Possible observation of the coexistence of superconductivity and long-range magnetic order in NdRh4B4

The ternary rare earth compound NdRh₄B₄ has been studied by means of critical field, low temperature heat capacity, and static magnetic susceptibility measurements. Features in the upper critical field and heat capacity data at 1.31 K and 0.89 K suggest the occurrence of long-range magnetic order in the superconducting state. The temperature dependence of the static magnetic susceptibility follows a Curie-Weiss law with an effective magnetic moment μ_eff = 3.58 ± 0.05 μ_B and a Curie-Weiss temperature θ_p = ?6.2 ± 1.0 K between 20 K and room temperature. However,, magnetization vs. applied magnetic field isotherms suggest the development of a ferromagnetic component in the Nd³⁺ magnetization at low temperatures.     

Magnetic properties for the Mn2GeTe4 compound

Measurements of magnetic susceptibility χ, in the temperature range from 2 to 300 K, and of magnetization M vs. applied magnetic field B, up to 5 T, at various temperatures were made on polycrystalline samples of the Mn₂GeTe₄ compound. It was found that Mn₂GeTe₄ has a Néel temperature T_N of about 135 K, shows mainly antiferromagnetic behavior with a very weak superimposed ferromagnetic component that is attributed to spin canting. Also, the magnetic results suggest that a possible spin-glass transition takes place at T_f≈45 K. The spin-glass order parameter q(T), determined from the susceptibility data, was found to be in agreement with the prediction of conventional spin-glass theory. The M vs. B results indicated that bound magnetic polarons (BMPs) occur in the compound, and that the effects from BMPs disappear at approximately 80 K. The M vs. B curves were well fitted by a Langevin type of equation, and the variation of the fitting parameters determined as a function of temperature. Using a simple spherical model, the radius of the BMP in the material was found to be about 27 Å; this value is similar to the effective Bohr radius for an acceptor in the II-IV-V₂ and I-III-VI₂ ternary semiconductor compounds.     

Spin-glass-like behaviour and magnetic order in Mn[Cr0.5Ga1.5]S4 spinels

Magnetization and susceptibility were investigated as a function of temperature and magnetic field in polycrystalline Mn[Cr_0.5Ga_1.5]S₄ spinel. The dc susceptibility measurements at 919 Oe showed a disordered ferrimagnetic behaviour with a Curie-Weiss temperature θ_CW=−55 K and an effective magnetic moment of 5.96 μ_B close to the spin-only value of 6.52 μ_B for Cr³⁺ and Mn²⁺ ions in the 3d³ and 3d⁵ configurations, respectively. The magnetization measured at 100 Oe revealed the multiple magnetic transitions with a sharp maximum at the Néel temperature T_N=3.9 K, a minimum at the Yafet-Kittel temperature T_YK=5 K, a broad maximum at the freezing temperature T_f=7.9 K, and an inflection point at the Curie temperature T_C=48 K indicating a transition to paramagnetic phase. A large splitting between the zero-field-cooled (ZFC) and field-cooled (FC) magnetizations at a temperature smaller than T_C suggests the presence of spin-glass-like behaviour. This behaviour is considered in a framework of competing interactions between the antiferromagnetic ordering of the A(Mn) sublattice and the ferromagnetic ordering of the B(Cr) sublattice.     

The antiferromagnetic structure of TbB4

The magnetic structure of the rare earth tetraboride TbB₄ (crystallographic space group P4/mbm) has been determined by neutron diffraction on a polycrystalline sample. Below the experimentally determined Néel temperature of T_N = (43±1) K TbB₄ is ordered antiferromagnetically. The data refinement yielded a magnetic moment value of (7.7 ± 0.2) μ_B/Tb ion at 4.2 K which we interpret as Tb⁴⁺. The magnetic structure is antiferromagnetic collinear with the moments perpendicular to the tetragonal axis.     

Some structural and magnetic properties of 239PuD2.25 by neutron diffraction

A neutron powder diffraction study of ²³⁹PuD_2.25 compound was performed at different temperatures, in order to determine the deuterium atoms positions and to study the occurrence of structural and magnetic phase transitions. Vacancies of tetrahedral sites were found together with partial occupancy of octahedral special positions. No order disorder transitions were observed at low temperature. Below T = 60 K PuD_2.25 becomes ferromagnetically ordered with an ordered magnetic moment μ_ord = 0.8 μ_B per Pu atom.     

Magnetic properties of the intermetallic compound Ce5Ge4

Magnetic and magnetocaloric properties of the compound Ce₅Ge₄ have been studied. This compound has orthorhombic Sm₅Ge₄-type structure (space group Pnma, no. 62) and orders ferromagnetically at ~12 K (T_C). The paramagnetic Curie temperature is ~−20 K suggesting the presence of competing ferromagnetic and antiferromagnetic interactions in this compound. The magnetization does not seem to saturate even in fields of 90 kOe at 3 K consistent with the presence of competing interactions. Saturation magnetization value (extrapolated to 1/H→0) of only 0.8μ_B/Ce³⁺ is obtained compared to the free ion value of 2.14μ_B/Ce³⁺. This moment reduction in the ordered state of Ce₅Ge₄ could be due to partial antiferromagnetic/paramagnetic ordering of the Ce moments and may also be due to crystalline electric field effects. Magnetic entropy change near T_C, calculated from the magnetization vs. field data, is found to be moderate with a maximum value of ~9 J/kg/K at ~11 K for a field change of 90 kOe.     

Large negative magnetoresistance in thiospinel CuCrZrS4

We report on large negative magnetoresistance observed in ferromagnetic thiospinel compound CuCrZrS₄. The electrical resistivity increased with decreasing temperature according to the exp(T₀/T)^1/2, an expression derived from variable range hopping with strong electron-electron interaction. The resistivity under a magnetic field was expressed by the same form with the characteristic temperature T₀ decreasing with increasing magnetic field. Magnetoresistance ratio ρ(T,0)/ρ(T,H) is 1.5 for H=90 kOe at 100 K and increases divergently with decreasing temperature reaching 80 at 16 K. Results of magnetization measurements are also presented. A possible mechanism of the large magnetoresistance is discussed.     

Structural and magnetic properties and hyperfine interaction in La3.5Ru4O13 compound

Structural, magnetic and hyperfine interaction measurements have been carried out on the novel compound La_3.5Ru₄O₁₃ prepared under two different atmospheres (air and oxygen flow). This compound is formed in the orthorhombic structure (space group Pmmm, # 47). The coexistence of the triple-layered perovskite-type planes (quasi-2D structure) and the rutile-like slabs (1D structure) leads to interesting magnetic and electronic properties in this compound. The magnetic susceptibility of this system shows a peak at T~47 K associated with antiferromagnetic interactions. The Curie-Weiss behaviour of the susceptibility provides an effective magnetic moment consistent with Ru ions in low-spin state. Perturbed angular correlation measurements carried out with ¹¹¹Cd probe in the temperature range 10-60 K reveal only quadrupole interactions and indicate the occurrence of structural distortions for T<40 K.     

Magnetic properties of PrCo2 and its ternary hydride PrCo2H4

Magnetization and susceptibility data on PrCo₂ and PrCo₂H₄ are presented. The ac susceptibility of PrCo₂ measured in zero dc field displays a sharp and high peak at T_c = (39.9 ± 0.2) K. The magnetization versus temperature curves show ferromagnetic behaviour for B >1 T, but display a maximum at lower values of the applied field. These results, together with the behaviour of the hysteresis loops at different temperatures below T_c, indicate that PrCo₂ orders ferromagnetically, the magnetic hardness increasing strongly for T → 0. The saturation moment at 4.2 K equals 3.9 μ_B per formula unit, as found from the magnetization curve measured in a pulsed-field magnet up to B = 30 T.Similar experiments on PrCo₂H₄ provide evidence that the introduction of hydrogen in PrCo₂ not only destroys the long-range atomic order, but also considerably reduces the ferromagnetic interactions. Such an effect of the hydrogen is commonly observed in cobalt intermetallics. Part of the PrCo₂H₄ is found to have decomposed into PrH₂ and free Co. The clusters of free Co atoms give rise to a maximum in the zero-field ac susceptibility versus temperature curves, similar as observed in spin glasses or magnetic glasses. By increasing the ac frequency, the maximum shifts to higher temperatures. The behavior can be explained in terms of the Néel model for superparamagnetic particles with randomly oriented local anisotropy axes.     

Mössbauer spectroscopic study of the thermal spin crossover in [Fe(II)(isoxazole)6](ClO4)2

The ⁵⁷Fe Mössbauer spectroscopy of mononuclear [Fe(II)(isoxazole)₆](ClO₄)₂ has been studied to reveal the thermal spin crossover of Fe(II) between low-spin (S=0) and high-spin (S=2) states. Temperature-dependent spin transition curves have been constructed with the least-square fitted data obtained from the Mössbauer spectra measured at various temperatures between 84 and 270 K during a cooling and heating cycle. This compound exhibits an unusual temperature-dependent spin transition behaviour with T_C(↓)=223 and T_C(↑)=213 K occurring in the reverse order in comparison to those observed in SQUID observation and many other spin transition compounds. The compound has three high-spin Fe(II) sites at the highest temperature of study of which two undergo spin transitions. The compound seems to undergo a structural phase transition around the spin transition temperature, which plays a significant role in the spin crossover behaviour as well as the magnetic properties of the compound at temperatures below T_C. The present study reveals an increase in high-spin fraction upon heating in the temperature range below T_C, and an explanation is provided.     

Investigation of TmFe4Al8 and DyFe4Al8 by means of 169Tm and 161Dy Mössbauer spectroscopy

We have performed ¹⁶⁹Tm and ¹⁶¹Dy Mössbauer spectroscopy on TmFe₄Al₈ and DyFe₄Al₈. From the temperature dependence of the electric quadrupole splitting of the ¹⁶⁹Tm spectra of TmFe₄Al₈ we have determined the second order crystal field potential V⁰₂ = (100 ± 10) K and the exchange field term g_Jμ_BH_M = (1 ± 1) K. The temperature dependence of the hyperfine field of the ¹⁶¹Dy spectrum of DyFe₄Al₈ gives g_Jμ_BH_M = (15 ± 3) K. With these exchange fields magnetic transition temperatures of the rare earth sublattices were found, which are consistent with experiment. The relaxation behaviour of the Tm sublattice below T_N = 187 K is discussed.     

Ferromagnetism in LiTbF4

The magnetic properties of crystals of tetragonal LiTbF₄ are reported for the first time. A transition to an uniaxial, high-anisotropy, ferromagnetic state is observed at T_c = 2.86 ± 0.03 K. The saturation moment is 8.90 ± 0.03 μ_B, close to the theoretical maximum of 9 μ_B for Tb³⁺. Magnetic dipolar interactions are shown to be large, and the effects of crystal fields are discussed.     

Magnetic behaviour of Cu2FeGeSe4

Measurements of magnetic susceptibility χ as a function of temperature T and of magnetisation M as a function of applied magnetic field H at a number of fixed temperatures were made on polycrystalline samples of Cu₂FeGeSe₄. The χ versus T data show that an antiferromagnetic transition occurs at 20 K and that a second transition occurs at 8 K, indicating a transition to weak ferromagnetic form. The M versus H curves indicated that at all temperatures below 70 K bound magnetic polarons (BMP) occur, in the paramagnetic, antiferromagnetic and weak ferromagnetic ranges. Below 8 K, the M versus H curves exhibited magnetic hysteresis, and this is attributed to the interaction of the BMPs with tetragonally anisotropic matrix. The B versus H curves were well fitted by a Langevin-type of equation, and the variation of the fitting parameters determined as a function of temperature. These showed that above 20 K the total BMP magnetisation fell almost linearly with increasing temperature and effectively disappeared at 70 K. The number of BMPs remained practically constant with temperature having a mean value of 6.55×10¹⁸/cm³. The analysis gave a value of 213 μ_B for the average magnetic moment of a BMP, corresponding to 42.4 Fe atoms. Using a simple spherical model, this gives the radius of a BMP as 12.0 Å.     

Magnetic structures of PrCO2Si2 and TbCo2Si2 compounds

Neutron diffraction studies of polycrystalline PrCo₂Si₂ and TbCo₂Si₂ compounds were carried out at 4.2 and 293 K. Both samples have collinear antiferromagnetic order below T_N(31(1) and 46(1) K for Pr and Tb compound respectively), with their magnetic moments parallel to the c axis. The ordered magnetic moment values of Pr and Tb at 4.2 K (3.19 and 9.12 μ_B respectively), are close to the saturation value of the free ions. The corresponding magnetic space group P_l4/mnc (Sh⁴¹⁰₁₂₈) is body-anticentered ($\text{k =}\text{111}\text{222}$ refering to P_l cell).     

Magnetodielectric coupling in MnCr2O4 spinel

We have investigated the magnetic and dielectric properties of polycrystalline samples of the spinel MnCr₂O₄. Below the ferrimagnetic ordering temperature at T_N∼43 K, both magnetization and dielectric measurements show signatures of the onset of a conical structure at T_s∼17 K and a lock-in temperature at T_f∼14 K. These values are similar to those previously reported for single-crystal samples, where the spiral structure is short-range ordered (SRO) at low temperatures. The application of magnetic field suppresses the dielectric anomaly at T_f indicating that the coherence length of the ordering increases. MnCr₂O₄ exhibits a symmetrical magnetodielectric response between T_f and T_s that scales with the square of the magnetization. This suggests that the magnetodielectric coupling originates from the P²M² term in the free energy expansion. The magnetodielectric response becomes asymmetric with respect to field below T_f.     

Magnetic properties of the compounds N(CH3)4MnIIMIII(CN)6 ·8 H2O(MIII = Mn,Fe)

In the isostructural cyanobridged chain compounds N(CH₃)₄Mn^IIM^III(CN)₆ · 8H₂O high spin Mn(II) ions couple antiferromagnetically to low spin Mn(III) of Fe(III) ions. The Mn^II–Mn^III compound orders ferrimagnetically below T_N = 28.5 ± 1 K. The tetragonal a and b axes are easy ones for the magnetic moments. In the Mn^II–Fe^III compound antiferromagnetic order occurs below T_N = 9.3 K, with spins aligned along the tetragonal c axis. The compound undergoes a meta-magnetic transition from the antiferromagnetic to a ferrimagnetic phase. This occurs at 2 K for a field H_crit ≈ 1.2 T. The temperature dependence of H_crit, which vanishes at T_N, is followed. The tricritical temperature T¹ is ～ 5 K.     

Molecular material—{N(n-C4H9)4[Ni(II)0.5 Fe(II)0.5 Fe(III)(C2O4)3]}∞: Magnetic, Mössbauer and electrical conductivity studies

We have attempted to characterize the magnetic and electrical properties of a new mixed-metal molecular material {NBu₄[Ni(II)_0.5Fe(II)_0.5Fe(III)(ox)₃]}_N synthesized by the use of trioxalatoferrate as the building block. Mössbauer spectroscopy was utilized in order to understand local spin structures in this compound. The results indicate that the compound is a semiconducting ferrimagnet with T_N=30 K and room temperature conductivity of 6×10⁻¹⁵ Ω⁻¹ cm⁻¹ along with 1.8 eV activation energy under dark. The compound has no appreciable electrical response towards illumination.     

Magnetic and electronic properties of the antiferromagnetic YbFe4Al8 compound

The magnetic, electrical and electronic properties of the tetragonal ternary YbFe₄Al₈ compound have been investigated. This compound was supposed to be an antiferromagnetic superconductor due to the negative magnetization signal appearing at a low field of the field cooling mode, however, based on the measurements of the temperature dependence of magnetization and resistivity we do not confirm the presence of superconductivity in this material and we ascribe the negative magnetization to the complicated non-collinear magnetic structure. A switch to the antiferromagnetic order at about 150 K has been visible both on the M(T) and ρ(T) curves. The valence state of the Yb ions has been studied by X-ray photoemission spectroscopy. The valence band spectrum at the Fermi level exhibits the domination of the hybridized Yb(4f) and Fe(3d) states.     

Magnetic anomalies in single crystalline ErPd2Si2

Considering certain interesting features in the previously reported ¹⁶⁶Er Mössbauer effect, and neutron diffraction data on the polycrystalline form of ErPd₂Si₂ crystallizing in the ThCr₂Si₂-type tetragonal structure, we have carried out magnetic measurements (1.8–300 K) on the single crystalline form of this compound. We observe significant anisotropy in the absolute values of magnetization (indicating that the easy axis is c-axis) as well as in features due to magnetic ordering in the plot of magnetic susceptibility χ versus temperature T at low temperatures. The χ(T) data reveal that there is a pseudo-low-dimensional magnetic order setting in at 4.8 K, with a three-dimensional antiferromagnetic order setting in at a lower temperature (3.8 K). A new finding in the χ(T) data is that, for H∥〈1 1 0〉 but not for H∥〈0 0 1〉, there is a broad shoulder in the range 8–20 K, indicative of the existence of magnetic correlations above 5 K as well, which could be related to the previously reported slow-relaxation-dominated Mössbauer spectra. Interestingly, the temperature coefficient of electrical resistivity is found to be isotropic; no feature due to magnetic ordering could be detected in the electrical resistivity data at low temperatures, which is attributed to magnetic Brillioun-zone boundary gap effects. The results reveal the complex nature of magnetism of this compound.