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.     

Low temperature thermodynamical properties of ErCu2Si2

ErCu₂Si₂ crystallises in the tetragonal ThCr₂Si₂-type crystal structure. In this paper results of magnetometric, electrical transport, specific heat as well as neutron diffraction are reported. Results of electrical resistivity and specific heat measurements performed at low temperature yield existence of magnetic ordering roughly at 1.3 K. These results are in concert with neutron diffraction measurements, which reveal simple antiferromagnetic ordering between 0.47 and 1.00 K. At temperatures ranging from 1.00 up to 1.50 K an additional incommensurate magnetic structure was observed. The propagation vector k=(0;0;0.074) was proposed to describe magnetic reflections within the amplitude modulated magnetic structure. Basing on specific heat studies the crystal field levels splitting scheme and magnetic entropy were calculated.     

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.     

Effect of pressure and magnetic field on bilayer La1.25Sr1.75Mn2O7 single crystal

We report the temperature dependence of susceptibility for various pressures, magnetic fields and constant magnetic field of 5 T with various pressures on La_2−2xSr_1+2xMn₂O₇ single crystal to understand the effectiveness of pressure and magnetic field in altering the magnetic properties. We find that the Curie temperature, T_c, increases under pressure (dT_c/dP=10.9 K/GPa) and it indicates the enhancement of ferromagnetic phase under pressure up to 2 GPa. The magnetic field dependence of T_c is about 26 K for 3 T. The combined effect of pressure and constant magnetic field (5 T) shows dT_c/dP=11.3 K/GPa and the peak structure is suppressed and broadened. The application of magnetic field of 5 T realizes 3D spin ordered state below T_c at atmospheric pressure. Both peak structure in χ_c and 3D spin ordered state are suppressed, and changes to 2D-like spin ordered state by increase of pressure. These results reveal that the pressure and the magnetic field are more competitive in altering the magnetic properties of bilayer manganite La_1.25Sr_1.75Mn₂O₇ single crystal.     

Anisotropic and large low-field magnetic entropy change in a La4/3Sr5/3Mn2O7 single crystal

We have studied the magnetocaloric effect (MCE) in a bilayered La_4/3Sr_5/3Mn₂O₇ single crystal with applied field along both ab-plane and c-direction. Due to the quasi-two-dimensional structure, the crystal exhibits a strong anisotropy in the MCE. The difference of magnetic entropy change between two crystallographic directions depends on external magnetic fields and has a maximum of 2 J/kg K. A large low-field magnetic entropy change, reaching 3.2 J/kg K for a magnetic field change of 15 kOe, is observed when the applied field is along ab-plane. This large low-field magnetic entropy change is attributed to the rapid change of magnetization in response to external magnetic fields in the easy magnetizing plane.     

Magnetic ordering in the frustrated system FeSc2S4

The sample of FeSc₂S₄ was prepared by solid reaction method. The crystallographic structure and the magnetic properties of the fabricated compound were investigated by X-ray, and superconducting quantum interference device (SQUID) magnetometer and Mössbauer spectroscopy. The polycrystalline FeSc₂S₄ confirmed the normal cubic spinel structure (space group Fd3m). The lattice constants a₀ and anion parameter u are 10.519 Å and 0.255, respectively. The Mössbauer spectroscopy has been studied for the FeSc₂S₄ at various temperatures, ranging from 4.2 K to room temperature. The spectra consist of two doublets at 4.2 K while a single line at room temperature. It is noticeable that the Mössbauer spectra of two doublet patterns with large electric quadrupole splitting (ΔE_Q) remain over the Néel temperature. Those are interpreted as a result of large electric quadrupole interaction compared to magnetic dipole interaction. The magnetic susceptibility measurements were performed with a SQUID magnetometer for temperatures 2<T<320 K, in external fields up to 5 kOe. Magnetic behavior shows antiferromagnetic behavior and the magnetic superexchange interactions between the Fe ions are weakly antiferromagnetic. The paramagnetic susceptibilities follow Curie–Weiss (CW) law with CW temperature Θ_CW=−100 K, and frustration parameter f=−Θ_CW/T_N is of the order of 1000. We conclude that two sublattices are coupled antiferromagnetically, leading to strong frustration effects.     

Antiferromagnetic phase transition in garnet-type AgCa2Co2V3O12 and AgCa2Ni2V3O12

Antiferromagnetic phase transition in two vanadium garnets AgCa₂Co₂V₃O₁₂ and AgCa₂Ni₂V₃O₁₂ has been found and investigated extensively. The heat capacity exhibits sharp peak due to the antiferromagnetic order with the Néel temperature T_N=6.39 K for AgCa₂Co₂V₃O₁₂ and 7.21 K for AgCa₂Ni₂V₃O₁₂, respectively. The magnetic susceptibilities exhibit broad maximum, and these T_N correspond to the inflection points of the magnetic susceptibility χ a little lower than T(χ_max). The magnetic entropy changes from zero to 20 K per mol Co²⁺ and Ni²⁺ ions are 5.31 J K⁻¹ mol-Co²⁺-ion⁻¹ and 6.85 J K⁻¹ mol-Ni²⁺-ion⁻¹, indicating S=1/2 for Co²⁺ ion and S=1 for Ni²⁺ ion. The magnetic susceptibility of AgCa₂Ni₂V₃O₁₂ shows the Curie-Weiss behavior between 20 and 350 K with the effective magnetic moment μ_eff=3.23 μ_B Ni²⁺-ion⁻¹ and the Weiss constant θ=−16.4 K (antiferromagnetic sign). Nevertheless, the simple Curie-Weiss law cannot be applicable for AgCa₂Co₂V₃O₁₂. The complex temperature dependence of magnetic susceptibility has been interpreted within the framework of Tanabe-Sugano energy diagram, which is analyzed on the basis of crystalline electric field. The ground state is the spin doublet state ²E(t₂⁶e) and the first excited state is spin quartet state ⁴T₁(t₂⁵e²) which locates extremely close to the ground state. The low spin state S=1/2 for Co²⁺ ion is verified experimentally at least below 20 K which is in agreement with the result of the heat capacity.     

Spin glass like behavior in Cd0.42Mn0.58In2S4

The magnetic behavior of the diluted magnetic semiconductor Cd_0.42Mn_0.58In₂S₄ has been study by dc magnetization and ac susceptibility experiments. Zero field cooled and field cooled measurements reveal irreversibility below T_irr=2.60±0.15 K. Ac susceptibility data, performed as a function of the temperature and the frequency, confirm the spin-glass like behavior of the material with T_f=2.75±0.15 K. High temperature susceptibility data follow a typical Curie-Weiss law with θ=−74±1 K which suggests predominant antiferromagnetic interactions. The randomness of the magnetic ions, necessary to explain the magnetic behavior of the material, has been determined by X-ray powder diffraction experiments.     

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.     

Neutron diffraction studies of Tb2Rh3Si5 compound

In this work neutron diffraction studies of Tb₂Rh₃Si₅ compound are reported. The compound crystallizes in the monoclinic crystal structure of Lu₂Co₃Si₅-type. At 1.5 K an antiferromagnetic ordering with a propagation vector k=(1/2;1/2;1/2) was observed. The Tb magnetic moments of 9.8(2) μ_B form a non-collinear magnetic structure. In the vicinity of Néel temperature of 8 K a change of the magnetic ordering is evidenced. The change seems to be connected with phase transition from commensurate to incommensurate sine-wave modulation of the Tb magnetic moments.     

Magnetic and transport properties of Pr2Pd3Si5

We have investigated the magnetic and transport properties of a new ternary intermetallic compound Pr₂Pd₃Si₅ which forms in U₂Co₃Si₅-type orthorhombic structure (space group Ibam). At low field (0.01 T) magnetic susceptibility exhibits an abrupt increase below 7 K and peaks at 5 K, revealing a magnetic phase transition. The onset of magnetic order is also confirmed by well defined anomalies in the specific heat and electrical resistivity data. Apart from the sharp λ-type anomaly, magnetic part of specific heat also shows a broad Schottky-type hump due to crystal field effect. Magnetoresistance data as a function of temperature exhibits a pronounced peak in paramagnetic state which could be interpreted in terms of crystal field effect and short-range ferromagnetic correlations.     

Synthesis and physical characterization of superconductivity-magnetism crossover compound RuSr2EuCeCu2O10−δ

We carefully studied the nonsuperconducting sample of the magneto-superconducting RuSr₂(Eu_1−xCe_x)Cu₂O_10−δ series with composition RuSr₂EuCeCu₂O_10−δ. This compound seems to exhibit a complex magnetic state as revealed by host of techniques like resistivity, thermopower, magnetic susceptibility, and MR measurements. The studied compound exhibited ferromagnetic like M(H) loops at 5, 20, and 50 K, and semiconductor like electrical conduction down to 5 K, with −MR^7 T of up to 4% at low temperatures. The −MR^7 T decreases fast above 150 K and monotonically becomes close to zero above say 230 K. Below, 150 K −MR^7 T decreases to around 3% monotonically down to 75 K, with further increase to 4% at around 30 K and lastly having a slight decrease below this temperature. The thermopower S(T) behavior closely followed the −MR^7 T steps in terms of d(S/T)/dT slopes. Further, both MR^7 T steps and d(S/T)/dT slopes are found in close vicinity to various magnetic ordering temperatures (T_mag) of this compound.     

Crystal and magnetic structures of Y2CrS4

Chromium(II) sulfide, Y₂CrS₄, prepared by a solid-state reaction of Y₂S₃ and CrS, showed an antiferromagnetic transition at 65 K. The neutron diffraction patterns at 10 and 90 K were both well refined with the space group Pca2₁. At 90 K, cell parameters were a=12.5518(13) Å, b=7.5245(8) Å, and c=12.4918(13) Å. At 10 K, magnetic peaks were observed, which could be indexed on the same unit cell. Magnetic moments of chromium ions were parallel to the b-axis and antiferromagnetically ordered in each set of the 4a sites.     

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.     

High pressure effects on the electrical resistivity behavior of the Kondo lattice, YbPd2Si2

We report the influence of external high-pressure (P up to 8 GPa) on the temperature (T) dependence of electrical resistivity (ρ) of a Yb-based Kondo lattice, YbPd₂Si₂, which does not undergo magnetic ordering under ambient pressure condition. There are qualitative changes in the ρ(T) behavior due to the application of external pressure. While ρ is found to vary quadratically below 15 K (down to 45 mK) characteristic of Fermi-liquids, a drop is observed below 0.5 K for P=1 GPa, signaling the onset of magnetic ordering of Yb ions with the application of P. The T at which this fall occurs goes through a peak as a function of P (8 K for P=2 GPa and about 5 K at high pressures), mimicking Doniach's magnetic phase diagram. We infer that this compound is one of the very few Yb-based stoichiometric materials, in which one can traverse from valence fluctuation to magnetic ordering by the application of external pressure.     

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.     

Ground-state magnetism of chromium-substituted LiMn2O4 spinel

Comparative crystal structure and magnetic properties studies have been conducted on quaternary powder spinel samples LiMn_1.82Cr_0.18O₄ obtained by two different synthesis methods, glycine-nitrate (GN) and ultrasonic spray-pyrolysis (SP). Although both samples possess the same spinel structure of the cubic space group Fd3¯m, their low-temperature magnetic properties display significant differences. While the SP sample undergoes only spin-glass transition at the freezing temperature T_f=20 K, the GN sample possesses more complicated low-temperature magnetic behavior of the reentrant spin-glass type with the Néel temperature T_N=42 K and freezing temperature T_f=22 K. High-temperature magnetic susceptibility of both samples is of the Curie–Weiss type with the effective magnetic moments in agreement with the nominal compositions. This fact together with the results of the chemical analysis discards the existence of the diversity in chemical compositions as a possible cause for the observed differences in the low-temperature magnetism. On the other hand, the crystal structure analysis done by the Rietveld refinement of the X-ray powder diffraction data points to the strong influence of the cation distribution on the ground-state magnetism of these systems. An explanation of this influence is proposed within the framework of a collective Jahn–Teller effect.     

Mössbauer study of antiferromagnetic CuFeO2

We have studied the magnetic spin structure of antiferromagnetic CuFeO₂ by X-ray diffraction (XRD) and Mössbauer spectroscopy. Its crystal structure determined by XRD analysis was a rhombohedral structure (space group R-3m) and lattice constants a₀ and c₀ were 3.0333 and 17.1595 Å, respectively. In spite of 4-Fe sublattices in a delafossite CuFeO₂, its Mössbauer spectra were analyzed with 1-set (6-Lorentzian lines) below 10 K due to the collinear-commensurate spin structure, but the spectra were fitted with 4-sextet above 10 K due to the incommensurate spin structure. This phenomenon was attributed to the spin–lattice relaxation effect. Magnetic Néel temperature was also determined at 18 K, which corresponded to the high-spin Fe³⁺ valance state. On the other hand, CuFe_0.98Al_0.02O₂ powder with a noncollinear spin structure was fitted with 4-sextet at 4.2 K.     

Magnetocaloric effect in R2Fe17 (R=Sm,Gd, Tb,Dy, Er)

A series of R₂Fe₁₇ (R=Sm, Gd, Tb, Dy, Er) have been synthesized. The magnetocaloric effect (MCE) of these compounds has been investigated by means of magnetic measurements in the vicinity of their Curie temperature. The Curie temperature of Er₂Fe₁₇ is 294 K. The maximum magnetic entropy change of Er₂Fe₁₇ under 5 T magnetic field is ∼3.68 J/kg K. In the R₂Fe₁₇ (R=Sm, Gd, Tb, Dy, Er) system, the maximum magnetic entropy change under 1.5 T magnetic field is 1.72, 0.89, 1.32, 1.59, 1.68 J/kg K corresponding to their Curie temperature (400, 472, 415, 364, 294 K), respectively.