Heat capacity and magnetic phase transitions of rare-earth orthoferrite HoFeO3

Heat capacity of two rare-earth orthoferrites HoFeO₃ and LuFeO₃ were measured between 1.8 and 200 K. A distinctly large and two small heat capacity anomalies were detected for HoFeO₃ under zero magnetic field around 3.3, 53 and 58 K, respectively. The low-temperature anomaly with a peak at 3.3 K is due to the ordering of Ho³⁺ ions and the estimated magnetic entropy for this transition was favorably compared with the expected (R ln 2). Application of magnetic field significantly affects the positions and the magnitudes of the anomaly at 3.3 K. Energies of low-lying levels of the lowest J-term of Ho³⁺ ion were roughly estimated through analysis of the Schottky heat capacity.     

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.     

Schottky-like anomaly in the low-temperature specific heat of single-crystal NdMnO3

The specific heat of single-crystal NdMnO₃ was investigated from 2 to 20 K under different magnetic fields up to 8 T. All the specific heat data show a Schottky-like anomaly, which becomes more indistinctive as increasing magnetic field. The experiment data were successfully fitted by taking into account factors such as crystal-field splitting, the two-level Schottky anomaly, the lattice vibration, and type-A antiferromagnetic (A-AF) spin waves. It was found that the splitting of the ground state doublet of Nd³⁺ ion increases linearly with magnetic field. The above phenomena can be interpreted in terms of the model of unchanged effective molecular field at Nd³⁺ site caused by the ferromagnetic component of A-AF structure of Mn spins. This ferromagnetic component is likely caused by the GdFeO₃-type octahedron rotation. In addition, it was also found that the magnetic field increases the spin-wave stiffness coefficient, but reduces the Debye temperature.     

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.     

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.     

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.     

Magnetic phase coexistence in Tb- and Sr-doped La0.7Ca0.3MnO3 manganite:A temperature-dependent neutron diffraction study

We report the results of the temperature-dependent neutron diffraction measurements on the nearly half-doped (La_0.325Tb_0.125)(Ca_0.3Sr_0.25)MnO₃ manganite sample. The simultaneous doping of magnetic Tb³⁺ and divalent Sr²⁺ in the La_0.7Ca_0.3MnO₃ system results into a large A-site size disorder. Rietveld refinement of neutron diffraction data reveal that the single phase sample crystallizes in a distorted orthorhombic structure. Increased 〈r_A〉 value affects the transport behavior that results into an insulating-like behavior of the sample. Under application of 1 T field sample exhibit insulating-like behavior while insulator-metal transition (T_IM) is exhibited under 5 and 8 T fields. Variable range hoping (VRH) mechanism of charge carriers is exhibited in the insulating region. Field cooled and zero field cooled magnetization measurement shows the Curie temperature (T_C)~47 K. The refinement of the ND data collected at various temperatures below 300 K shows that there is no structural phase transition in the compound. Around 100 K, a magnetic peak appears at lower angle that can be ascribed to the presence of the A-type antiferromagnetic (AFM) phase. Two more peaks are observed around 50 K at lower angles that can be fitted in CE-type antiferromagnetic phase. Splitting of the peaks at lower temperatures is the signature of orbital ordering in the presently studied nearly half-doped manganite system. Results of the detailed structural analysis of the temperature-dependent ND measurements on (LaTb)_0.45(CaSr)_0.55MnO₃ sample has been discussed in the light of coexisting A-type and CE-type antiferromagnetic phases present in the sample at low temperature.     

Infrared study in high magnetic fields of the crystal-field excitations in PrMnO3

Pr³⁺ ion crystal field (CF) excitations in PrMnO₃ single crystals have been studied by infrared transmission, in the 1800–8000 cm⁻¹ range, as a function of temperature and applied magnetic field up to 13 T. No noticeable frequency shifts which might occur below T_N∼100 K, as a result of the antiferromagnetic transition, are observed in the Pr³⁺ CF levels. A set of CF parameters that fit the experimental levels as well as the low temperature Pr³⁺ magnetic moment in PrMnO₃ has been determined.     

Magnetic field influence on the low temperature heat capacity of the spin-Peierls compound CuGeO3

We have investigated the effect of magnetic field on the low-temperature heat capacity C_p of the undoped spin-Peierls inorganic compound CuGeO₃ in the dimerized phase. Below 1 K, C_p is dominated by a Schottky anomaly, which is removed above 1 K for field B higher than 3 T. This anomaly is well accounted for by a molar concentration x=0.75×10⁻³ of intrinsic defects, which occur predominantly on the Cu chains. This amount is confirmed by magnetization measurements. A second contribution, varying as T^−ν with ν=1 or 2, rises up with the field for B>1 T in the lower temperature range (from 70 mK to 0.3 K). At high field this contribution becomes very sensitive to the experimental dynamics.     

A re-evaluation of the heat capacity of cerium zirconate (Ce2Zr2O7)

The heat capacity of cerium zirconate pyrochlore, Ce₂Zr₂O₇, was measured from 0.4 to 305 K by hybrid adiabatic relaxation method for various magnetic field strengths. Magnetisation measurements were performed on the sample also. The results revealed a low-temperature anomaly that showed Schottky-type characteristics with increasing magnetic field strength. The estimated entropy due to the magnetic ordering of the two Ce³⁺ moments is 1.37R, close to the theoretical value for a doublet ground state (1.39R). The enthalpy increments relative to 298.15 K were measured by drop calorimetry from 531 to 1556 K. The obtained results significantly differ from those reported in the literature; the origin of the discrepancy is due to the probable oxidation of the pyrochlore structure into fluorite.     

Effects of cation size disorder and lattice distortion on metamagnetism in phase-separated manganites

The effects of A-site cation size disorder in ABO₃ type charge-ordered and antiferromagnetic Pr_0.5Ca_0.5MnO₃ system have been studied by substituting La³⁺, Sr²⁺ or Ba²⁺, while keeping the valency of Mn ions and the tolerance factor (t=0.921) constant in the substituted compounds. We find that the substitutions by these larger cations induce successive sharp step-like metamagnetic transitions at 2.5 K. The critical field for metamagnetism is the lowest for 3% Ba substituted compound, which has the largest A-site cation size disorder and the least distorted MnO₆ octahedra, among the compounds reported here. These cation substitutions give rise to ferromagnetic clusters within antiferromagnetic matrix, indicating phase-separation at low temperatures. The growth of the clusters is found to vary with the substitution amount. The local lattice distortion of MnO₆ octahedra enhances the charge ordering temperature and reduces the magnetization at high fields (>1 T) in these manganites.     

Low temperature specific heat of bi-layered manganites La2−2xSr1+2xMn2O7 (x=0.3 and 0.5)

The specific heat (C) of bi-layered manganites La_2−2xSr_1+2xMn₂O₇ (x=0.3 and 0.5) is investigated for the ground state of low temperature excitations. A T^3/2 dependent term in the low temperature specific heat (LTSH) is identified at zero magnetic field and suppressed by magnetic fields for x=0.3 sample, which is consistent with a ferromagnetic metallic ground state. For x=0.5 sample, a T² term is observed and is consistent with a two-dimensional (2D) antiferromagnetic insulator. However, it is almost independent of magnetic field within the range of measured temperature (0.6-10 K) and magnetic field (6 T).     

Charge order melting and magnetic transition in Nd0.5(1+x)Ca0.5(1−x)Mn(1−x)CrxO3 system

The magnetic property of double doped manganite Nd_0.5(1+x)Ca_0.5(1−x)Mn_(1−x)Cr_xO₃ with a fixed ratio of Mn³⁺:Mn⁴⁺=1:1 has been investigated. For the undoped sample, it undergoes one transition from charge disordering to charge ordering (CO) associated with paramagnetic (PM)-antiferromagnetic (AFM) phase transition at T<250 K. The long range AFM ordering seems to form at 35 K, rather than previously reported 150 K. At low temperature, an asymmetrical M-H hysteresis loop occurs due to weak AFM coupling. For the doped samples, the substitution of Cr³⁺ for Mn³⁺ ions causes the increase of magnetization and the rise of T_c. As the Cr³⁺ concentration increases, the CO domain gradually becomes smaller and the CO melting process emerges. At low temperature, the FM superexchange interaction between Mn³⁺ and Cr³⁺ ions causes a magnetic upturn, namely, the second FM phase transition.     

Very high field magnetization and AC susceptibility of native horse spleen ferritin

The magnetization of native horse spleen ferritin protein is measured in pulsed magnetic fields to 55 T at T=1.52 K. The magnetization rises smoothly with negative curvature due to uncompensated Fe³⁺ spins and with a large high field slope due to the underlying antiferromagnetic ferritin core. Even at highest fields the magnetic moment is only ∼4% of the saturation moment of the full complement of Fe³⁺ in the ferritin molecule. The AC magnetic susceptibility, χ_AC(T,f), responding to the uncompensated spins, reaches a maximum near the superparamagnetic blocking temperature with the temperature of the maximum, T_M, varying with excitation frequency, T_M⁻¹ α log f for 10?f?10⁴ Hz.     

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.     

Effect of magnetic field on Nd0.7Pb0.3MnO3 single crystal

Magnetization and specific heat of Nd_0.7Pb_0.3MnO₃ single crystal are studied at applied magnetic field. Magnetization measurement at 0.3 T shows ferromagnetic phase below 150 K (T_C) and below 20 K displays an antiferromagnetic component. The latter appears to be destroyed at 4.8 T. This anomalous increase below 50 K is probably due to reorientation of Nd moments at high magnetic field. Heat capacity has been measured at 0-10 T at low temperature. The data have been fitted to contributions from free electrons (γ), ferromagnetic spin excitations (β_3/2), lattice and a Schottky-like anomaly related to the rare-earth magnetism of the Nd ions. Fitting yields that β_3/2 term is very small at 6 and 10 T because of introducing paramagnetic component in ferromagnetic phase at applied magnetic field. Peak due to Schottky anomaly is observed to be broadened with application of magnetic field and the magnitude of Schottky gap(Δ_Sch) also increases accordingly.     

Effect of Ca doping on the magnetic properties of Nd0.5Sr0.5MnO3 studied by electron spin resonance

The magnetic properties of Ca-doped Nd_0.5Sr_0.5MnO₃ have been studied by electron spin resonance (ESR) and dc magnetization measurements. The antiferromagnetic order and charge order are found to occur separately at T_N=200 K and T_co=150 K, respectively. Compared to the undoped Nd_0.5Sr_0.5MnO₃, the ferromagnetic correlations are suppressed by doping of the small Ca²⁺ ion. In addition, the antiferromagnetic transition temperature is enhanced to 200 K, which can be explained by an increase of superexchange interaction between Mn³⁺ and Mn⁴⁺ ions as their distance decreases.     

Electrical and magnetic properties of TmCoIn5 and YbCoIn5 single crystals

Electrical and magnetic properties of TmCoIn₅ and YbCoIn₅ single crystals were investigated by means of electrical resistivity and magnetization measurements in the temperature range from 300 to 0.5 K under the magnetic field up to 5 T. TmCoIn₅ is an antiferromagnetic metal with a Néel temperature T_N=2.6 K. YbCoIn₅ shows non-magnetic behavior, reflecting of divalent Yb ion.     

Mössbauer spectroscopy as a probe of magnetic states in La0.5Ca0.5FeO3−δ perovskite

Charge disproportionation in La_0.5Ca_0.5FeO_3−δ perovskite has been detected by zero-field Mössbauer spectra from 20 K to room temperature. On the basis of the parameters of center shifts and hyperfine fields, Mössbauer spectra identified that the iron ionic states are Fe³⁺ and Fe⁵⁺ below 150 K, Fe³⁺, Fe⁴⁺ and Fe⁵⁺ in the intermediate temperature region, as well as Fe³⁺ and Fe⁴⁺ above 220 K. At low temperatures, the system exhibits a cluster-glass-like state resulting from competition between antiferromagnetic interaction of Fe³⁺–Fe³⁺ and ferromagnetic interaction of Fe³⁺–Fe⁵⁺.     

Antiferromagnetic order and spin glass behavior in Dy2CuIn3

The magnetic properties of the intermetallic compound Dy₂CuIn₃ have been investigated. Ac and dc-susceptibility measurements indicate an onset of antiferromagnetic ordering at T_N=19.5 K and an additional frequency dependent transition at T_ds∼9 K. Neutron diffraction studies confirm the ordered transition at 19.5±1 K. The magnetic unit cell can be described by the propagation vector k=(0.25,0.25,0) with the magnetic moment μ=2.63(4)μ_B/Dy³⁺ parallel to the c-axis. Nevertheless, neutron diffraction reveals no additional magnetic phase transition around or below 9 K, which suggests that, at lower temperatures, a spin glass state may be formed in coexistence with the antiferromagnetic mode as a result of frustration and the antagonism between ferromagnetic and antiferromagnetic exchange interactions.