Anisotropic dielectric properties of PbYb1/2Ta1/2O3 single crystals

PbYb_1/2Ta_1/2O₃ single crystals were obtained for the first time. They were grown by the flux method. The PbOPbF₂B₂O₃ system was used as a solvent. Dielectric investigations were carried out in 1 0 0_c, 1 1 0_c and 1 1 1_c pseudocubic directions. These studies pointed to anisotropy of dielectric properties. Frequency-independent ε′(T) and ε″(T) maxima related to the antiferroelectric–paraelectric (AFE—PE) phase transition are observed for all directions at 562 K. The frequency-dependent ε′(T) and ε″(T) maxima near 400 K related to the ferroelectric (FE)–AFE phase transition are observed only in 1 1 1_c direction. The hysteresis loops were observed in this direction only. These results point that ferroelectric relaxor properties appear only in 1 1 1_c direction. We propose to consider the ferroelectric phase as ferrielectric one.     

Magnetic phase transition in (Fe,Mn)65Ni35 alloys

Magnetization measurements on the Fe₆₀Mn₅Ni₃₅ and Fe₅₀Mn₁₅Ni₃₅ alloy samples were carried out in the temperature range 80T300 K and in magnetic fields up to 8 kOe. The Fe₆₀Mn₅Ni₃₅ was found to order ferromagnetically with a Curie temperature, T_c, above 300 K. From the temperature dependence of the spontaneous magnetization, M_s, it was concluded that the magnetic behavior of Fe₆₀Mn₅Ni₃₅ follows Wohlfarth theory of weak itinerant ferromagnet. The Fe₅₀Mn₁₅Ni₃₅ sample exhibits a magnetic phase transition from ferromagnetism to paramagnetism at T_c=242 K. The critical amplitudes and critical exponents (β, γ and δ) have been determined by using Arrott plots, Kouvel–Fisher method and scaling plots of the reduced magnetization and reduced magnetic field. The values of β, γ and δ are discussed and compared with the results obtained for various theoretical models and also with the experimentally determined values for related systems obtained by others.     

Phase transition in Pb4.9A0.1Ge2.7Si0.3O11 (A=Ca,Sr,Ba) ferroelectrics

Polycrystalline samples of modified lead germanate Pb_4.9A_0.1Ge_2.7Si_0.3O₁₁ (A=Ca,Sr,Ba) have been prepared by solid-state reaction technique. X-ray studies have been carried out to check the formation of single-phase composition and to obtain preliminary structural data. Measurements of dielectric permittivity () and loss (tan δ) have been studied both as a function of frequency (10²–10⁴ Hz) and temperature (room temperature to 180°C). Phase transition was observed in all three cases but with different T_c value. From the plots of conductivity vs. temperature using dielectric data, collected at 10 kHz activation energy was calculated to investigate the conduction mechanism in them.     

Pressure–temperature studies on conductivity of TlX(X=Cl,Br,I) compounds:: I: phase diagram. II: ionic mobility

We have measured the conductivity σ of TlX(X=Cl, Br, I) compounds up to 5.3 GPa and between 300–823 K. The σ–T dependence for all compounds can be divided into three distinct regions: (i) low temperature (LT), <400 K, with unusual negative σ–T dependence, (ii) intermediate temperature (IT), 400<650 K, with positive σ–T dependence and (iii) high temperature (HT), T>650 K, with positive σ–T dependence. The σ–T isobars were used to construct the T–P solid phase diagram for each compound. The LT region data indicate a new meta-stable phase in the 1.0–3.5 GPa range. The LT→IT transition is characterized by an inverse σ–T dependence followed by normal Arrhenius behavior up to and including the HT region. The extrapolation to 1 atm of the P-dependent boundary between IT and HT regions above 3 GPa for each compound in the P–T plot yields a value close to its respective normal (1 atm) T_melt suggesting a solid order–disorder transition type paralleling -AgI behavior. The abrupt drop in conductivity in the LT region for P between 2.5–4.1 GPa of all compounds is at variance with the Arrhenius behavior observed for unperturbed ion migration implying the appearance of a second factor overriding the Arrhenius temperature dependence. Normal Arrhenius σ–T dependence prevails in both IT and HT regions with Q_c values of 85–100 kJ mol⁻¹ and 50–75 kJ mol⁻¹, respectively. The higher conductivities at 0.4 GPa for TlBr and TlI relative to their 1 atm data and the increasing σ with P are in strong contrast to the normal σ-P behavior of TlCl. The dependence of activation volume ΔV^‡ on T for TlCl, i.e. ΔV^‡>0, shows abnormally high values with a maximum at 500 K for P<3.0 GPa but reasonable ΔV^‡ values appear above 3.0 GPa. The ΔV^‡–T dependence for both TlBr and TlI with ΔV^‡<0 is incompatible with an ion transport mechanism suggesting an electronic conduction process and implying an ionic–metallic transition at higher pressures. These contrasting conductivity features are discussed and interpreted in terms of electronegativity differences and bonding character rather than structure.     

Peak effect and oxygen ordering in YBa2Cu3O7−δ single crystals

We have investigated the second magnetization peak in pure YBa₂Cu₃O_7−δ single crystals with various oxygen contents (6.91<7−δ<6.97) and degrees of oxygen vacancy ordering, as achieved by low (1 bar) and high (100 bar) oxygen pressure annealing. Although the position of the peak changes drastically with oxygen stoichiometry, no dependence on the distribution of oxygen vacancies has been found for temperatures below 70 K. For T>70 K, however, ordering effects become important as demonstrated by the disappearance of the peak for the high pressure annealed samples. These results suggest that while at low temperatures, pinning of the vortex system by clusters or a more homogeneous distribution of oxygen vacancies is similar, at elevated T, the former are much stronger pinning sites leading to larger hysteresis and the presence of the peak.     

Double peak behavior of resistivity curves in Cd doped LaMnO3 perovskite systems

The effect of Cd doping on transport, magnetotransport, and magnetic properties has been investigated in the perovskite La_1−xCd_xMnO₃ (0x0.5) systems. The ρ(T) curves exhibit a sharp metal insulator transition (T_p1), which is close to paramagnetic to ferromagnetic transition (T_c) obtained from M−T curves for all samples. In addition, ρ(T) curves for Cd doped samples exhibit another broad transition (T_P2) below T_p1. This transition becomes more prominent and the transition temperature (T_p2) shifts to lower temperature with increasing Cd content. Such double peak behavior in the ρ(T) curve is attributed to the phase separation between the ferromagnetic metallic phases and the ferromagnetic insulating phases induced by the electronic inhomogeneity in the samples.     

Investigation of the static and dynamic magnetic properties of CoFe2O4 nanoparticles

We have investigated the magnetic behavior of cobalt ferrite nanoparticles with a mean diameter of 7.2 nm. AC susceptibility of colloidal cobalt ferrite nanoparticles was measured as a function of temperature T from 2 to 300 K under zero external DC field for frequencies ranging from f=10 to 10,000 Hz. A prominent peak appears in both χ′ and χ″ as a function of T. The peak temperature T₂ of χ″ depends on f following the Vogel–Fulcher law. The particles show superparamagnetic behavior at room temperature, with transition to a blocked state at T_B^m94 K in ZFC and 119 K in AC susceptibility measurements, respectively, which depends on the applied field. The saturation magnetization and the coercivity measured at 4.2 K are 27.3 emu/g and 14.7 kOe, respectively. The particle size distribution was determined by fitting a magnetization curve obtained at 295 K assuming a log-normal size distribution. The interparticle interactions are found to influence the energy barriers yielding an enhancement of the estimated magnetic anisotropy, K=6×10⁶ erg/cm³. Mössbauer spectra obtained at higher temperatures show a gradual collapse of the magnetic hyperfine splitting typical for superparamagnetic relaxation. At 4.2 K, the Mössbauer spectrum was fitted with two magnetic subspectra with internal fields H_int of 490, 470 and 515 kOe, corresponding to Fe³⁺ ions in A and B sites.     

Magnetic properties of YCo5 (70%wt)+Y2Co17 (30%wt) nanocomposite powders at low temperatures

Nanostructured YCo₅ (70%wt)+Y₂Co₁₇ (30%wt) composite powders were prepared by mechanical milling and subsequent annealing at 1073 K for 1.5 min. The average grain size D of the YCo₅ and Y₂Co₁₇ phases, obtained from XRD data, was 14 and 12 nm, respectively. The temperature dependence of the magnetic properties was studied by DC magnetization measurements at temperatures T ranging from 3 to 300 K. Hysteresis loops (H_max=70 kOe) show that both the coercivity H_C and the squareness σ_r/σ_max are temperature-dependent. The coercivity increases from 12 kOe at room temperature to 18 kOe at T=3 K. The observed enhanced remanence (σ_r/σ_max>0.5) indicates that a strong exchange coupling is present at all temperatures used in this study. The maximum magnetization σ_max changes little with temperature and has a value of about 70% of the effective saturation magnetization of the title compound.     

Linear and nonlinear critical magnetic properties and transport in Nd0.75Ba0.25MnO3 single crystal: evidence for its anomalous critical behavior near TC

The data on the resistance and magnetoresistance (MR) as well as measurements of the linear and nonlinear susceptibilities are presented for a Nd_0.75Ba_0.25MnO₃ single crystal with the Curie temperature T_C≈129 K. Although this compound remains insulating in the ferromagnetic state, its resistance has an anomaly near T_C and it reveals the colossal magnetoresistance. The data on the magnetic response are well described by the dynamic scaling theory for 3D isotropic ferromagnets in the paramagnetic critical region at τ>τ^*≈0.11, τ=(T−T_C)/T_C. Below τ^* an anomalous critical behavior is found that suggests the coexistence of two magnetic phases. This behavior is discussed in terms of a phase separation which can occur in the moderately doped manganites exhibiting an orbital ordering.     

Thermodynamic properties of the clathrate-type silver-oxide Ag6O8AgHF2

We report normal-state and superconducting properties of the clathrate-type silver-oxide Ag₆O₈AgHF₂. We present electrical resistivity, DC- and AC-susceptibility and specific-heat measurements of single crystalline Ag₆O₈AgHF₂. In the normal state, Ag₆O₈AgHF₂ exhibits metallic conductivity and a phase transition near 110 K, possibly a structural phase transition as observed in the related compound Ag₆O₈AgNO₃. The onset of superconductivity of our samples is observed around 1.2–1.5 K, and the H–T phase diagram is determined for the first time. The upper critical field H_c2(0) is estimated to be about 2000–2200 Oe and the coherence length ξ_GL(0) to be 40 nm.     

Specific heat and anisotropic superconducting and normal-state magnetization of HoNi2B2C

The magnetization of single-crystal HoNi₂B₂C has been measured as a function of applied field (H) and temperature in order to probe the interplay between superconductivity and magnetism in this complex layered system. The normal-state magnetic susceptibility of HoNi₂B₂C is highly anisotropic with a Curie-Weiss-like temperature dependence for H applied perpendicular to the c-axis and with a much weaker temperature dependence for H applied parallel to the c-axis, indicating that the Ho⁺³ magnetic moments lie predominately in the tetragonal a−b plane below 20 K. High-field magnetization (2000 Oe), low-field magnetization (20 Oe) and zero-field specific heat all give an antiferromagnetic ordering temperature of T_N=5.0 K. Remarkably, in 20 Oe applied field both superconductivity (T_c=8.0 K) and antiferromagnetism (T_N=5.0 K) clearly make themselves manifest in the magnetization data. From these magnetization data a phase diagram in the H−T plane was constructed for both directions of applied field. This phase diagram shows a non-monotonic temperature dependence of H_c2 with a deep minimum at T_N=5 K. The high-field magnetization data for H applied perpendicular to the c-axis also reveal a cascade of three phase transitions for T < 5 K and H < 15 000 Oe, contributing to the rich H versus T phase diagram for HoNi₂B₂C at low temperatures.     

The effect of oxygen vacancy on the oxide ion mobility in LaAlO3-based oxides

The electrical property of (La_1−xSr_x)_1−z(Al_1−yMg_y)O_3−δ (LSAM; x≤0.3, y≤0.15 and z≤0.1) was measured using the DC four-probe method as a function of temperature (500–1000°C) and oxygen partial pressure (1–10⁻²² atm). Among LSAMs, (La_0.9Sr_0.1)AlO_3−δ showed the highest ionic conductivity, σ_i=1.3×10⁻² S cm⁻¹ at 900°C. A simultaneous substitution at A and B sites or A site deficiency is expected to create larger oxygen vacancy and higher ionic conductivity. However, it showed a negative effect. The effect of the vacancy increase did not effect monotonously the ionic conductivity. It was found that the concentration of oxygen vacancy, [V_O], influences not only the oxide ion conductivity, σ_i, but also the mobility, μ_v, of [V_O]. These properties exhibit a maximum at around [V_O]=0.05. With the increase in [V_O], the activation energy, E_a, of the ionic conduction dropped from 1.8 to ca. 1.0 eV at [V_O]=0.05 and became almost constant at [V_O]>0.05. The dependency of the pre-exponential term, μ⁰_v, and E_a on [V_O] was analyzed and their effect on μ_v and σ_i was discussed with respect to crystal structure and defect association. It was estimated that the crystal structure mainly governs these properties. The effect of defect association could not be ignored but is considered to be a complicated correlation.     

Tuning the multiferroic properties of Pb(Fe1/2Nb1/2)O3 by cationic substitution

A series of substituted lead iron niobate compounds with the general formula Pb²⁺_(1−x)A^Z_x(Fe_{{(1−(2−Z)x)/2}}Nb_{{(1+(2−Z)x)/2}})O₃ (0<x<0.6 and A=La³⁺, K⁺ or Sr²⁺) were prepared by a modified solid-state synthesis. The relative concentrations of Fe³⁺ and Nb⁵⁺ were adjusted to compensate the charge imbalance due to the aliovalent substitution. The dielectric constant and magnetic susceptibilities were studied as a function of temperature. The temperature of the dielectric maximum, T_M, of the substituted compounds decreased linearly with increasing concentration of the substituent ions. The magnetic measurements showed an antiferromagnetic transition at temperatures T_N1 due to the superexchange interactions mediated by Fe–O–Fe and an additional antiferromagnetic-type transition at T_N2. T_N1 linearly increased with the increasing concentration of Fe³⁺ ion at the B-site of ABO₃-type substituted compounds. T_M is shown to be directly dependent on the concentration of the ferroactive Nb⁵⁺ ions at the B-site and Pb²⁺ ions at the A-site.     

Aspects of “low field” magnetotransport in epitaxial thin films of the ferromagnetic metallic oxide SrRuO3

Epitaxial thin films of the conductive ferromagnetic oxide SrRuO₃ were grown on an (0 0 1) SrTiO₃ (STO) substrate by using DC sputtering technique. The magnetic and magnetoresistive properties of the films were measured by applying the magnetic field both perpendicular (out-of-plane) and parallel (in-plane) to the film plane and ever maintaining the direction of the applied field perpendicular to that of the transport current. The films grown on an (0 0 1) STO substrate showed identical magnetization properties in two orthogonal crystallographic directions of the substrate, [1 0 0]_S and [0 0 1]_S (in-plane and out-of-plane geometry), which suggests the presence of a multi domain structure within the plane of the film. For such samples, no anisotropic field (hard axis) along de [0 0 1]s direction, i.e., perpendicular to the film-plane could be detected. Nevertheless, a distinguishable temperature dependent out-of-plane anisotropic magnetoresistance (MR) along with strong temperature dependent low field hysteretic MR(H) behavior was detected for the studied films. A negative MR ratio MR(T)=[ρ(μ₀H=9 T; T)−ρ( μ₀H=0 T; T)]/ρ( μ₀H=0 T; T) on the order of a few percent, with maximums of 6% and 4% (right at the Curie temperature, T_C 160 K) was calculated for an in-plane and out-of plane measuring geometry, respectively. In addition there is an equally strong MR effect at low temperatures, which might be related to the temperature dependence of the magnetocrystalline anisotropy together with a magnetization rotation. Both the MR(T) behavior and the achieved values (except for T<30 K) are similar to those obtained on SrRuO₃ films grown on 2° miscut (0 0 1) STO substrates with the current parallel to the field and parallel to the direction, which was identified as the easier axis for magnetization.     

Systematic thermopower measurements of the thallium cuprates Tl(Ba,Sr)2Cam−1CumO2m+3−δ and Tl2Ba2Cam−1CumO2m+4+δ

The thermoelectric power (TEP) S versus temperature has been systematically investigated for several series of the superconducting cuprates Tl(Ba,Sr)₂Ca_m−1Cu_mO_2m+3−δ (m = 2, 3) and Tl₂Ba₂Ca_m−1Cu_mO_2m+4+δ (m = 1, 2, 3). The consideration of the S(T_c) curves allows two important points to be found evidence for. The first one deals with the fact that all these superconducting thallium cuprates are systematically overdoped whatever T_c, and whatever the number of Cu or Tl layers; no underdoped superconducting cuprate could be obtained. The second point shows that there exist two classes of Tl cuprates: the weakly overdoped cuprates that exhibit a T_{c max} ≥ 100 K (all the triple copper layer cuprates and the 2212 cuprates) and those which can be heavily doped that exhibit a T_{c max} ≤ 90 K (the 2201 and the 1212 cuprates). The different behavior of thallium cuprates compared to YBa₂Cu₃O_7−δ and to bismuth cuprates is discussed.     

Dielectric and magnetic properties of xNiFe2O4+(1−x)Ba0.9Sr0.1TiO3 composites

Magnetoelectric composites, namely, xNiFe₂O₄+(1−x)Ba_0.9Sr_0.1TiO₃ were prepared by standard double sintering ceramic method. The X-ray diffraction analysis was carried out to check the phases formed during sintering and to calculate the lattice parameters. Scanning electron microscope (SEM) micrographs were taken to understand the microstructure of the samples. The dielectric constant (ε′) and loss tangent (tan δ) were measured as a function of frequency in the frequency range 100 Hz–1 MHz. Variation of dielectric constant and loss tangent with temperature and composition has been reported. The hysteresis measurements were done to determine saturation magnetization (M_S) and coersivity (H_c). The variation of saturation magnetization and magnetic moment is interpreted in terms of composition.     

Electron paramagnetic resonance measurements for (La,Y)2/3(Ca,Ba)1/3MnO3

We have measured the paramagnetic (PM) resonance behavior as a function of temperature for various manganese perovskites (La,Y)_2/3(Ca,Ba)_1/3MnO₃ with an average A-site size r_A basically covering the whole region of ferromagnetic (FM) metallic ground state. We show that at least three regions with different magnetic behaviors can be distinguished by two phase lines: T_onset−r_A and T_c−r_A. For each given r_A, the complete PM and long-range FM behaviors appear above T_onset and below T_c, respectively; while some anomalous PM behaviors appear for the intermediate temperature range of T_onset<T<T_c . A possible magnetic transition process is discussed in order of decreasing temperature from high-T complete paramagnetism to low-T long-range ferromagnetism.     

Dielectric and modulus behavior of LiFe1/2Ni1/2VO4 ceramics

The polycrystalline sample of LiFe_1/2Ni_1/2VO₄ was prepared by a standard solid-state reaction technique and confirmed by X-ray diffractometry. LiFe_1/2Ni_1/2VO₄ has orthorhombic crystal structure whose dielectric and electric modulus properties were studied over a wide frequency range (100 Hz–1 MHz) at different temperatures (296–623 K) using a complex impedance spectroscopy (CIS) technique. The frequency and temperature dependence of dielectric constant (ε_r) and tangent loss (tan δ) of LiFe_1/2Ni_1/2VO₄ are studied. The variation of ε_r as a function frequency at different temperatures exhibits a dispersive behavior at low frequencies. The variation of the ε_r as a function of temperature at different frequencies shows the dielectric anomaly in ε_r at 498 K with maximum value of dielectric constant 274.49 and 96.86 at 100 kHz and 1 MHz, respectively. Modulus analysis was carried out to understand the mechanism of the electrical transport process, which indicates the non-exponential type of conductivity relaxation in the material. The activation energy calculated from electric modulus spectra is 0.38 eV.     

Effects of crystallographic ordering on the magnetic behaviour of (AgIn)1-zMn2zTe2 and (CuIn)1-zMn2zTe2 alloys

Measurements of magnetic susceptibility in the temperature range 4.2–300 K were made on polycrystalline samples of the (AgIn)_{1 - z}Mn_2zTe₂ and (CuIn)_{1 - z}Mn_2zTe₂ alloys, and the data used to give values of spin-glass transition te mperature T_g and Curie-Weiss paramagnetic temperature θ. For any sample for which the X-ray powder photograph indicated an apparently single phase condition, either zinc-blende or chalcopyrite, the susceptibility data could show up to three separate T_g values. These different magnetic conditions are attributed to crystallographic ordering of the Mn ions on the chalcopyrite and zinc-blende lattices, the three observed T_g values corresponding to disordered zinc-blende, ordered zinc-blende and ordered chalcopyrite. The value of θ obtained from the 1/χ vs. T plot is shown to be a weighted mean of the separate values of θ for the phases present. The relative sizes of the T_g peaks and the values of θ for any given sample gives an indication of the amount of each phase present. These amounts were varied by using different methods of heat treatment and it was shown that the magnetic behaviour was consistent with the T(z) phase diagram for the two alloy systems.     

Influence of the Tl- and Hg-content on magnetic and transport properties of the Pb, Sr-doped Tl-1223 and Hg-1223 superconductors

The effects of the thallium and mercury content x on the as-sintered and post annealed samples of M_xPb_0.4Sr_1.6Ba_0.4Ca₂Cu₃O_8+δ {M: Tl (0.32≤x≤0.74) or Hg (0.18≤x≤0.68)} have been studied by magnetization and transport measurements. For Tl-1223 we have found the optimum Tl doping level to be x=0.53 regarding the grain properties, the content of superconducting phase, the first penetration field H_pl^wl, the transport (J_c^tr), magnetic intergrain (J_c^M) and intragrain (J_c^g) critical current densities. The critical temperature T_c of the as-sintered Tl-1223 sample decreased with increasing Tl content. Post-annealing in oxygen improved the T_c for Tl contents of x≥0.53 and had generally positive effects on the critical current densities. The intergrain properties of the Hg-1223 samples were much worse than those of the Tl-based superconductors.