Understanding the magnetic ground state of rare-earth intermetallic compound Ce4Sb3: Magnetization and neutron diffraction studies

Magnetization and neutron diffraction studies have been performed on Ce₄Sb₃ compound (cubic Th₃P₄-type, space group I4¯3d, no. 220). Magnetization of Ce₄Sb₃ reveals a ferromagnetic transition at ∼5 K, the temperature below which the zero-field-cooled and field-cooled magnetization bifurcate in low applied fields. However, a saturation magnetization (M_S) value of only ∼0.93μ_B/Ce³⁺ is observed at 1.8 K, suggesting possible presence of crystal field effects and a paramagnetic/antiferromagnetic Ce³⁺ moment. Magnetocaloric effect in this compound has been computed using the magnetization vs. field data obtained in the vicinity of the magnetic transition, and a maximum magnetic entropy change, −ΔS_M, of ∼8.9 J/kg/K is obtained at 5 K for a field change of 5 T. Inverse magnetocaloric effect occurs at ∼2 K in 5 T indicating the presence of antiferromagnetic component. This has been further confirmed by the neutron diffraction study that evidences commensurate antiferromagnetic ordering at 2 K in zero magnetic field. A magnetic moment of ∼1.24μ_B/Ce³⁺ is obtained at 2 K and the magnetic moments are directed along Z-axis.     

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.     

Valence fluctuation in Ce2Co3Ge5 and crystal field effect in Pr2Co3Ge5

Polycrystalline samples of ternary rare-earth germanides R₂Co₃Ge₅ (R=La, Ce and Pr) have been prepared and investigated by means of magnetic susceptibility, isothermal magnetization, electrical resistivity and specific heat measurements. All these compounds crystallize in orthorhombic U₂Co₃Si₅ structure (space group Ibam). No evidence of magnetic or superconducting transition is observed in any of these compounds down to 2 K. The unit cell volume of Ce₂Co₃Ge₅ deviates from the expected lanthanide contraction, indicating non trivalent state of Ce ions in this compound. The reduced value of effective moment (μ_eff≈0.95 μ_B) compared to that expected for trivalent Ce ions further supports valence-fluctuating nature of Ce in Ce₂Co₃Ge₅. The observed temperature dependence of magnetic susceptibility is consistent with the ionic interconfiguration fluctuation (ICF) model. Although no sharp anomaly due to a phase transition is seen, a broad Schottky-type anomaly is observed in the magnetic part of specific heat of Pr₂Co₃Ge₅. An analysis of C_mag data suggests a singlet ground state in Pr₂Co₃Ge₅ separated from the singlet first excited state by 22 K and a doublet second excited state at 73 K.     

Effect of thermal treatment on the magnetization processes of nanocrystalline Fe80Ge3Nb10B7 alloys

The dynamic magnetization processes of nanocrystalline Fe₈₀Ge₃Nb₁₀B₇ alloys after annealing at different temperatures are studied through the permeability spectroscopy. Three steps of crystallization are found when amorphous Fe₈₀Ge₃Nb₁₀B₇ alloys are heated from 300to 1200 K. The dominant magnetization process varies with different annealing temperatures. Domain wall bulging is the main magnetization mechanism under weak applied field. When the applied field exceeds pinning field H_p, the depinning-involved domain wall displacement occurs. Different annealing temperature results in different H_p. The lower value of μ′ and high relaxation frequency after heating at 923 and 973 K are due to the strengthened domain wall pinning and the increase of magnetocrystalline anisotropy.     

Magnetic ordering in CeMnCuSi2

Temperature and field-dependent magnetization measurements on polycrystalline CeMnCuSi₂ reveal that the Mn moments in this compound exhibit ordering with a ferromagnetic (FM) component ordered instead of the previously reported purely antiferromagnetic (AFM) ordering. The FM ordering temperature, T_c, is about 120 K and almost unchanged with external fields up to 50 kOe. Furthermore, an AFM component (such as in a canted spin structure) is observed to be present in this phase, and its orientation is modified rapidly by the external magnetic field. The Ce L₃-edge X-ray absorption result shows that the Ce ions in this compound are nearly trivalent, very similar to that in the heavy fermion system CeCu₂Si₂. Large thermomagnetic irreversibility is observed between the zero-field-cooled (ZFC) and field-cooled (FC) M(T) curves below T_c indicating strong magnetocrystalline anisotropy in the ordered phase. At 5 K, a metamagnetic-type transition is observed to occur at a critical field of about 8 kOe, and this critical field decreases with increasing temperature. The FM ordering of the Mn moments in CeMnCuSi₂ is consistent with the value of the intralayer Mn–Mn distance R^a_Mn–Mn=2.890 Å, which is greater than the critical value 2.865 Å for FM ordering. Finally, a magnetic phase diagram is constructed for CeMnCuSi₂.     

Magnetic properties of NdAu2Ge2

Physical properties of NdAu₂Ge₂, crystallising with the tetragonal ThCr₂Si₂-type crystal structure, were investigated by means of magnetic, calorimetric and electrical transport measurements as well as by neutron diffraction. The compound exhibits antiferromagnetic ordering below T_N=4.5 K with a collinear magnetic structure of the AFI-type. The neodymium magnetic moments are parallel to the c-axis and amount to 1.04(4) μ_B at 1.5 K. The observed magnetic behaviour is strongly influenced by crystalline electric field effect.     

Large vertical loop shifts in mechanically synthesized (Mn,Fe)2O3−t nanograins

Magnetic properties of zero field cooled (ZFC) and field cooled (FC) sample of (Mn,Fe)₂O_3−t nanograins have been investigated by magnetometry (up to 70 kOe) and Mössbauer spectroscopy (up to 60 kOe) in the temperature interval 4.2–300 K. Large horizontal (up to 0.8 kOe) and vertical (up to 80%) shifts of the magnetization hysteresis loops are observed in the FC regime. The obtained results are discussed in terms of exchange interaction between an antiferromagnetic core and a spin-glass-like state of the nanograins boundaries. It is shown that hysteresis loop shifts (horizontal and vertical) depend on the field cooling magnitude, an effect that can be understood by the change of the boundary magnetic structure induced by the external magnetic field. The vertical magnetization shift is described by a phenomenological model, which takes into account the magnetic interaction between the spin-glass like boundary spins and the applied field.     

A magnetic study of the ThCr2Si2-type RPd2Ge2 (R=Pr, Nd) compounds. Magnetic structure of PrPd2Ge2 from powder neutron diffraction

The magnetic properties of the PrPd₂Ge₂ and NdPd₂Ge₂ compounds have been investigated by magnetic measurements, specific heat measurements and neutron diffraction experiments. The PrPd₂Ge₂ compound orders antiferromagnetically below T_N=5.0(2) with an original modulated magnetic structure characterized by a magnetic cell three times larger than the chemical one by tripling of the c parameter. The palladium atom is non magnetic and the Pr moments are parallel to the c-axis with a value of ≈2.0 μ_B at 2 K. The specific heat measurements clearly detect a low temperature transition for the NdPd₂Ge₂ compound, interpreted as a Nd sublattice antiferromagnetic ordering below 1.3(2) K.     

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.     

Magnetic phase transitions in Nd7Rh3 single crystal

Magnetic phase transitions in rare earth intermetallic compound Nd₇Rh₃ have been investigated using a single crystal. Measurement results of magnetization, magnetic susceptibility, specific heat, and electrical resistivity reveal that Nd₇Rh₃ has two magnetic phase transitions at T_N=34 K, T_t2=9.1 K and a change of the magnetic feature at T_t1=6.8 K in the absence of an external magnetic field. Antiferromagnetic orderings exist in all the three magnetic states; a large magnetic anisotropy between the c-axis and the c-plane is observed. In the magnetic phase below T_t2, an irreversible field-induced magnetic phase transition takes place in the c-plane; after removing external magnetic field, a coexistence state of ferro- and antiferromagnetic ordering or a ferrimagnetic state having a remanent magnetization M_R is stabilized. The M_R decays to a certain value for several hours after the first process; a magnetic field cooling effect was also observed in the c-plane below T_t2. In the antiferromagentic state above T_t2, the irreversibility disappears and an ordinary antiferromagnetic state takes place. As the origin of this phenomenon, a kind of martensitic structural transition that is observed in Gd₅Ge₄ can be considered.     

Magnetic properties of Mn3B4 under high magnetic field

The magnetic properties of antiferromagnetic compound Mn₃B₄ were examined using pulsed magnetic field up to 470 kOe. It was found that Mn₃B₄ shows a clear metamagnetic transition under 360 kOe at 4.2K. The present results are not explained by the magnetic structure proposed by Neov and a modified magnetic structure is proposed to understand the present magnetization curve. The magnetic phase diagram in the H-T plane is shown.     

Ferromagnetism in amorphous Ge1−xMnx grown by low temperature vapor deposition

Magnetic properties of amorphous Ge_1−xMn_x thin films were investigated. The thin films were grown at 373 K on (100) Si wafers by using a thermal evaporator. Growth rate was ∼35 nm/min and average film thickness was around 500 nm. The electrical resistivities of Ge_1−xMn_x thin films are 5.0×10⁻⁴∼100 Ω cm at room temperature and decrease with increasing Mn concentration. Low temperature magnetization characteristics and magnetic hysteresis loops measured at various temperatures show that the amorphous Ge_1−xMn_x thin films are ferromagnetic but the ferromagnetic magnetizations are changing gradually into paramagnetic as increasing temperature. Curie temperature and saturation magnetization vary with Mn concentration. Curie temperature of the deposited films is 80-160 K, and saturation magnetization is 35-100 emu/cc at 5 K. Hall effect measurement at room temperature shows the amorphous Ge_1−xMn_x thin films have p-type carrier and hole densities are in the range from 7×10¹⁷ to 2×10²² cm⁻³.     

Magnetic dynamics of charge ordered Nd0.80Na0.20MnO3 compound

The magnetic dynamics of charge ordered Nd_0.8Na_0.2MnO₃ compound was studied by measuring the temperature variation of magnetization for different magnetic fields up to 7 T and, the field variation of magnetization at different temperatures down to 5 K. This sample exhibits a charge-ordering transition at 180 K, followed by a weak ferromagnetic (FM) transition at around 100 K and a spin glass like transition below 40 K. Suppression of charge-ordering and spin glass like transition and increase in FM T_C were observed with an increase in magnetic field. A reversible metamagnetic transition above a threshold field (H_f) of 4.5 T was observed at 130 K, followed by a saturation magnetization of 3.2 μ_B/f.u. However at 5 K, an irreversible field induced first order phase transition from charge ordered state to FM state was observed at H_f=5 T. For comparison, the temperature and field variations of magnetization were studied on a FM compound from the same series with the composition Nd_0.90Na_0.10MnO₃. A clear FM transition with a T_C of 113 K and a saturation magnetization of 4.3 μ_B/f.u was observed.     

Magnetic properties and charge ordering in Pr0.75Na0.25MnO3 manganite

The structural and magnetic properties of Pr_0.75Na_0.25MnO₃ have been investigated experimentally. At room temperature, the compound shows paramagnetic characteristic. Along with decreasing temperature, a peak appears in the magnetization versus temperature curve around 220 K. To clarify whether this peak is associated with the ordering arrangement of Mn³⁺ and Mn⁴⁺ ions, electron diffraction experiments were carried out below and above 220 K respectively. Only basic Brag diffraction spots can be observed at high temperatures, however, superlattice diffraction appears below 220 K. This provides direct evidence for the existence of charge ordering in Pr_0.75Na_0.25MnO₃. We find the Mn³⁺ and Mn⁴⁺ cations form zigzag chains in a-c plane by analyzing the diffraction patterns. Combining with the magnetization measurements and the results of electron spin resonance, we confirm the antiferromagnetic phase and ferromagnetic component coexist in Pr_0.75Na_0.25MnO₃ below 120 K.     

Magnetocaloric effect in DyCu2

The magnetocaloric effect of the rare-earth intermetallic compound DyCu₂ is explored through magnetization measurements. DyCu₂ is paramagnetic at the room temperature but becomes antiferromagnetic below 27 K (Neel temperature). Strong temperature and field dependence of magnetization in DyCu₂ at and around the Neel temperature lead to a large magnetocaloric effect. An appreciable magnetocaloric effect persists well above the Neel temperature probably because of the presence of short-range ferromagnetic correlations in the paramagnetic state of DyCu₂. This along with the absence of magnetic hysteresis lead to a large effective refrigerant capacity of 194 J/kg below 44 K, which makes the material important as a potential magnetic refrigerant for the cryogenic liquefier cycles.     

Some aspects of antiferromagnetic ordering in LiMnP0.85V0.15O4: Neutron diffraction and DC-magnetization studies

V-substituted LiMnPO₄ has been synthesized by the solid state reaction route. Combined Rietveld refinement of neutron and X-ray data revealed that all vanadium ions are located in the same positions as the phosphorus ions. The magnetic structure of LiMnP_0.85V_0.15O₄ was found to be the same as that described for undoped antiferromagnetic LiMnPO₄ (T_N=34.5 K). DC-magnetization measurements were carried out to study the peculiarities of magnetic ordering in LiMnP_0.85V_0.15O₄. An irreversible behavior of DC magnetization was found at magnetic fields less than ∼2 kOe. It was demonstrated that an increase in the magnitude of the applied field leads to a reduction of the discrepancy between zero-field-cooled and field-cooled processes. These effects were explained by the movement of domain walls and by transition of the system to a monodomain state. The anomaly in the magnetization vs field dependence attributed presumably to the spin-flop transition was observed at ∼40 kOe. The existence of magnetic inhomogeneity in the paramagnetic phase of LiMnP_0.85V_0.15O₄ was proved by the analysis of the χ?T product. It was concluded that the observed changes in χ?T are indicative of a competition between ferromagnetic and antiferromagnetic correlations at temperatures slightly exceeding T_N.     

Field induced sign reversal of magnetocaloric effect in Gd2In

We report the magnetocaloric effect in the metamagnetic compound Gd₂In obtained from magnetization measurement. Gd₂In was previously reported to have two magnetic transitions: (i) a paramagnetic to ferromagnetic transition below 190 K and (ii) a ferromagnetic to an antiferromagnetic state below 105 K. The low temperature antiferromagnetic state is unstable under an applied magnetic field and undergoes metamagnetic transition to a ferromagnetic like state. We observe conventional positive magnetocaloric effect (the magnetic entropy change, ΔS_M<0) around 190 K at all applied fields. The magnetocaloric effect is found to be inverse (negative) at low fields around 105 K (ΔS_M>0), however it turns positive at higher fields (ΔS_M<0). The observed anomaly is found to be related to the field induced transition which drives the system from an antiferromagnetic to a ferromagnetic state.     

Investigation of magnetocaloric effect in La0.45Pr0.25Ca0.3MnO3 by magnetic,differential scanning calorimetry and thermal analysis

We investigated magnetocaloric effect in La_0.45Pr_0.25Ca_0.3MnO₃ by direct methods (changes in temperature and latent heat) and indirect method (magnetization isotherms). This compound undergoes a first-order paramagnetic to ferromagnetic transition with T_C=200 K upon cooling. The paramagnetic phase becomes unstable and it transforms into a ferromagnetic phase under the application of magnetic field, which results in a field-induced metamagnetic transition (FIMMT). The FIMMT is accompanied by release of latent heat and temperature of the sample as evidenced from differential scanning calorimetry and thermal analysis experiments. A large magnetic entropy change of ΔS_m=−7.2 J kg⁻¹ K⁻¹ at T=212.5 K and refrigeration capacity of 228 J kg⁻¹ are found for a field change of ΔH=5 T. It is suggested that destruction of magnetic polarons and growth of ferromagnetic phase accompanied by a lattice volume change with increasing magnetic field is responsible for the large magnetocaloric effect in this compound.     

Ferromagnetism and spin reorientation in Sm12Fe14Al5

The single crystal of the new ternary compound Sm₁₂Fe₁₄Al₅ was grown and its crystallographic and magnetic properties were investigated. Sm₁₂Fe₁₄Al₅ has a hexagonal structure of the space group p-3m1 and shows ferromagnetism with a Curie temperature of 245 K. The easy direction of magnetization is parallel to the c-axis at temperatures between 245 and 85 K; however, it changes to the c-plane below 85 K through a first-order-like phase transition. No saturation is observed in the magnetization curve even under the applied field of 55 kOe at 5 K. Sm₁₂Fe₁₄Al₅ seems to have a large coercive field at very low temperatures. The anisotropy field was estimated at 5 and 120 K and the saturation magnetization of low temperature phase is explained assuming a ferromagnetic coupling between Fe and Sm sublattices.