Neutron diffraction studies of the magnetic ordering in the rare earth compounds TbNi2Si2, HoCo2Si2 and TbCo2Si2

Neutron diffraction studies and magnetic measurements on the compounds TbNi₂Si₂ (1), HoCo₂Si₂ (2) and TbCo₂Si₂ (3) revealed a collinear antiferromagnetic order below T_N = 10 ± 1 K (1), T_N = 13 ± 1 K (2) and T_N = 30 ± 2 K (3) with the rare earths moments oriented along the c-axis [m₀ = 8.8 ± 0.2 μ_B (1), m₀ = 8.1 ± 0.2 μ_B (2), m₀ = 8.8 ± 0.2 μ_B (3)] and the corresponding wavevector are $\text{k}\text{= [}\text{1}\text{2}\text{1}\text{2}\text{0] (1)}\text{and}\text{k}\text{= [ 0 0 1] (2) (3)}$. The magnetic structure of the compounds HoCo₂Si₂ and TbCo₂Si₂ consists of ferromagnetic layers perpendicular to the c-axis coupled antiferromagnetically (+?+?) while for TbNi₂Si₂ the ordering within (0 0 1) plane is antiferromagnetic and the planes (0 0 1) are indeed decoupled.     

The antiferromagnetic structure of ErCo2Si2 by neutron diffraction

The magnetic structure of the tetragonal ErCo₂Si₂ compound is determined by neutron diffraction on powder sample at 4.2 K. The magnetic ordering is connected with a symmetry lowering, magnetic space group P_2s$\text{1}$ (Sh⁷₂)k = 000. The structure is collinear antiferromagnetic with the erbium magnetic moments making an angle of 56.2° with the c axis. The magnetic moment value for erbium is 6.75μ_B.     

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).     

Magnetic phase transition in TbMn2Ge2

The crystal and magnetic stucture of TbMn₂Ge₂ are determined by neutron diffraction using a powder sample. The crystal structure of this compound is of the ThCr₂Si₂ type with small mixing of Mn and Ge atoms between 4(d) and 4(e) positions. At RT the antiferromagnetic collinear structure consist of a+?+? sequence of ferromagnetic layers of Mn atoms with the magnetic moment parallel to the c-axis. At 85 K, the ferromagnetic ordering within the Tb sublattice is observed. The magnetic moment (～7.7 μ_B) is parallel to the c-axis. At 4.2 K additional reflections are observed, which correspond to antiferromagnetic components in a monoclinic unit cell.     

Neutron diffraction study of the crystal and magnetic structure of the ionic ferromagnet Cs2CrCl4

Neutron powder diffraction has been used to investigate the crystal and magnetic structure of the ionic ferromagnet Cs₂CrCl₄, T_c ～ 58K. Data taken at ambient temperature, 78 and 4.2K indicate the structure remains tetragonal $\text{I4}\text{mmm}$ at low temperatures. A ferromagnetic alignment of the spins is confirmed. The ordered moment at 4.2K is found to be 4.1 ± 0.2μ_B, and the best agreement between the calculated profile and the data suggests its direction lies at an angle of 56 ± 6° to the unique axis.     

Neutron diffraction study of magnetic ordering in PrCu2Si2, PrCu2Ge2, PrFe2Ge2 and NdFe2Ge2

A neutron diffraction study of polycrystalline PrCu₂Si₂ [1], PrCu₂Ge₂ [2], PrFe₂Ge₂ [3] and NdFe₂Ge₂ [4] intermetallics carried out at liquid helium temperature shows the presence of a collinear antiferromagnetic order below T_N = 19 ± 1 K [1], T_N = 16 ± 1 K [2], T_N = 9 ± 1 K [3] and 13 ± 1 K [4]. Magnetic moment, parallel to the c-axis is localized on RE ions only. The magnetic structure of these compounds consists of ferromagnetic layers perpendicular to the c-axis coupled antiferromagnetically with sequence +-+- for PrCu₂Si₂ and PrCu₂Ge₂ and +--+ for PrFe₂Ge₂ and NdFe₂Ge₂. The RE moments amount close to the free ion values for Fe containing compounds but are smaller in those containing Cu suggesting a fairly strong influence of crystal field.     

Crystals and magnetic structure of RMn2Si2 (R = Pr, Nd, Y) and YMn2Ge2

Crystallographic and magnetic properties of PrMn₂Si₂, NdMn₂Si₂, YMn₂Si₂ and YMn₂Ge₂ intermetallics were studied by X-ray, neutron diffraction and magnetometric measurements. The crystal structure of all four compounds was confirmed to be body-centered tetragonal (space group I4/mmm). All were found to be antiferromagnetic with Néel points at 368, 380, 460 and 395 K respectively. Neutron diffraction results indicate that their magnetic structure consists of ferromagnetic layers composed of Mn ions piled up along the c-axis. Each layer is antiferromagnetically coupled to adjacent layer. The magnetic space group is I_p4/m′m′m′. No magnetic ordering of the R sublattice was observed at 1.8 K in the case of R = Pr and Nd.     

The antiferromagnetic structures of TbCu2Ge2 and HoCu2Ge2 by neutron diffraction

The magnetic structures of TbCu₂Ge₂ and HoCu₂Ge₂ were studied by neutron diffraction. At 293 K the chemical structure is tetragonal body centered, space group I 4/mmm. The magnetic cell at 4.2 K is four times larger than the chemical one with a wave vector $\text{k =}\text{1}\text{2}\text{0}\text{1}\text{2}$. The magnetic space group is triclinic P_a$\text{1}$(Sh₂⁷) for both compounds. The moment values and directions are μ_Tb = 8.48(6) [μ_B] along [110] tetr. and μ_HO = 6.5(1)[μ_B] making an angle of 81.4(°) with c and 80(°) with a₁. The structure consists of ferromagnetic (101) layers stacked antiferromagnetically.     

Magnetic properties of ternary RMn2Si2 and RMn2Ge2 compounds

Magnetic properties of RMn₂Si₂ and RMn₂Ge₂ compounds, where R is a rare earth metal, have been investigated by magnetometric measurements. RMn₂Ge₂ (where R is a light rare earth) and LaMn₂Si₂ are ferromagnets. Remaining compounds have antiferromagnetic properties. DyMn₂Si₂ and ErMn₂Si₂ show ferromagnetic properties at low temperatures. It was confirmed that the value of Curie (or Néel) temperature for the Mn sublattice decreases with increasing c constant.     

Critical behavior of Fe15Ni65B18Si2 ferromagnetic glass

AC susceptibility, magnetization and electrical resistivity around the Curie temperature (T_c) were measured for Fe₁₅Ni₆₅B₁₈Si₂ glass. The results yield T_c = (307.6±0.1) K and the following critical exponents γ = 1.50±0.03, β = 0.375±0.01, δ = 5.1±0.1 andα = -0.29±0.05. These values were obtained in the reduced temperature interval $\text{1×10}{}^{-3}\text{?}\text{|T?T}{}_{\mathrm{c}}\text{|}\text{T}{}_{\mathrm{c}}\text{?5 ×10}{}^{-2}$. In spite of the fact that these values for the critical exponents were obtained from different measurements they obey the equality relations γ = β(δ?1) and γ+2β+α = 2. Reduced magnetisation and field follow a magnetic equation of state derived for a second-order phase transition over a wide temperature range. This set of critical exponents is compared with those derived from the Heisenberg model as well as with the usual ones for a pure crystalline ferromagnets. The comparison shows that the values of |α| and γ, for our alloy, are considerably larger than those from the model and the usual crystalline ones. A similar difference is also observed in some other amorphous and dilute crystalline ferromagnets and is probably due to magnetic inhomogeneities.     

First order magnetic phase transition in tetragonal NpCu2Si2

Magnetization and Np²³⁷ Mössbauer studies of the tetragonal compounds NpM₂Si₂ (M = Cr, Mn, Fe, Co, Ni, Cu) were performed. NpMn₂Si₂ is ferromagnetic. All other compounds order antiferromagnetically. Only in NpCu₂Si₂ the Mössbauer studies reveal a first order magnetic phase transition at T_N = 34 K. It is interpreted in terms of Blume's model, originally developed for cubic UO₂.     

Superconductivity in CeCu2Si2

Resistivity measurements of CeCu₂Si₂ are carried out under pressures p up to 12 kbars. Unlike polycrystalline samples, no traces of superconductivity have been observed in CeCu₂Si₂ at ambient pressure. When pressure is applied, CeCu₂Si₂ monocrystals become superconducting with anomalously large ratio H_c2(0)/T_c (0) = 34 K0e/K and with the derivative dH_c2/dT(T=T_c) = 140 K0e/K     

Neutron diffraction study of RECo2Si2 intermetallics

A neutron diffraction study of polycrystalline RECo₂Si₂ intermetallics (RE = Pr, Nd, Tb, Ho, Er) carried out at liquid helium temperature shows the presence of a collinear antiferromagnetic ordering of +?+? type. Magnetic moment is localized on RE ions only and amounts to the RE³⁺ free ion value. In ErCo₂Si₂ the magnetic moment is normal to the tetragonal unique axis, whereas in the remaining compounds the magnetic moment is aligned along it. Néel points were determined from the temperature dependence of magnetic peak heights.     

Magnetism and structural chemistry of ternary silicides: (RE,Th, U)Pt2Si2 (RE = rare earth)

Ternary silicides (RE, U, Th)Pt₂Si₂ have been prepared from the elements. All the compounds (RE= Y, La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu and U, Th) were found to be isotypic and crystallize with the primitive tetragonal CePt₂Si₂-type structure closely related to the CaBe₂Ge₂-type. The magnetic properties of these alloys were studied in the temperature range 1.5 K < T < 1100 K and in fields up to 1.3 T revealing a typical Van Vleck paramagnetism of free RE³⁺-ions for temperatures T > 200 K. A nonmagnetic ground state is reflected from the magnetic susceptibility data of CePt₂Si₂, which are interpreted in terms of interconfiguration fluctuations (ICF). The magnetic results of SmPt₂Si₂ (μ_eff = 0.7 BM) compare well with the ideal Van Vleck behavior of Sm₃₊ ions with a $\text{J =}\text{5}\text{2}$ ground state and a low-lying excited first level $\text{J =}\text{7}\text{2}$. At temperatures below 40 K antiferromagnetic ordering is found for (Gd, Tb, U)Pt₂Si₂; whereas in case of (Dy, Ho, Er, Tm)Pt₂Si₂ the onset of ferromagnetism is indicated below 4 K. None of the samples exhibited a superconducting transition above 1.8 K.     

The magnetic structure of HoCo2Si2

We have carried out neutron diffraction on a HoCo₂Si₂ powder sample at 4.2 K. The magnetic structure of this compound is collinear antiferromagnetic with the holmium magnetic moments parallel to the c-axis of the crystal. The magnetic moment value of holmium is 9.85 μ_B. The magnetic space group is I4/mm'm' (Sh⁴¹⁰₁₂₈) k = 000 The ordering temperature is t_n = 12(1) K.     

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 properties and structural data of ternary silicides: (RE,Th,U) Os2Si2 (RE= rare earth)

New ternary silicides (RE,Th,U) Os₂Si₂ have been synthesized from the elements. All the compounds (RE= Y,La,Ce,Pr,Nd,Sm,Gd,Tb,Dy,Ho,Er,Tm,Yb, Lu) were found to be isotypic and to crystallize with the ordered BaAl₄-type of structure (ThCr₂Si₂-type). Magnetic properties of these alloys — studied in the temperature range 1.5<T<1100 K — reveal a typical Van Vleck paramagnetism of free RE³⁺ ions at temperatures higher than 300 K. The observed effective paramagnetic moment of CeOs₂Si₂, μ(eff)=0.98 BM, is compatible with a rather low concentration (15%) of Ce³⁺. The effective moment of SmOs₂Si₂, μ(eff)=0.47 BM, is in reasonable agreement with a Hund's rule $\text{J=}\text{5}\text{2}$ ground level for free Sm³⁺. For temperatures above 25 K, the magnetic susceptibility as a function of temperature corresponds to the Van Vleck behavior for free Sm³⁺ (closely spaced multiplet, $\text{J=}\text{5}\text{2}$,$\text{J=}\text{7}\text{2}$. Magnetic ordering temperatures of REOs₂Si₂ silicides are generally below 42 K. (Pr,Nd,Ho,Er,Tm) Os₂Si₂ exhibit ferromagnetic ordering whereas (Sm,Gd, Tb,Dy) Os₂Si₂ show antiferromagnetic behavior. Above 1.8 K none of the samples was found to be superconducting.     

Neutron diffraction study of Ho(Rh0.3Ir0.7)4B4

Using powder neutron diffraction techniques, we have examined the magnetic order of the pseudoternary compound Ho(Rh_0.3Ir_0.7)₄B₄ below the Néel temperature T_N=2.7K. The magnetic structure consists of stacked antiferromagnetic basal plane sheets forming a body centered tetragonal unit cell, with a sublattice magnetization corresponding to 9.6±0.6μ_B per Ho³⁺ion at 1.5 K. Magnetic intensity versus temperature measurements indicate that the transition is second order and reveal no anomalous effects when the compound becomes superconducting at T_c=1.34K.     

Neutron diffraction study of the layered compounds MnPSe3 and FePSe3

In the insulating compounds MnPSe₃ (1) and FePSe₃ (2) the divalent transition metal ions form planar honeycomb lattices. A neutron diffraction study revealed a collinear antiferromagnetic order below T_N = 74 ± 2 K (1) and T_N = 119 ± 1 K (2) with the corresponding wavevectors k = [000] (1) and $\text{k = [}\text{1}\text{2}\text{0}\text{1}\text{2}\text{]}$ (2). In MnPSe₃ the magnetic moments (m₀ = 4.74 μ_B) lie within the basal plane and in FePSe₃ (m₀ = 4.9 μ_B) they are pointing along the c-axis. The collinear structures are determined by the dominating intralayer interactions between first (J₁), second (J₂) and third neighbours (J₃) which in MnPSe₃ are all antiferromagnetic whereas in FePSe₃J₁ is ferromagnetic and J₂ and J₃ are antiferromagnetic.     

Magnetic structure of the canted 1D-antiferromagnet NaBaFe2F9

NaBaFe₂F₉ crystallizes with the Ba₂CoFeF₉ structural type (space group P2₁/n, Z = 4). In this structure, infinite cis double [M₂F₉]^3? chains of corner sharing octahedra are isolated one from each other by sodium and barium ions. At 4.5 K, the cell parameters (Å) are found to be: a = 7.3236(3), b = 17.4525(7), c = 5.4586(2), β = 91.840(3)°. Antiferromagnetic interactions dominate but, below T_N ? 19 K, a parasitic ferromagnetic component appears with σ_r(4.5K) = 0.03(1) μ_B·mole^?.The magnetic structure (C_xF_yC_z mode) was foreseen by the macroscopic theory of Bertaut and established from neutron powder diffraction. Using the Rietveld profile refinement method, the 4.5 K spectrum was analysed at $\text{λ =}\text{1.909}\text{A}\text{?}\text{(R}{}_{\mathrm{<mtext>Profile</mtext>}}\text{=}\text{0.093}\text{, R}{}_{\mathrm{<mtext>Nucl</mtext>}}\text{=}\text{0.053}\text{, R}{}_{\mathrm{<mtext>Mag</mtext>}}\text{=}\text{0.126}\text{)}$ and the 4.5–35K difference spectrum at $\text{λ =}\text{2.518}\text{A}\text{?}\text{(R}{}_{\mathrm{<mtext>Mag</mtext>}}\text{=}\text{0.049}\text{, R}{}_{\mathrm{<mtext>Profile</mtext>}}\text{=}\text{0.092}\text{)}$. The magnetic moments on two Fe³⁺ sites, lie mainly in the (0 1 0) plane, approximately at 45° from the a- and c-axes. They form a pseudo G-type antiferromagnetic arrangement (μ(Fe1) = 3.60(4) μ_B;μ(Fe2) = 3.61(6)μ_B).