Phonon Raman scattering in Nd1+xBa2−xCu3O7−δ and Pr1+xBa2−xCu3O7−δ single crystals

The polarized Raman spectra of Nd_1+xBa_2−xCu₃O_7−δ (−0.023≤x≤0.107) and Pr_1+xBa_2−xCu₃O_7−δ (0.01≤x≤0.15) single crystals have been investigated. It was found that the Cu(2) A_g mode softens by 6 cm⁻¹ in Nd 1:2:3 and 4 cm⁻¹ in Pr 1:2:3 as x increases. These frequency shifts cannot be explained by the change in the relevant bond lengths due to Nd(Pr)-substitution for Ba. The variations with x of the two low frequency modes may be affected by change of their hybridization and/or change of their force constants. The linewidths of Ba mode in Pr 1:2:3 are broader than those in Y 1:2:3. This result suggests that the Pr substitution on Ba sites occurred even in a very small value of x. In x(yy) geometry the relative intensity of the Ba and O(4) modes in Nd 1:2:3 is greater than those in Pr 1:2:3. The difference between Nd 1:2:3 and Pr 1:2:3 in the relative intensity of the Ba and O(4) modes may be produced by the chains.     

Ramans study of Y1−xPrxBa2Cu3O7−δ and YB2Cu3−xZnxO7−δ single crystals

Single crystals with known T_c values of Y_1−xPr_xBa₂Cu₃O_7−δ (Y---Pr1:2:3) and YBa₂Cu_3−xZn_3−xZn_xO_7−δ (Y---Zn1:2:3) systems are studied by Raman measurements. The Raman spectra for (Y---Pr1:2:3) single crystals show that the frequencies of Ba and O_z modes increase as the Pr content increases. The results are consistent with the hole-localization scheme proposed for the suppression of superconductivity in the polycrystalline Y---Pr1:2:3 systems. On the other hand, in the Y---Zn1:2:3 system, all the Raman modes do not change in frequencies. However, the FWHM of the Cu(2) mode increases with the decrease of T_c, indicating strong scattering of charge carriers by the substituted Zn ions in the CuO₂ planes. The induced disorder in the CuO₂ planes may be related with suppression of T_c in the Y---Zn1:2:3 system. Thus, the suppression mechanism in the Y---Zn1:2:3 systems seems to be different from that in the Y---Pr1:2:3 systems.     

Transient creep of YBa2Cu3O7−x superconductor

Rapid changes of oxygen partial pressure (P_O2) between 10³ and 2.1×10⁴ Pa have been carried out during steady-state plastic deformation of polycrystalline YBa₂Cu₃O_7−x (YBCO) at temperatures between 825 and 900°C. Transient creep was observed after such P_O2 changes. The analysis of these creep transients allowed the determination of the chemical diffusion coefficient for reequilibration, which is identical to that found from thermogravimetry and electrical conductivity experiments for oxygen vacancies.     

AC and DC magnetic studies of critical currents in ceramics of the Ho1−xPrxBa2Cu3O7−δ system

AC magnetic susceptibility measurements were performed for ceramics of the Ho_1−xPr_xBa₂Cu₃O_7−δ system as a function of temperature, frequency, field amplitude and static magnetic field. From the measurements, temperature dependences of intergranular critical currents and corresponding pinning energies at grain boundaries were determined for different Pr concentrations. These critical currents strongly decrease with Pr doping. They are limited by superconductor–insulator–superconductor or superconductor–normal metal–superconductor junctions and for higher Pr concentrations additionally suppressed by flux creep. Also intragranular critical current at 4.3 K was determined as a function of Pr concentration from magnetic hysteresis loops. It is a monotonically decreasing function of Pr doping.     

A study on the structural–microstructural characterisation and defect structure of Ru based magnetosuperconductor, RuSr2Eu1.6Ce0.4Cu2O10−δ

The structural–microstructural characterization and defect structure of Ru based magnetosuperconductor RuSr₂Eu_1.6Ce_0.4Cu₂O_10−δ has been investigated by selected area electron diffraction pattern and high resolution electron microscopy. Under the present investigations, RuSr₂Eu_1.6Ce_0.4Cu₂O_10−δ magnetosuperconductor shows the presence of both Ru-1222 and Ru-1212 phases. Analysis of the selected area electron diffraction pattern indicates superstructure in Ru-1212 while Ru-1222 phase does not show the presence of superlattice structure. A careful and detailed investigations of the HRTEM image shows the presence of defects like 90° domains, intergrowths, and dislocations.     

Crystal growth of superconductive PrBa2Cu3O7−y

Superconductive PrBa₂Cu₃O_7−y (Pr123) crystals have been grown successfully by the travelling-solvent floating-zone (TSFZ) method using 3.7–5.8% PrO, 27–37% BaO, and 60–69% CuO composition solution with the 0.1–0.4% oxygen mixed argon gas atmosphere. The grown crystals have been identified to be Pr123 by a precession camera, X-ray powder diffractions and scanning electron microscopy–X-ray energy dispersion spectroscopy (SEM-EDS). Some portion of the grown TSFZ crystal boules show bulk superconductivity below about 80 K after annealing in oxygen.     

Field induced flux pinning in Nd1+xBa2−xCu3O7−δ single crystal

The flux pinning behavior of a Nd_1+xBa_2−xCu₃O_7−δ (Nd123) single crystal, which exhibited a peak effect, has been studied by monitoring the time decay of the magnetic moment. The apparent pinning energy (U₀^*) was deduced from flux creep data on the basis of the Anderson-Kim model. The magnetic field dependence of U₀^* showed maxima at peak fields which depended on the temperatures, in a similar manner to those of critical current densities. In addition, the temperature dependence of U₀^* showed several features. To explain the increase in U₀^* with the field as well as its temperature and field dependence, we made a numerical calculation by introducing an additional pinning energy which increased with increasing field. The results are in good agreement with the experimental data, especially at temperatures above 60 K, where the contribution of field induced pinning centers is believed to be dominant.     

Nax/2Bi1−x/2MoxV1−xO4 and Bi1−x/3MoxV1−xO4 New Scheelite-related phases

New Scheelite-related solid solutions of the compositions Na_x/2Bi_1−x/2Mo_xV_1−xO₄ (0≤x≤1) and Bi_1−x/3 Mo_xV_1−xO₄(0≤x≤0.2) have been synthesised by the substitution of Na and Mo at the A and B sites respectively of the ABO₄ type ferroelastic BiVO₄. The phases were characterised using chemical analysis, powder X-ray diffraction, scanning electron microscopy, EDAX, and Raman spectroscopy. While almost a continuous solid solution is obtained for the series Na_x/2Bi_1−x/2Mo_xV_1−xO₄, the absence of Na at the A-site results only in a narrow stability region for the other series, Bi_1−x/3 Mo_xV_1−xO₄ where 0≤x≤0.2. Raman spectra of selected samples at room temperature also suggest that vanadium and molybdenum atoms are disordered at the tetrahedral sites.     

Electrical and structural properties of epitaxially grown Y1Ba2Cu3O7 − x and Y2Ba4Cu8O16 − x thin films using the BaF2 method

Thin films of Cu, Y and BaF₂ are co-condensed in ultrahigh vacuum onto SrTiO₃ (1 0 0)-substrates at room temperature without any additional oxygen supply. It is found that the temperature of the ex situ fluorine-oxygen exchange reaction in flowing wet oxygen essentially determines whether the Y₁Ba₂Cu₃O_{7 − x}-phase (T_ex = 850°C) or the Y₂Ba₄Cu₈O_{16 − x}-phase (T_ex = 800°C) forms or any mixture of both phases in between. Small-angle X-ray diffraction verifies the strictly epitaxial growth of the superconducting phases. The variation of the composition around the ideal 1,2,3-stoichiometry affects only the superconducting and normal conducting properties which are measured using the four-probe Montgomery method. The values of the normal state resistivity and its temperature dependence are discussed in combination with a reduced cross section of the conduction paths in the films.     

Oxygen nonstoichiometry and phase transitions of the neodymium-rich Nd1+xBa2−xCu3Oz solid solution

On the basis of chemical, thermal analysis and Cu K-edge X-ray absorption measurements, oxygen content in the Nd_1+xBa_2−xCu₃O_z solid solution was determined between 1000°C in air and 400°C in oxygen for x=0.05–0.9 compositions. It has been observed that the oxygen nonstoichiometry Δz of the Nd_1+xBa_2−xCu₃O_7+x/2−Δz solid solution decreases 2–2.5 times for a large substitution (Δz≈0.3–0.33 for x=0.9), despite of the acclaimed higher total oxygen content. The difference in nonstoichiometry is explained by a higher average value of the copper oxidation state (ACV), which is vital for the solid solution with large x even at elevated temperatures (ACV≈2–2.05 for x>0.3 at 1000°C, PO₂=0.21 atm). On the contrary, the ACV after complete oxygenation is almost constant (about 2.25–2.3) for the whole series. The x-dependence of the oxygen content is not monotonous and structural phase transitions can be observed at x=0.3 and x=0.6, as confirmed by the X-ray diffraction and the Raman scattering spectroscopy. The first well-known transition is connected with the oxygen disorder due to the Nd substitution for Ba at random Ba-sites. In the present work, it is proved by the apical oxygen mode broadening in Raman spectra. Ordering of the Nd and Ba atoms with a subsequent orthorhombic distortion of the lattice may occur even at 1000°C in air due to the second transformation at x≈0.6. The invariable orthorhombicity of the Nd-rich solid solution with x>0.6 is not caused by the oxygen absorption as in the x=0.05 case. Existence of high- and low-temperature orthorhombic modifications of this solid solution has been observed for the first time. Finally, a tentative 3D (z–x–T) diagram is suggested for the Nd_1+xBa_2−xCu₃O_z solid solution up to 1000°C in air, including the new x=0.6–0.9 region.     

Synthesis and investigation of the complex copper oxides Bi2Sr2R2−xCexCu2O10+δ (R=rare earth)

Bi-2222 phases were prepared by solid state reactions and were studied using X-ray diffraction, chemical and EDS-analysis. Compounds with composition Bi₂Sr₂R_1.33Ce_0.67Cu₂O_10+δ were obtained for R=Pr, Nd, Sm-Er. The phases Bi₂Sr₂Cu₂O_10+δ with similar structure but without Ce were prepared for R = Pr, Sm-Dy. For Bi₂Sr₂Eu_2−xCe_xCu₂O_10+δ the solubility limit was determined and the effect of treatment under different oxygen pressures was investigated. Weak diamagnetic signals (<3%) were detected for some of these samples.     

Hole density and Tc behaviour in YBa2Cu3O7 − x

The behaviour of the hole number in YBCO systems as a function of the oxygen deficiency x is studied theoretically by calculating the density of electron states for several different superstructures formed by periodic arrangements of the oxygen vacancies. The characteristic features of the electronic properties for chain copper sites with different coordination are pointed out and their relevance in determining the number of carriers for oxygen planes is illustrated. It is shown that the curve of the hole number as a function of x shows plateaus and jumps similar to those found in the T_c versus x curves if the de-oxygenation process takes place by forming fragmented chains. Structures formed by filled and empty chains only give a smooth hole behaviour as a function of the composition. The results of the numerical calculations can be understood by a simple model giving the Fermi energy shift in terms of the concentrations of Cu(1) sites with different coordination.     

Properties of YBa2Cu3O7−δ/YBa2CoxCu3−xOy/YBa2Cu3O7−δ Josephson edge junctions with 0.1 x 0.3 and the effect of flux flow on their normal resistance

YBa₂Cu₃O_7−δ (YBCO) based SNS edge junctions with cobalt doped YBCO barriers were prepared and characterized. At 77 K, good junctions had RSJ-like I–V curves with excess current, magnetic suppression of I_c of about 50% or more, and clear microwave steps. The conductance values 1/R_N at 77 K of junctions with different barrier thickness and composition, were proportional to the junction areas A, but show little correlation with the thickness of the barriers t_B in the range of 15t_B100nm. The corresponding I_cR_N products were observed to scale as J^0.66±0.09_c, similar to what was found by others. At the same time, the measured values of R_N are much smaller than what is expected based on the dimensions of the junction and the resistivity of the barrier material. To explain all of this, we propose a model in which at high supercurrent densities, flux flow of Josephson vortices in the junction leads to R_N values which are lower than expected. This model predicts

Full-size image (1K)

, which fits the observed results very well.     

Structural characteristics and morphology of SmxCe1−xO2−x/2 thin films

Effect of the deposition temperature (200 and 500 °C) and composition of Sm_xCe_1−xO_2−x/2 (x = 0, 10.9–15.9 mol%) thin films prepared by electron beam physical vapor deposition (EB-PVD) and Ar⁺ ion beam assisted deposition (IBAD) combined with EB-PVD on structural characteristics and morphology/microstructure was investigated. The X-ray photoelectron spectroscopy (XPS) of the surface and electron probe microanalysis (EPMA) of the bulk of the film revealed the dominant occurrence of Ce⁴⁺ oxidation state, suggesting the presence of CeO₂ phase, which was confirmed by X-ray diffraction (XRD). The Ce³⁺ oxidation states corresponding to Ce₂O₃ phase were in minority. The XRD and scanning electron microscopy (SEM) showed the polycrystalline columnar structure and a rooftop morphology of the surface. Effects of the preparation conditions (temperature, composition, IBAD) on the lattice parameter, grain size, perfection of the columnar growth and its impact on the surface morphology are analyzed and discussed.     

Vortex core physics in the cuprate superconductor Nd2−xCexCuOy

Flux-flow voltage steps and negative differential resistivity in the cuprate Nd_2−xCe_xCuO_y are explained in terms of subbands between the Fermi energy and the energy gap affecting the quasiparticle dynamics.     

Neutron diffraction study of the U(Pd1−xFex)2Ge2 magnetic structure

The neutron diffraction and magnetic susceptibility studies have shown that the magnetic structure of UPd₂Ge₂ changes dramatically even under very low iron doping. Though the general magnetic structure of pure UPd₂Ge₂ and of 1%Fe-doped samples is the same, the temperature intervals of existence of different magnetic phases are different. The values of transition temperatures, where (i) the ‘square’ modulated longitudinal spin-density wave (LSDW) structure with the propagation vector k=(0; 0; ) starts to transform into the sinusoidal modulated LSDW structure and (ii) the commensurate phase transforms into incommensurate one, shift under the 1%Fe doping to the higher temperatures (from 50 to 65 K and from 80 to 90 K, respectively). In the pure and 1%Fe-doped UPd₂Ge₂, the magnetic transition from the commensurate to incommensurate phase is accompanied by the drastic decrease of the propagation vector k_z. In the 2%Fe-doped sample, besides the Néel point of T_N=135 K, we have found two additional characteristic temperatures of 65 and 93 K. Below 65 K, the material has a simple antiferromagnetic (AF) structure with the propagation vector k=(0; 0; 1) and, at 65 K<T<T_N, the magnetic structure is LSDW with sinusoidal modulation. Over almost the total region 65 K<T<T_N, the LSDW magnetic structure is incommensurate. Only at about 93 K, the propagation vector passes the commensurate value of , whereas at 65<T<93 K and at 93 K<T<T_N. We have found that the magnetic susceptibility and the uranium magnetic moment are sensitive to the transition. With increasing iron concentration to x0.15, the simple AF structure with k=(0; 0; 1) develops over all temperature region up to the Néel point. Below T_N, the uranium magnetic moments are always parallel to the tetragonal c-axis.     

Magnetic polarons in Ca1−xYxMnO3

Experimental evidence shows that in the magnetoresistive manganite Ca_1−xY_xMnO₃, ferromagnetic (FM) polarons arises in an antiferromagnetic (AF) background, as a result of the doping with yttrium. This hypothesis is supported in this work by classical Monte Carlo calculations performed on a model where FM double exchange and AF superexchange compete.     

Unusual resistivity broadening in the mixed state of NdBa2Cu3O7−δ crystals grown by a crystal-pulling technique

In order to clarify the origin of a strong peak effect in the magnetization curve of NdBa₂Cu₃O_7−δ crystals, we investigated the superconductivity transition behavior of the in-plane resistivity in static magnetic fields up to 8 T. Comparing the results for the samples exhibiting and not exhibiting the peak effect, we found that the former (peak effect sample) shows lower resistivity above the vortex melting temperature. This implies that the pinning force is effective in the vortex liquid state. We also found that the normal state resistivity behaviors of some samples were unusual, indicating inhomogeneous current flow. These results suggest an existence of sheet-like pinning centers perpendicular to the conduction planes.     

Magnetic doping in Zn7−xMxSb2O12 spinels (M=Ni and Co)

In this article we present a concise report on our studies on the magnetic behavior and structural arrangements of the inverse spinel Zn_7−xM_xSb₂O₁₂ system (M=Ni, Co). Studies on the temperature dependence of the magnetization (M) of several samples in this system showed the occurrence of a spin-glass-like state in temperatures around 10 K. The capability of this system to hold magnetic ions in either octahedral and/or tetrahedral positions is responsible for the occurrence of competing ferromagnetic and antiferromagnetic interactions. This condition is likely to cause the appearance of the observed spin-glass-like behavior.     

Tunneling studies on NdBa2Cu3O7−y

Tunneling measurements were performed at 4.2 K on well-characterized NdBa₂Cu₃O_7−y samples using a sandwich configuration with an artificially grown barrier layer (sputtered indium oxide) and Pb_0.5In_0.5 counter electrode. The conductance spectra exhibited well-defined structures characteristic of gap opening. Fitting the data to a life-time broadened BCS density of states function yielded the following values: 20 meV for the energy gap Δ, 1.5 meV for the line width Γ and 5.3 for 2Δ/k_BT_c.