Inelastic magnetic X-ray scattering from highly correlated electron systems: La1.2Sr1.8Mn2O7, La0.7Sr0.3MnO3 and Fe3O4

Magnetic Compton profiles have been measured for the colossal magnetoresistance manganites La_1.2Sr_1.8Mn₂O₇ and La_0.7Sr_0.3MnO₃, and for magnetite Fe₃O₄, along various crystallographic directions, over a wide range of temperatures and magnetic fields. The experimental results are interpreted via first-principles computations for the double layer manganite, La_1.2Sr_1.8Mn₂O₇, and by using a simple model involving atomic d-orbitals and free electrons for the other two compounds. For all three materials a preference for the occupation of e_g orbitals is found, particularly, for orbitals of dx²−y² symmetry. An itinerant electron contribution is adduced at all temperatures in magnetite; such a contribution also appears in La_1.2Sr_1.8Mn₂O₇, but it is present only at low temperatures in La_0.7Sr_0.3MnO₃.     

Intrinsic inhomogeneity and non-linear conduction in charge-ordered Bi0.5Ca0.4Sr0.1MnO3

Systematic studies of X-ray, magnetic, electronic transport, and elastic properties have been performed on polycrystalline Bi_0.5Ca_0.4Sr_0.1MnO₃ sample. The sample exhibits charge ordering (CO) state below T_CO (=304 K), accompanied by a distinct maximum in magnetization. The softening of Young's modulus in the vicinity of T_CO indicates that there is a strong coupling of electron-phonon due to Jahn-Teller (JT) effect. The dynamic ferromagnetic spin correlations are observed at high temperatures above T_CO, which are replaced by antiferromagnetic (AFM) spin fluctuations at a concomitant CO transition. Below 32 K, a spin-glass (SG) state dominates at low temperatures. The voltage-current (V-I) characteristics measurement results indicate that the non-linear conduction starts above a threshold current, giving rise to a region of negative differential resistance (NDR). The origin of the non-linear conduction is discussed in view of current induced collapse of CO state associated with phase-separation mechanism.     

Magnetoresistive properties of Zn1−xCoxFe2O4 ferrites

The magnetic and magnetoresistive properties of spinel-type Zn_1−xCo_xFe₂O₄ (x=0, 0.2 and 0.4) ferrites are extensively investigated in this study. A large negative magnetoresistance (MR) effect is observed in Zn_1−xCo_xFe₂O₄ ferrites of spinel structure. These materials are either ferrimagnetic or paramagnetic at room temperature, and show a spin-(cluster) glass transition at low temperatures, depending on the chemical compositions. The MR curves as a function of magnetic fields, MR(H), are parabolic at all temperatures for paramagnetic polycrystalline ZnFe₂O₄. The MR for ZnFe₂O₄ at 110 K in the presence of 9 T applied magnetic field is 30%. On the other hand, MR(H) are linear for x=0.2 and 0.4 ferrimagnetic Zn_1−xCo_xFe₂O₄ samples up to 9 T. The MR effect is independent of the sintering temperatures, and can be explained with the help of the spin-dependent scattering and the Yafet–Kittel angle of Zn_1−xCo_xFe₂O₄ mixed ferrites.     

Sound velocity in La0.5Ca0.5MnO3

In this Letter the microscopic theory of the relative change in velocity of sound with temperature of La_0.5Ca_0.5MnO₃ is reported. The phonon Green function is calculated using the Green function technique of Zubarev in the limit of zero wave vector and low temperature. The lattice model electronic Hamiltonian in the presence of the phonon interaction with hybridization between the conduction electrons and the l-electrons is used. The relative change in velocity of sound at various temperatures is studied for different model parameters namely the position of the l-level, the effective phonon coupling strength and hybridization strength. The phonon anomalies observed experimentally at different temperatures are explained theoretically. An abrupt change in velocity at Neel temperature (TN) is observed clearly. It is observed that different parameters influence the velocity of sound.     

Electric and magnetic properties of the system between Cr3S4 and VCr2S4

The electrical resistivity and magnetization of V_xCr_3?xS₄ (x = 0.0 - 1.0) have been measured. Weak ferromagnetic moments are observed at low temperatures for x ≠ 0.0. Curie temperatures are determined from magnetization curves and resistivity anomalies.     

Ferromagnetism and spin reorientation in Sm12Fe14Al5

The single crystal of the new ternary compound Sm₁₂Fe₁₄Al₅ was grown and its crystallographic and magnetic properties were investigated. Sm₁₂Fe₁₄Al₅ has a hexagonal structure of the space group p-3m1 and shows ferromagnetism with a Curie temperature of 245 K. The easy direction of magnetization is parallel to the c-axis at temperatures between 245 and 85 K; however, it changes to the c-plane below 85 K through a first-order-like phase transition. No saturation is observed in the magnetization curve even under the applied field of 55 kOe at 5 K. Sm₁₂Fe₁₄Al₅ seems to have a large coercive field at very low temperatures. The anisotropy field was estimated at 5 and 120 K and the saturation magnetization of low temperature phase is explained assuming a ferromagnetic coupling between Fe and Sm sublattices.     

Effect of annealing temperature on the optical and electrical properties of amorphous As45.2Te46.6In8.2 thin films

The optical absorption of the As-prepared and annealed As_45.2Te_46.6In_8.2 thin films are studied. Films annealed at temperatures higher than 453 K show a decrease in the optical energy gap (E_o). The value of E_o increases from 1.9 to 2.43 eV with increasing thickness of the As-prepared films from 60 to 140 nm. The effect of thickness on high frequency dielectric constant (?_∞) and carrier concentration (N) is also studied. The crystalline structures of the As_45.2Te_46.6In_8.2 thin films resulting from heat treatment of the As-prepared film at different elevated temperatures is studied by X-ray diffraction. An amorphous-crystalline transformation is observed after annealing at temperatures higher than 453 K. The electrical conductivity at low temperatures is found due to the electrons transport by hopping among the localized states near the Fermi level. With annealing the films at temperatures higher than 473 K (the crystallization onset temperature) for 1 h, the electrical conductivity increases and the activation energy decreases, which can be attributed to the amorphous-crystalline transformations.     

Influence of Dy addition on the magnetocaloric effect of La0.67Ca0.33Mn0.9V0.1O3 ceramics

The influence of partial substitution of La by Dy on the magnetocaloric response of (La_1−xDy_x)_0.67Ca_0.33Mn_0.9V_0.1O₃, where x=0.03, 0.15 and 0.25 is studied. Rietveld refinement of X-ray diffraction pattern using GSAS method shows that the compounds adopt the orthorhombic structure with Pnma space group. The systematic change in lattice parameters and magnetic phase transition indicates the substitution effect of Dy. From the magnetization isotherms at different temperatures, magnetic entropy change close to their respective transition temperatures (T_C) has been evaluated. The maximum value of entropy change near T_C is found to be about 4.8 J/kg K at 187.5 K for LCMVDy_0.03, 2.45 J/kg K at 107.5 K for LCMVDy_0.15 and 2.15 J/kg K at 92.5 K for LCMVDy_0.25 at 4 T. Dy addition produces a reduction in T_C and in magnitude of the magnetic entropy change. Even though the entropy change decreases with increasing Dy substitution the refrigerant temperature range, ΔT, is found to be 10 K for LCMVDy_0.03, 31 K for LCMVDy_0.15 and 35 K for LCMVDy_0.25 compounds [90%] at 4 T. The field dependence of the magnetic entropy change is also analyzed showing the power law dependence, ΔS_M∞Hⁿ where n=0.75(2) for LCMVDy_0.03, n=0.80(4) for LCMVDy_0.15 and n=0.92(8) for LCMVDy_0.25 compounds at their respective transition temperatures. The relative cooling power and its field dependance are also analyzed.     

Hyperfine interactions in some Aurivillius Bim+1Ti3Fem−3O3m+3 compounds

X-ray diffraction and Mössbauer spectroscopy were applied as complementary methods to investigate the structure and hyperfine interactions in the series of Bi_m+1Ti₃Fe_m−3O_3m+3 Aurivillius compounds with m=4, 6, 7 and 8. Samples were synthesized by the solid-state sintering method at various temperatures. As X-ray diffraction analysis proved, the compounds formed single phases at temperature above 993 K. Mössbauer studies have confirmed diffraction measurements. Compounds synthesized at 993 K contained residual hematite, however these sintered at elevated temperatures were single-phased materials. Room-temperature Mössbauer spectra of Bi_m+1Ti₃Fe_m−3O_3m+3 compounds revealed their paramagnetic properties, what is consistent with the literature data concerning the Néel temperature of these ceramics (T_N is smaller than room temperature). Detailed analysis of MS spectra allowed to state that iron ions may occupy both tetrahedral and octahedral sites in the crystallographic lattice of Aurivillius compounds.     

High-throughput characterization of local conductivity of Nd0.9Ca0.1Ba2Cu3O7−δ thin film by the low-temperature scanning microwave microscope

We developed a scanning microwave microscope (SμM) designed for high-throughput electric-property screening as well as for rapid construction of electronic phase diagrams at low temperatures. As a sensor probe, we used a high-Qλ/4 coaxial cavity resonator to which a thin needle with ball-tip end was attached. The sensor module was mounted on the low-temperature XYZ stage, which allowed us to map out the change of resonance frequency and quality factor due to the local tip-sample interaction at low temperatures. From the measurements of combinatorial thin films, such as Ti_1−xCo_xO_2−δ and Nd_0.9Ca_0.1Ba₂Cu₃O_7−δ (NCBCO), it was demonstrated that this SμM system has enough performance for the high-throughput characterization of sample conductance under variable temperature conditions.     

Spin glass ordering of Zn0.75Co0.25Fe0.5Cr1.5O4 cubic spinel

The linear and nonlinear low field AC susceptibilities of Zn_0.75Co_0.25Fe_0.5Cr_1.5O₄ show peaks due to non-critical contributions, which mask the peak due to spin glass ordering. They extend into the region of temperatures in which Mössbauer spectra do not show any magnetic component. When a DC field of 200 Oe suppresses the non-critical contributions, peak due to spin glass ordering is clearly visible. The spin glass ordering is thus shown to be a thermodynamic transition. The critical exponent is found to fall within the range found using other spin glasses. Mössbauer spectra in zero fields provide T_SG, which agrees with the peak temperature of AC susceptibilities in the absence of non-critical contributions. 〈S_Z〉 determined using Mössbauer spectra does not show any anomaly. In the presence of a field of 5 T, the spectra show SG ordering at 4.2 K, which converts into ferrimagnetic ordering at higher temperatures.     

Electron-phonon coupling and longitudinal sound velocity of La0.5Ca0.5MnO3

In this paper, the microscopic theory of the relative change in velocity of sound with temperature of La_0.5Ca_0.5MnO₃ is reported. The phonon Green function is calculated using the Green function technique of Zubarev in the limit of zero wave vector and low temperature. The lattice model electronic Hamiltonian in the presence of the phonon interaction with hybridization between the conduction electrons and the l-electrons is used. The relative change in velocity of sound at various temperatures is studied for different model parameters, namely the position of the l-level, the effective phonon coupling strength and hybridization strength. The phonon anomalies observed experimentally at different temperatures are explained theoretically. An abrupt change in velocity at Neel temperature (T_N) is observed clearly. It is observed that different parameters influence the velocity of sound.     

The current-induced effect on the Jahn-Teller distortion in the La0.5Ca0.5MnO3 manganite

The influence of dc current on the resistivity ρ and the Young's modulus E of La_0.5Ca_0.5MnO₃ compound has been investigated by means of an in situ measuring method. At low temperatures, both the resistivity ρ and the relative modulus ΔE increase with the current. A relaxation behavior of ρ to the higher resistive state is observed at a fixed temperature and a constant current. After storing the sample for a few days, ρ decreases with the current, accompanying a slight drop of ΔE at low temperatures. Current-induced effects on ρ and ΔE are interpreted according to the current-induced interwinning of Mn³⁺O₆ octahedral distortion modes between Q₂- and Q₃-types, which is suggested to contribute to the variation of the resistivity.     

Dielectric and AC conductivity behavior of BaBi2Nb2O9 ceramics

The complex dielectric and AC conductivity response of BaBi₂Nb₂O₉ relaxor ferroelectric ceramics were studied as a function of frequency (100 Hz-10 MHz) at various temperatures. The observed dielectric behavior was characterized by two types of relaxation processes which were described by the ‘universal relaxation law’. The frequency dependence of conductivity which showed a classical relaxor behavior followed the Jonscher's universal law σ(ω)=σ₀+Aωⁿ. The exponent n exhibited a minimum in the vicinity of temperatures of dielectric anomaly while the pre-factor A showed a maximum. The temperature dependence of n followed the Vogel-Fulcher relation with activation energy of about 0.14 eV.     

Magnetic disorder resistivity of RECu2Si2 compounds

The resistivity of RECu₂Si₂ compounds contains a term which is due to a mixture of spin and aspherical Coulomb scattering. The disorder resistivities and the ordering temperatures scale well with each other but deviate strongly from the de Gennes factor. The deviations scale with an anomaly of the c/a ratio which develops at low temperatures for the RE ions with L ≠ 0.     

Temperature dependence of magnetic anisotropy in nanoparticles of CoxFe(3−x)O4

In this paper we present a study of the magnetic anisotropy constant of nanocrystalline magnetic particles of Co_xFe_(3−x)O₄, with x ranging from 0.05 to 1.6, synthesized by a combustion reaction. The magnetic anisotropy constants were obtained by fitting the high-field part of the major hysteresis loops with the law of approach equation down to temperatures of 4 K and up to fields of 60 kOe. The anisotropy constant depends strongly on both temperature and cobalt content x, exhibiting a nonmonotic dome-shaped dependence on x with a maximum at x=1.0. We found that fits at lower temperatures, i.e., 4 and 72 K, give values of K₁ that are approximately one order of magnitude higher than those at higher temperatures, i.e., 272 and 340 K. For example, K₁ for specimens with x=0.8 and 1.0 are 4.21×10⁷ and 4.22×10⁷ ergs/cm³ at 4 K, and 7.64×10⁶ and 7.51×10⁶ ergs/cm³ at 340 K, respectively. Thus, our determination of temperature-dependence of the anisotropy constant represents an improvement over existing works.     

N2- and O2-broadening coefficients in the ν2 and ν5 bands of CH3F at 183 and 298 K

The N₂- and O₂-broadening coefficients of 33 rovibrational lines in the ν₂ and ν₅ bands of ¹²CH₃F were measured at 183 K using a diode-laser spectrometer. The measurement of these coefficients was also realized at room temperature for 10 of these lines to determine their temperature dependence. The line parameters were obtained by fitting to the experimental profile the Voigt lineshape, and the Rautian and Galatry models taking into account the collisional narrowing. Calculations of the pressure-broadening coefficients were also performed for the same temperatures from a semiclassical model involving electrostatic, induction and dispersion interactions in the intermolecular potential. The calculated values reproduce well the experimental data for both temperatures and both perturbers and the theoretical temperature dependence of the broadening coefficients is in satisfactory agreement with that derived from the measurements.     

Magnetic phase diagram of double-layered La2−2xCa1+2xMn2O7 manganite

Double-layered manganite La_2−2xCa_1+2xMn₂O₇ have been synthesized for compositions ‘x’=0.0, 0.1, 0.2, 0.3, 0.4 and 0.5 by solid state reaction method. From X-ray diffraction study, their crystal structures were found to be tetragonal perovskite with lattice parameters decreasing with increasing ‘x’. The decreasing lattice parameters affect the balance between in-plane, intra-bilayer and inter-bilayer exchange interactions, which is reflected on magnetotransport properties. The metal-to-insulator transition temperature is found to vary with composition and peaked around ‘x’=0.3. From ac-susceptibility study, 2D-ferromagnetic ordering was observed at higher temperatures for all compositions whereas 3D-ferromagnetic ordering was observed at quite low temperatures. In low-temperature region, decreasing susceptibility shows antiferromagnetic state for all compositions. On the basis of electrical and magnetic properties, a magnetic phase diagram is given.     

Influence of temperature on critical fields in ZnCr2Se4

The complex ac dynamic magnetic susceptibility was used to study the influence of temperature on critical fields in polycrystalline ZnCr₂Se₄ spinel. An antiferromagnetic order with a Néel temperature T_N=20.7 K and a strong ferromagnetic exchange evidenced by a positive Curie-Weiss temperature θ_CW=55.1 K were established. An increasing static magnetic field shifts T_N to lower temperatures while a susceptibility peak at T_m in the paramagnetic region—to higher temperatures. The non-zero and negative values both of the second and third harmonics of susceptibility suggest only a parallel spin coupling in ferromagnetic clusters in the range between the Néel and Curie-Weiss temperatures. Below T_N the magnetic field dependence of susceptibility, χ_ac(H), shows two peaks at critical fields H_c1 and H_c2. The values of H_c1 decrease slightly with temperature while the values of H_c2 drop rapidly with temperature. The strong changes of H_c2 temperature induced are mainly responsible for a spin frustration of the re-entrant type in the spinel under study.     

Magnetic anisotropy in Co73Mo2Si15B10 and (Co0.89Fe0.11) 72Mo3Si15B10 metallic glasses,induced by stress-annealing

Annealing temperature dependence of the stress-induced magnetic anisotropy in Co₇₃Mo₂Si₁₅B₁₀ (λ_s < 0) and (Co_0.89Fe_0.11) ₇₂Mo₃Si₁₅B₁₀ (λ > 0) metallic glass ribbons has been studied experimentally. The room temperature values of the induced anisotropy constants K depend strongly on the annealing conditions, and reveal a change of sign at annealing temperatures well below T_cryst. It is concluded that transient creep and steady-state creep at the elevated temperature give rise to compressive and tensile stresses, respectively, in the expression for the magnetoelastic coupling energy at room temperature.