 18 K, and in phase III (T < 12 K), single crystal magnetisation data have shown that the spin structure is collinear antiferromagnetic, with magnetic moments along the crystal a axis. From a ¹⁵¹Eu M?ssbauer absorption study, we show that, at any temperature within phase III, all the moments have equal sizes, and that in phase II (12 K< T <18 K) the magnetic structure is modulated and incommensurate with the lattice spacings. The modulation is close to a pure sine-wave just below T _N = 18 K, and it squares up as temperature is lowered. We measured the thermal variations of the first and third harmonics of the moment modulation, and we could determine the first and third harmonics of the exchange coupling. We furthermore show that the antiferromagnetic-incommensurate transition at 12 K is strongly first order, with a hysteresis of 0.05 K, and that the incommensurate-paramagnetic transition at 18 K is weakly first order. Finally, we present an explanation of the spin-flop transition observed in the single crystal magnetisation data in phase III when || in terms of an anisotropic molecular field tensor. Received 17 January 2001 and Received in final form 20 March 2001     

Magnetization and resistivity steps in the phase separated PrCaMn NiO manganites

The low temperature magnetic and transport properties of the Pr_0.5Ca_0.5Mn_1-xNi_xO₃ manganites ( 0≤ x ≤0.1) have been investigated. The presence of Ni hinders the charge and orbital ordering observed in Pr_0.5Ca_0.5MnO₃ and favors the creation of ferromagnetic regions, leading to phase separation. The ferromagnetic fractions induced by the Ni substitution have been estimated from magnetization measurements, they are large and reach 40% for 4% of Ni. Steps are observed in the M ( H ) and ρ( H ) curves of all the samples at T < 5 K. They are similar to the steps observed in Pr_0.5Ca_0.5Mn_1-xM_xO₃, where M is a non magnetic cation (Mg²⁺, Ga³⁺,...), and for which the ferromagnetic fractions are very small (less than 2%), however, their appearance is restricted to lower temperatures (T < 5 K) with Ni dopant than with non magnetic cations. This study shows that steps can be observed in a wide range of phase-separated systems, even when the ferromagnetic fraction is very large. Received 5 April 2002 / Received in final form 8 July 2002 Published online 14 October 2002 RID="a" ID="a"e-mail: antoine.maignan@ismra.fr     

Magnetic resonance on LiCuVO 4

EPR and ⁷Li NMR measurements were performed in the distorted inverse spinel V(LiCu)O₄ down to 1.5 K. Anisotropy effects on magnetic resonance spectra due to the Jahn-Teller distortion of the oxygen octahedra surrounding the copper ions are discussed. The estimation of the spin-spin interactions deduced from the EPR-relaxation rate Δ H reveals a situation comparable to the prototypical one-dimensional S = 1/2 Heisenberg antiferromagnet CuGeO₃. Approaching three-dimensional antiferromagnetic order ( T _N ≈ 2 K) from above, both magnetic relaxation rates, Δ H _EPR and ⁷ (1/ T ₁ ), respectively, exhibit nearly the same critical divergence reminding to the onset of three-dimensional order in two-dimensional layered systems. Received 22 January 2001 and Received in final form 6 May 2001     

Magnetic structure and anisotropy of YFe 6 Ga 6 and HoFe 6 Ga 6

The magnetic structure of RFe₆Ga₆ intermetallic compounds with R = Y, Ho have been determined by neutron powder diffraction, ⁵⁷Fe M?ssbauer spectroscopy, AC susceptibility, TGA (Thermo-Gravimetric Analysis) and magnetization measurements. Both compounds crystallize in the tetragonal ThMn₁₂ structure (space group I4/mmm) with the magnetic structure of YFe₆Ga₆ consisting of a simple ferromagnetic alignment of Fe moments in the basal plane with a Curie temperature of 475(5) K. Gallium atoms are found to fully occupy the 8i site, with Fe and Ga atoms equally distributed over the 8j site, whilst Fe atoms fully occupy the 8f site. The average Fe moments are 1.68(10) and 1.46(10) at 15 and 293 K, respectively. The average room temperature Fe magnetic moments determined by neutron diffraction are in overall agreement with the average Fe moment deduced from M?ssbauer spectroscopy and bulk magnetization measurements on this compound. The magnetic anisotropy of the compound HoFe₆Ga₆ is also planar in the temperature range 6-290 K, with Ho magnetic moments of 9.28(20) and 2.50(20) at 6 K and 290 K, respectively, coupled anti-ferromagnetically to the Fe sublattice and a Curie temperature of 460(10) K. The magneto-crystalline anisotropies of both compounds are comparable at low temperatures. Received 8 March 2001 and Received in final form 18 June 2001     

Magnetization and neutron scattering studies of the pressure effect on the magnetic transition in Er Y Co

Neutron powder diffraction was employed to study the pressure effect on the magnetic transition in the pseudobinary Laves-phase compound Er_0.57Y_0.43Co₂ and to determine the magnetic moments of the Er- and Co-subsystems. Our studies reveal that the onset of long-range magnetic order for both the localized 4 f (Er) and itinerant 3 d (Co) electron moments appears at about the same temperature at ambient pressure. The pressure effect on T_c is found to be negative and equal for both sublattices, namely T _c / p ∼ - 0.4 K/kbar. The values of the magnetic moments of the Er and the Co ions are found = 5.40±0.15μ _B /atom, = 0.50±0.07μ _B /atom and 5.35±0.15μ _B /atom, 0.37±0.09μ _B /atom, for p = 0 and 6 kbar, respectively. Our experimental results give evidence for short-range magnetic order formation at temperatures already above T_c and for a coexistence short- and long-range order below T_c down to 4 K. Received 20 December 2001 / Received in final form 12 June 2002 Published online 31 October 2002 RID="a" ID="a"e-mail: andrew.podlesnyak@psi.ch     

Infrared spectra and lattice vibrations of the spin-chain compound LiCuVO 4

The infrared spectra of the one-dimensional antiferromagnet LiCuVO₄ are measured in the frequency range from 10 cm^-1 to 10 000 cm^-1 and at temperatures from 2 K to 300 K, for the electric field vector E of the radiation polarized either along the a- or along the b-crystallographic directions. For each polarization six infrared active phonon modes are observed in accordance with factor group analysis of the crystal structure of LiCuVO₄. The theoretical group analysis of the possible spinel low-symmetry phases is performed within the framework of Landau's theory of phase transitions. The parameters of several phonon lines show noticeable anomalies around 150 K where the magnetic correlations appear in the copper chains, which may indicate a finite interaction between the phonon and the magnon subsystems in LiCuVO₄. Received 19 February 2001 and Received in final form 26 June 2001     

A lower bound for the volume-averaged mean-square magnetostatic stray field

Based on a micromagnetics model, we develop a method through which quantitative information on the volume-averaged mean-square magnetostatic stray field 〈|H ^b _d|²〉 _v due to non-zero divergences of the magnetization M within the bulk of a ferromagnetic body can be obtained by analysis of magnetic-field-dependent small-angle neutron scattering data. In the limit of high applied magnetic field H _a, when the direction of M deviates only sligthly from H _a, we have estimated a lower bound for 〈|H ^b _d|²〉 _v as a function of the external field, and we have applied the method to bulk samples of nanocrystalline electrodeposited Ni and Co and coarse-grained polycrystalline cold-worked Ni. The root-mean-square magnetostatic stray field, which is inherent to a particular magnetic microstructure, shows a pronounced field dependence, with values ranging from about 5 to 50mT. Even at applied fields as large as 1.7T, the quantity μ〈|H ^b _d|²〉^1/2 _v of nanocrystalline Co is still 24mT, which suggests that contributions to the total magnetostatic field originating from the bulk are significant in nanocrystalline ferromagnets; therefore, 〈|H ^b _d|²〉 _v cannot be ignored in the interpretation of e.g. measurements of magnetization or spin-wave resonance. A comparison of 〈|H ^b _d|²〉 _v with the volume-averaged mean-square anisotropy field reveals that both quantities are of comparable magnitude. Received 25 April 2002 Published online 31 October 2002 RID="a" ID="a"e-mail: anmi@nano.uni.saarland.de     

Evolution of magnetism in U(Ni 1- xPd x) Si single crystals

Single crystals of U(Ni_1-xPd_x)₂Si₂ with x = 0.05, 0.09 and 0.135 have been grown. Magnetization and electrical resistivity measurements were performed in a wide range of temperatures and magnetic fields in order to study stability of magnetic phases in the solid solutions between UNi₂Si₂ and UPd₂Si₂ with a special emphasis on the type of ground state. In UPd₂Si₂ the simple AFI-type antiferromagnetic structure of U moments is observed at low temperatures. UNi₂Si₂ adopts the uncompensated AF structure (UAF) with the + + - stacking of U moments along the c-axis and consequently this compound exhibits a spontaneous magnetization corresponding to 1/3 of the U moment. The substitution of Pd for Ni leads to a rapid decay of the spontaneous magnetization. The evolution of magnetization and electrical resistivity behavior with Pd doping is tentatively attributed to the coexistence of the AF-I and UAF phases in the ground state of U(Ni_0.91Pd_0.09)₂Si₂ and U(Ni_0.865Pd_0.135)₂Si₂. In this scenario, the volume fraction of the AF-I phase rapidly grows with Pd doping on account of the UAF. At lowest temperatures an irreversible transition to the UAF phase is observed when a sufficiently high magnetic field is applied along the c-axis. Received 28 March 2002 / Received in final form 8 August 2002 Published online 19 December 2002 RID="a" ID="a"e-mail: sech@mag.mff.cuni.cz     

Magnetic properties of the cyclic spincluster Fe6:bicine

The magnetic properties of the cyclic compound [Fe₆(bicine)₆] LiClO₄ ^. 2MeOH are reported. The cluster Fe₆(bicine)₆ forms an antiferromagnetically coupled ring structure of Fe ^III ions. The magnetic susceptibility is measured between 2 and 300 K and yields the exchange coupling of J/k _B = - 27.5±0.5 K. The field dependence of the magnetic moment is studied at 3 and 6 K in magnetic fields up to 5 T. The zero-field splitting of the first excited spin states with S = 2 and 3 are determined by ESR at 94 GHz. The intra-molecular interactions of the Fe ^III ions are analyzed and the on-site anisotropy of the Fe ^III due to the ligand-configuration is determined to d /k _B = - 0.633±0.008K. Received 28 October 2002 / Received in final form 22 February 2003 Published online 20 June 2003 RID="a" ID="a"e-mail: bernd@piobelix.physik.uni-karlsruhe.de     

CEF nature of the magnetic excitations in ordered HoNi B C

The magnetic excitations in the antiferromagnetic phase of HoNi₂B₂C are studied by inelastic neutron scattering on single crystals for the first time. Spectra measured at constant T = 2 K along symmetry directions of the reciprocal space are well explained in terms of crystal electric field (CEF) magnetic excitons within the J = 8 ground state multiplet of Ho³⁺. Very modest bandwidth with planar energy dispersion describes the magnetic exciton dynamics. A perturbative model approach consisting of the CEF states in the effective exchange mean-field provides a simple but applicable characterization of the experimental observations. The microscopic determination of the relevant exchange parameters is discussed in connection with previous works on the subject. Received 25 February 2002 / Received in final form 13 May 2002 Published online 14 October 2002 RID="a" ID="a"e-mail: nordal.cavadini@psi.ch     

Magnetic phase transition and magnetic structure of ground state in CsDyW O

Magnetic phase transition in the CsDyW₂O₈ magnet has been studied by means of low temperature specific heat C ( T ) measurements. The magnetic ordering temperature of the Dy³⁺ sublattice was established to be 1.34 K. The experimental results indicate on the antiferromagnetic character of interactions between Dy³⁺ ions. The behavior of the C ( T ) dependencies above and below T _N is discussed in frames of different theoretical models. The measurements data on temperature and field dependencies of magnetization are used to calculate the exchange and dipole-dipole interactions energy and to determine the possible magnetic structure of the ground state. Received 7 January 2002 / Received in final form 15 May 2002 Published online 7 September 2002     

Magnetic order in LaEuSrCuO studied [2pt] by Fe Mössbauer spectroscopy

⁵⁷Fe M?ssbauer effect studies of La_1.65Eu_0.20Sr_0.15CuO₄ doped with 0.5 at% ⁵⁷Fe performed in the temperature region 300 K > T > 4.2 K give an onset temperature for magnetic ordering of K. This temperature practically is the same as that found in Nd doped La_2-xSr_xCuO₄. It indicates that the magnetic ordering temperature in the LTT phase of rare earth (RE) doped La_2-xSr_xCuO₄ is independent of the RE moment. The direction of the ⁵⁷Fe magnetic moment in the magnetically ordered state is within the CuO₂ plane, while it has been found to be parallel to the c-axis in Nd doped La_2-xSr_xCuO₄. Received: 23 June 1998 / Accepted: 14 July 1998     

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