Magnetoresistance in La1−xCaxMnO3 (0≤x<0.4)

The magnetic and transport properties of La_1−xCa_xMnO₃ (0≤x<0.4) have been systematically studied. The magnetoresistance (MR) maximum appears at x=0.2-0.25 and the temperature dependence of MR for x>0.25 shows a much broader profile than that of samples for x=0.2-0.25. Based on a scenario in which there is a short-range charge ordering (CO) state coexisting in the ferromagnetic state matrix for x>0.25, and the least or even no short-range CO state exists in samples for x=0.2-0.25, the above observations can be understood.     

Disorder induced ferromagnetism in the Cu-doped molybdate SrMo1−xCuxO3 (0≤x≤0.20)

The effect of Cu-doping at Mo-site on structural, magnetic, electrical transport and specific heat properties in molybdates SrMo_1−xCu_xO₃ (0≤x≤0.2) has been investigated. The Cu-doping at Mo-site does not change the space group of the samples, but decreases the structural parameter a monotonously. The magnetic properties change from Pauli-paramagnetism for x=0 to exchange-enhanced Pauli-paramagnetism for x=0.05 and 0.10, and then ferromagnetism for x=0.15 and 0.20. All samples exhibit metallic-like transport behavior in the whole temperature range studied. The magnitude of resistivity increases initially to x=0.10 and then decreases with increasing Cu-doping concentration. The results are discussed according to the electron localization due to the disorder effect induced by the random distribution of Cu at Mo site in the samples. In addition, the temperature dependence of specific heat for the Cu-doped sample has also been studied.     

Magnetocaloric effects in (Gd1−xTbx)Co2

The structures and magnetocaloric effects of (Gd_1−xTb_x)Co₂ (x=0, 0.25, 0.4, 0.5, 0.6, 0.7, 0.8, and 1) pseudobinary compounds were investigated by X-ray powder diffraction and magnetic properties measurement. The results show that the T_c of the alloy is near room temperature when X=0.6. The magnetic entropy changes of the compounds increase from 1.7 to 3.6 J/kg K with increasing the content of Tb under an applied field up to 2 T. All the compounds exhibit second order magnetic change. As a result, the values of their ΔS_M are lower than that of some large magnetocaloric effect materials.     

Electrical and magnetic properties of non-stoichiometric (La0.8Sr0.2)1−xMnO3 perovskites

The structure, transport and magnetic properties of (La_0.8Sr_0.2)_1−xMnO₃ (0≤x≤0.30) polycrystalline perovskite manganites have been investigated. For all the samples the Curie temperatures, T_c, remain nearly unchanged (329±3 K). Resistivity versus temperature curves for the samples show a double-peak behavior. A significant magnetoresistance (MR) effect and different temperature dependences of the MR ratios of the samples are observed. The shapes of the MR-T curves of the samples can be adjusted by changing x. For the x=0.30 sample, a nearly constant MR ratio of (9.5±0.5)% is obtained over the temperature range from 205 to 328 K.     

The large low-field magnetic entropy changes in Ni43Mn46Sn11−xSbx alloys

A series of Ni₄₃Mn₄₆Sn_11−xSb_x (x=0, 1, and 3) alloys were prepared by an arc melting method. The martensitic transition shifts to higher temperature with the increasing Sb content. The isothermal magnetization curves and Arrott plots around martensitic transition temperatures show a typical metamagnetic behavior. Under a low applied magnetic field of 10 kOe, large magnetic entropy changes around the martensitic transition temperature are 10.4, 8.9, and 7.3 J/kg K, for x=0, 1, and 3, respectively. The origin of the large magnetic entropy changes and potential application for Ni₄₃Mn₄₆Sn_11−xSb_x alloys as working substances in magnetic refrigeration are discussed.     

Large magnetoresistance in low temperature metallic region of manganite compounds (La0.7−2xEux)(Ca0.3Srx)MnO3 (0.05≤x≤0.15)

Magnetoresistance (MR) and magnetization (dc and ac) measurements have been carried out on the manganites, (La_0.7−2xEu_x)(Ca_0.3Sr_x)MnO₃ (0.05≤x≤0.15), in the temperature range of 5-320 K. At 5 K, an unusually large MR of almost 98% is observed in the x=0.15 sample, nearly up to fields of 4-5 T. This large high-field MR occurs in the metallic region, far below the insulator-metal transition temperature, and does not vary linearly with applied field. The unusual magnetoresistance is explained in the light of various possibilities such as phase segregation, cluster spin-glass behavior, etc.     

Metal-insulator transition in the spinel-type Cu(Ir1−xCrx)2S4 system

A normal thiospinel CuIr₂S₄ exhibits a temperature-induced metal-insulator (M-I) transition around 230 K with structural transformation, showing hysteresis on heating and cooling. On the other hand, CuCr₂S₄ has the same normal spinel structure without the structural transformation. CuCr₂S₄ has been found to be metallic and ferromagnetic with the Curie temperature T_c~377 K. In order to see the effect of substituting Cr for Ir on the M-I transition, we have carried out a systematic experimental study of electrical and magnetic properties of Cu(Ir_1−xCr_x)₂S₄. The M-I transition temperature shifts to lower temperature with increasing Cr-concentration x and this transition is not detected above x~0.05. The ferromagnetic transition temperature decreases as x is decreased and the transition does not occur below x~0.20.     

Structural stability and magnetic properties of Bi1−xLa(Pr)xFeO3 solid solutions

In this work, X-ray diffraction data taken on Bi_1−xLa_xFeO₃ solid solutions are used to verify the following structural phase transitions: “polar rhombohedral-antipolar orthorhombic” at x≈0.16 and “commensurate-incommensurate” within the orthorhombic phase at x≈0.18. In contrast, in the Bi_1−xPr_xFeO₃ series, the polar rhombohedral phase transforms into an antipolar orthorhombic one at x≥0.13. The polar rhombohedral phase near the morphotropic phase boundary exhibits an isothermal transformation into an antipolar orthorhombic phase, though the transformation occurs much faster in the case of La-doped compounds. The incommensurate structural phase was not detected in Bi_1−xPr_xFeO₃ solid solutions. The ternary structural phase diagram is constructed for (Bi,La,Pr)FeO₃ systems. In addition, the polar rhombohedral phase exhibits a magnetic field-induced transition from the modulated antiferromagnetic state into a homogeneous weak ferromagnetic state whereas the antipolar phase is a weak ferromagnetic state in the absence of an external field.     

Structure and dielectric properties of (Na0.50Bi0.50)1−xBaxTiO3: 0≤x≤0.10

Solid solution of (1−x)Na_0.5Bi_0.5TiO₃-xBaTiO₃ is investigated in the composition range 0.00≤x≤0.10. It is shown that the system exhibits rhombohedral structure up to x=0.055 and then becomes ‘nearly cubic’ for x≥0.06. Temperature dependent dielectric measurements reveals three peaks in the imaginary part of the dielectric constant for compositions exhibiting rhombohedral as well as ‘nearly cubic’ structures. The first of these three peaks exhibits Vogel-Fulcher type relaxation behaviour.     

Low temperature specific heat of bi-layered manganites La2−2xSr1+2xMn2O7 (x=0.3 and 0.5)

The specific heat (C) of bi-layered manganites La_2−2xSr_1+2xMn₂O₇ (x=0.3 and 0.5) is investigated for the ground state of low temperature excitations. A T^3/2 dependent term in the low temperature specific heat (LTSH) is identified at zero magnetic field and suppressed by magnetic fields for x=0.3 sample, which is consistent with a ferromagnetic metallic ground state. For x=0.5 sample, a T² term is observed and is consistent with a two-dimensional (2D) antiferromagnetic insulator. However, it is almost independent of magnetic field within the range of measured temperature (0.6-10 K) and magnetic field (6 T).     

Anisotropy and FOMP in Tb3 (Fe28−xCox) V1.0 (x=0, 3 and 6) compounds

In this work, the structural and magnetic properties of Tb₃ (Fe_28−xCo_x) V_1.0 (x=0, 3, 6) compounds have been investigated. The structural characterization of compounds by X-ray powder diffraction is an evidence for a monoclinic Nd₃(Fe, Ti)₂₉-type structure (A2/m space group). The refined lattice parameters a and b (but not c) and the unit cell volume V, obtained from the XRD data by the Rietveld method, are found to decrease with increasing Co concentration. The unit cell parameters behavior has been attributed to the smaller Co atoms and a preferential substitution of Fe by Co. The anisotropy field (H_a) as well as critical field (H_cr) was measured using the singular point detection (SPD) technique from 5 to 300 K in a pulsed magnetic field of up to 30 T. At T=5 K, a FOMP of type 2 was observed for all samples and persists at all temperatures up to 300 K. For sample x=0, H_cr=10.6 and 2.0 T at 5 and 300 K, respectively, is equal to that reported earlier. The occurrence of canting angles between the magnetic sublattices during the magnetization process instead of high-order anisotropy contributions (at room temperature are usually negligible) has been considered to explain the survival of the FOMP at room temperature. The anisotropy and critical fields behave differently for samples with x=0, 3 compared with x=6. The observed behavior has been related to the fact that the Co substitution for Fe takes place with a preferential entrance in the inequivalent crystallographic sites of the 3:29 structure. The contribution of the Tb-sublattice in the Tb₃(Fe, V)₂₉ compound with uniaxial anisotropy has been scaled from the anisotropy field measured on a Y₃(Fe, V)₂₉ single crystal with easy plane anisotropy.     

Open atmosphere synthesis and wide range colossal magnetoresistance in La0.7Sr0.3−xHgxMnO3 (0≤x≤0.2) system

We have synthesized several polycrystalline samples with nominal compositions La_0.7Sr_0.3−xHg_xMnO_3+δ (0≤x≤0.2) by the standard solid-state reaction method. Instead of the sealed quartz tube method widely employed for the Hg-based systems, we adopted open atmosphere synthesis route. All the samples exhibited monophasic nature with rhombohedral structure as revealed by the X-ray diffraction data. A variation in the unit cell volume is observed with x, which is interpreted as a result of extra oxygen in-diffusion and subsequent cation vacancy creation. A broad metallic behavior is seen in the entire temperature range from 300 to 4 K. The samples showed varying amount of colossal magnetoresistance depending upon the temperature and applied magnetic field. The MR value as high as 30% was observed in x=0.2 sample and the MR is persistent over a wide temperature range with a little change in magnitude.     

Magnetic and transport property studies of nanocrystalline ZnxFe3−xO4

The magnetic and transport properties of nanocrystalline Zn_xFe_3−xO₄ with x=0.0, 0.2, 0.4, 0.5, 0.6, 0.8 and 1.0, respectively, fabricated by the sol-gel method have been investigated. Large magnetoresistance (MR) was observed and found to be originated both from the tunneling of the spin-polarized electrons across the adjacent ferromagnetic grains and the scattering by the canted spins at the grain surface near the grain boundaries. It has been revealed that the MR for the Zn_xFe_3−xO₄ samples (x=0, 0.5 and 1.0) increases with the temperature decreasing from room temperature until a maximum is reached at around 55 K. Then a sharp drop occurs with the further decrease in temperature, regarded as a spin (cluster) glass transition. For the samples studied, a biggest low field (0.5 T) MR value of about 20% for x=0 at 55 K has been obtained. The mechanism of the MR behavior of the materials was discussed.     

The magnetic behavior of La1−xTbxMn2Si2 (0≤x≤0.3) in weak magnetic fields

The structure and magnetic properties of La_1−xTb_xMn₂Si₂ (0≤x≤0.3) were studied by X-ray powder diffraction and DC magnetization measurements. All the compounds crystallize in ThCr₂Si₂-type structure. Substitution of Tb for La led to a linear decrease in the lattice constants and the unit-cell volume. A ferromagnetic phase for x≤0.15, and an antiferromagnetic phase for x=0.3 have been observed at about room temperature, whereas the compounds with x=0.2 and 0.25 exhibit a magnetic phase transition from ferromagnetism to antiferromagnetism.     

Charge order melting and magnetic transition in Nd0.5(1+x)Ca0.5(1−x)Mn(1−x)CrxO3 system

The magnetic property of double doped manganite Nd_0.5(1+x)Ca_0.5(1−x)Mn_(1−x)Cr_xO₃ with a fixed ratio of Mn³⁺:Mn⁴⁺=1:1 has been investigated. For the undoped sample, it undergoes one transition from charge disordering to charge ordering (CO) associated with paramagnetic (PM)-antiferromagnetic (AFM) phase transition at T<250 K. The long range AFM ordering seems to form at 35 K, rather than previously reported 150 K. At low temperature, an asymmetrical M-H hysteresis loop occurs due to weak AFM coupling. For the doped samples, the substitution of Cr³⁺ for Mn³⁺ ions causes the increase of magnetization and the rise of T_c. As the Cr³⁺ concentration increases, the CO domain gradually becomes smaller and the CO melting process emerges. At low temperature, the FM superexchange interaction between Mn³⁺ and Cr³⁺ ions causes a magnetic upturn, namely, the second FM phase transition.     

Observation of magnetoelectric behavior at room temperature in Pb(FexTi1−x)O3

The co-existence of ferroelectric and ferromagnetic properties at room temperature is very rarely observed. We have been successful in converting ferroelectric PbTiO₃ into a magnetoelectric material by partly substituting Fe at the Ti site. The Pb(Fe_xTi_1−x)O₃ system exhibits ferroelectric and ferromagnetic ordering at room temperature. Even more remarkably, our results demonstrate a coupling between the two order parameters. Hence it could be a futuristic material to provide cost effective and simple path for designing novel electromagnetic devices.     

Specific heat and magnetic susceptibility of single-crystalline ZnCr2−xAlxSe4 (x=0.15, 0.23)

A correlation between the second critical field H_c2 of the helix to paramagnetic transition and the magnetic specific heat C-peak was found in ZnCr_2−xAl_xSe₄ spinel single crystals with x=0.15, 0.23. The specific heat peak is anomalously sharp for all finite magnetic fields used here and this points to a first order magneto-structural transition (from cubic to tetragonal symmetry). The C(T)-peak is increasingly suppressed as the external field increases. Approaching the Neel temperature T_N, a broad ac-magnetic susceptibility peak is observed for zero dc-magnetic field. That peak does not show an energy loss and thus points towards a return to a second order type of transition. The magnetic contribution to the specific heat displays a sharp peak at T_N and is maximal at the spin fluctuation temperature T_sf=34 K. T_sf is related to the maximum of the magnetic susceptibility at T_m=40 K (at 50 kOe) in the spin fluctuation region, as evidenced by the entropy exceeding 90% of the entropy calculated classically for the complete alignment of the Cr spins, (2−x)R ln(2S+1). The X-ray photoelectron spectroscopy (XPS) data indicate that Al-substitution does not affect Cr³⁺ 3d³ electronic configuration.     

Structure, magnetic, and transport properties of the Co-doped manganites La0.9Te0.1Mn1−xCoxO3 (0≤x≤0.25)

The effect of Co doping at Mn-site on the structural, magnetic and electrical transport properties in electron-doped manganties La_0.9Te_0.1Mn_1−xCoxO₃ (0≤x≤0.25) has been investigated. The room temperature structural transition from rhombohedra to orthorhombic (Pbnm) symmetry is found in these samples with x≥0.20 by the Rietveld refinement of X-ray powder diffraction patterns. All samples undergo the paramagnetic-ferromagnetic (PM-FM) phase transition. The Curie temperature T_C of these samples decreases and the transition becomes broader with increasing Co-doping level. The magnetization magnitude of Co-doping samples increases at low temperatures with increasing Co-doping level for x≤0.15 and decreases with increasing Co-doping content further. The metal-insulator (M-I) transitions observed in the sample with x=0 are completely suppressed with Co doping, and the resistivity displays semiconducting behavior within the measured temperature region for these samples with x>0. All results are discussed according to the changes of the structure parameters and magnetic exchange interaction caused by Co-doping. In addition, the different effects between the Co doping and Cu doping in the Mn site for the electron-doped manganites are also discussed.     

Influence of Ce doping on electrical and thermal properties of La0.7−xCexCa0.3MnO3 (0.0≤x≤0.7) manganites

The effect of Ce-doping on structural, magnetic, electrical and thermal transport properties in hole-doped manganites La_0.7−xCe_xCa_0.3MnO₃ (0.0≤x≤0.7) is investigated. The structure of the compounds was found to be crystallized into orthorhombically distorted perovskite structure. dc Susceptibility versus temperature curves reveal various magnetic transitions. For x≤0.3, ferromagnetic regions (FM) were identified and the magnetic transition temperature (T_C) was found to be decreasing systematically with increasing Ce concentration. The electrical resistivity ρ(T) separates the well-define metal-semiconducting transition (T_MS) for low Ce doping concentrations (0.0≤x≤0.3) consistent with magnetic transitions. For the samples with 0.4≤x≤0.7, ρ(T) curves display a semiconducting behavior in both the high temperature paramagnetic (PM) phase and low temperature FM or antiferromagnetic phase. The electron–phonon and electron–electron scattering processes govern the low temperature metallic behavior, whereas small polaron hopping model is found to be operative in PM phases for all samples. These results were broadly corroborated by thermal transport measurements for metallic samples (x≤0.3) in entire temperature range we investigated. The complicated temperature dependence of Seebeck coefficient (S) is an indication of electron–magnon scattering in the low temperature magnetically ordered regime. Specific heat measurements depict a broadened hump in the vicinity of T_C, indicating the existence of magnetic ordering and magnetic inhomogeneity in the samples. The observation of a significant difference between ρ(T) and S(T) activation energies and a positive slope in thermal conductivity κ(T) implying that the conduction of charge carriers were dominated by small polaron in PM state of these manganites.     

ESR investigation of the spin dynamics in (Gd1−xYx)2PdSi3

We report electron-spin resonance (ESR) measurements in polycrystalline samples of (Gd_1−xY_x)₂PdSi₃. We observe the onset of a broadening of the linewidth and of a decrease of the resonance field at approximately twice the Néel temperature in the paramagnetic state. This characteristic temperature coincides with the electrical resistivity minimum. The high-temperature behavior of the linewidth is governed by a strong bottleneck effect.