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.     

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.     

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.     

Spin-glass-like behavior in ZnxCryAlzSe4

The magnetic and electrical properties of the Al-doped polycrystalline spinels Zn_xCr_yAl_zSe₄ (0.13≤z≤0.55) with the antiferromagnetic (AFM) order and semiconducting behavior were investigated. A complex antiferromagnetic structure below a Néel temperature T_N≈23 K for the samples with z up to 0.4 contrasting with the strong ferromagnetic (FM) interactions evidenced by a large positive Curie-Weiss temperature θ_CW decreasing from 62.2 K for z=0.13 to 37.5 K for z=0.55 was observed. Detailed investigations revealed a divergence between the zero-field-cooling (ZFC) and field-cooling (FC) susceptibilities at temperature less than T_N suggesting bond frustration due to competing ferromagnetic and antiferromagnetic exchange interactions in the compositional range 0.13≤z≤0.4. Meanwhile, for z=0.55 a spin-glass-like behavior of cluster type with randomly oriented magnetic moments is observed as the ZFC-FC splitting goes up to the freezing temperature T_f=11.5 K and the critical fields connected both with a transformation of the antiferromagnetic spin spiral via conical magnetic structure into ferromagnetic phase disappear.     

Magnetic properties for the Cu2MnSnSe4 and Cu2FeSnSe4 compounds

Magnetic susceptibility χ measurements in the range from 2 to 300 K were carried out on samples of the Cu₂FeSnSe₄ and Cu₂MnSnSe₄ compounds. It was found that Cu₂FeSnSe₄ was antiferromagnetic showing ideal Curie-Weiss behavior with a Néel temperature T_N of about 19 K and Curie-Weiss temperature θ=−200 K, while for Cu₂MnSnSe₄ the behavior was spin-glass with a freezing temperature T_f of about 22 K and Curie-Weiss temperature θ=−25 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.     

Charge and lattice dynamics of ordered state in La1/2Ca1/2MnO3: infrared reflection spectroscopy study

We report an infrared reflection spectroscopy study of La_1/2Ca_1/2MnO₃ over a broad frequency range and temperature interval which covers the transitions from the high temperature paramagnetic to ferromagnetic and, upon further cooling, to antiferromagnetic phase. The structural phase transition, accompanied by a ferromagnetic ordering at T_C=234 K, leads to enrichment of the phonon spectrum. A charge ordered antiferromagnetic insulating ground state develops below the Néel transition temperature T_N=163 K. This is evidenced by the formation of charge density waves and opening of a gap with the magnitude of 2Δ₀=(320±15) cm⁻¹ in the excitation spectrum. Several of the infrared active phonons are found to exhibit anomalous frequency softening. The experimental data suggest coexistence of ferromagnetic and antiferromangetic phases at low temperatures.     

Magnetoelectric effect in perovskite quantum paraelectric EuTiO3

On the basis of successful theoretical explanation of the observed large magnetic-field effect (by ∼7% with 1.5 T) on the dielectric constant below the Néel temperature T_N of 5.5 K, we have demonstrated convincingly the magnetoelectric effect in an antiferromagnetic quantum paraelectric EuTiO₃ system. The mutual control of electric and magnetic properties is revealed by the variation of the electric-field-induced polarization with applied magnetic fields as well as the change of the magnetic-field-induced spin moments under the control of electric fields. It is found that the applied electric field (magnetic field) acts like a fictitious magnetic field (electric field) on the EuTiO₃ system. The magnetoelectric susceptibility is deduced to be proportional to the product of the magnetization, electrical polarization, magnetic susceptibility and dielectric susceptibility.     

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.     

Mössbauer study of CoFeRhO4

CoFeRhO₄ has been studied by Mössbauer spectroscopy and X-ray diffraction. The crystal is found to have a cubic spinel structure with the lattice constant a₀=8.451±0.005 Å. The iron ions are in ferric states. The temperature dependence of the magnetic hyperfine field is analyzed by the Néel theory of ferrimagnetism. The intersublattice superexchange interaction is antiferromagnetic and strong with a strength of J_AB=−12.39k_B while the intrasublattice superexchange interactions are weak with strengths of J_AA=−4.96k_B and J_BB=6.20k_B. As the temperature increases toward the Néel temperature T_N, a systematic line broadening effect in the Mössbauer spectrum is observed and interpreted to originate from different temperature dependences of the magnetic hyperfine fields at various iron sites.     

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.     

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.     

Magnetic phase diagram of Tb3−xHoxCu4Sn4 system

Magnetic phase diagram of Tb_3−xHo_xCu₄Sn₄ was determined on the basis of magnetic and heat capacity data. X-ray diffraction data proved that these compounds crystallize in the orthorhombic Gd₃Cu₄Ge₄-type structure. The compounds are antiferromagnets at low temperatures and the reciprocal magnetic susceptibility obeys the Curie-Weiss law. The paramagnetic Curie temperatures are negative and their absolute values decrease with increasing Ho content. An anomalous concentration dependence of the Néel temperature is observed.     

Magnetic structure of TbNiAl4

Magnetisation and specific heat measurements, in the range 2 K to room temperature, demonstrate that three magnetic phases exist for the intermetallic compound TbNiAl₄. Powder neutron diffraction, also carried out over a wide temperature range, establishes that the intermediate magnetic phase is incommensurate, and confirms that the lowest temperature phase has a linear antiferromagnetic structure with a (0 1 0) propagation vector. The respective transition (Néel) temperatures, in zero applied magnetic field are 34.0 and 28.0 K.     

Proton NMR study of α-MnH0.06

Proton nuclear magnetic resonance (NMR) spectra and spin-lattice relaxation rates for the solid solution α-MnH_0.06 have been measured over the temperature range 11-297 K and the resonance frequency range 20-90 MHz. A considerable shift and broadening of the proton NMR line and a sharp peak of the spin-lattice relaxation rate are observed near 130 K. These effects are attributed to the onset of antiferromagnetic ordering below the Néel temperature T_N≈130 K. The proton NMR line does not disappear in the antiferromagnetic phase; this suggests a small magnitude of the local magnetic fields at H-sites in α-MnH_0.06. The spin-lattice relaxation rate in the paramagnetic phase is dominated by the effects of spin fluctuations.     

Antiferromagnetic resonance study of sodalite loaded with sodium by multi-frequency ESR

We have carried out electron spin resonance (ESR) measurements on powder samples of sodalite loaded with Na at several frequencies between 9.7 and 35 GHz and at temperatures between 1.5 and 60 K. The ESR absorption spectrum below a Néel temperature T_N turns into an asymmetric spectrum with a long tail at low fields from a symmetric one above T_N. The line shape of the spectra below T_N is analyzed by a powder pattern simulation of the antiferromagnetic resonance spectra with easy-plane anisotropy. The calculated line shape reproduces the experimental one considerably well by assuming a Gaussian distribution of the zero-field energy gap. We have evaluated a small anisotropy field of about 2×10⁻⁴ T by using the exchange coupling constant calculated from the Weiss and the Néel temperatures. This result indicates that the sodalite loaded with Na is quite an ideal Heisenberg antiferromagnet as expected from the s-electron character of Na clusters and the cubic arrangement of nano-spaces in the sodalite.     

Ferromagnetic semiconductor Ge1−x−ySnxMnyTe with phase transformation of ferroelectric type

It is expected that joint existence of ferromagnetic properties and ferroelectric structural phase transition in diluted magnetic semiconductors IV-VI leads to new possibilities of these materials. Temperature of ferroelectric transition for such crystals can be tuned by the change of Sn/Ge ratio. Magnetic susceptibility, Hall effect, resistivity and thermoelectric power of Ge_1−x−ySn_xMn_yTe single crystals grown by Bridgeman method (x=0.083-0.115; y=0.025-0.124) were investigated within 4.2-300 K. An existence of FM ordering at T_C∼50 K probably due to indirect exchange interaction between Mn ions via degenerated hole gas was revealed. A divergence of magnetic moment temperature dependences at T?T_C in field-cooled and zero-field-cooled regimes is obliged to magnetic clusters which are responsible for superparamagnetism at T>T_C≈T_f (freezing temperature) and become ferromagnetic at T_C arranging spin glass state at T<T_f≈T_C. Phase transition of ferroelectric type at T≈46 K was revealed. Anomalous Hall effect which allows to determine magnetic moment was observed.     

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 field magnetoresistance and conduction noise in layered manganite La1.4Ca1.6Mn2O7

Temperature dependence of conduction noise and low field magnetoresistance of layered manganite La_1.4Ca_1.6Mn₂O₇ (DLCMO) are reported and compared with the infinite layered manganite La_0.7Ca_0.3MnO₃ (LCMO). The double layered manganite was prepared using standard solid state reaction method and had a metal-insulator transition temperature (T_M-I) of 155 K. The temperature dependence of susceptibility showed evolution of ferromagnetic ordering at 168 K. The observed voltage noise spectral density (S_V) shows 1/f^α type of behaviour at all temperatures from 77 K to 300 K. In the ferromagnetic region (T<168 K), S_V/V² shows two peaks at 164 K and 114 K. The observed two peaks in normalised conduction noise of DLCMO is attributed to the excess noise generated due to setting up of short range 2D-ferromagnetic ordering and long range 3D-ferromagnetic ordering at two different temperatures T_C2 and T_C1. In temperature range between T_C1 and T_C2, the magnetoresistance (MR) showed a gradual increase with the magnetic field. The observed MR has been explained in the framework of the two phase model [ferromagnetic (FM) domains and paramagnetic (PM) regions].     

Magnetic and structural studies of the double perovskites Ba2REMoO6

A magnetic, electronic and structural study of the double perovskites Ba₂REMoO₆ (RE=Sm, Eu, Gd, Dy) has been performed. All materials crystallise in the cubic symmetry space group and the cell volume decreases as RE varies from Sm to Dy in accordance with Vegard's law. An antiferromagnetic transition is observed below T_N=130 and 112 K for RE=Sm and Eu, respectively. The Néel temperatures of these ordered rare earth molybdenum double perovskites are much higher than previously observed in double perovskites containing Eu or Sm and a 4d or 5d transition metal arranged in an ordered rock salt configuration. The high Néel temperatures arise due to a strong superexchange magnetic interaction via the Mo-O-RE-O-Mo pathway. All of the phases are electronically insulating and there is no evidence of magnetoresistance at any temperature.     

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.