Preparation and low field magnetoresistance of double layered manganite La1.4Ca1.6Mn2O7

Double layered manganite of La_1.4Ca_1.6Mn₂O₇ (DLCMO) was prepared using solid state reaction method and had a metal-insulator transition temperature (T_MI) of 125 K. The short range 2D-feerromagnetic ordering (T_C2) starts growing when T<168 K and it gets converted into 3D-ferromagnetic ordering (T_C1) at 114 K. Low field magnetoresistance (MR) behaviour of the DLCMO was investigated and compared with an infinite layered manganite La_0.7Ca_0.3MnO₃ (LCMO). For DLCMO, in the temperature range between T_C1 and T_C2, the MR showed a gradual increase with the magnetic field. The observed MR and R-T behaviour of double layered manganite for T_C1<T<T_C2 has been explained in the frame work of the two phase model [ferromagnetic (FM) domains and paramagnetic (PM) regions] and percolative behaviour of transport in FM-PM mixture.     

Study of magnetotransport in double-layered La1.4Ca1.6Mn2O7 manganite: Presence of nano-ferromagnetic domains in paramagnetic matrix

Double-layered manganite La_1.4Ca_1.6Mn₂O₇ has been synthesized using the solid-state reaction method. It had a metal-to-insulator transition at temperature T_M1≈127 K. The temperature dependence of ac susceptibility showed a broad ferromagnetic transition. The two-dimensional (2D)-ferromagnetic ordering temperature (T_C2) was observed as ≈245 K. The temperature dependence of its low-field magnetoresistance has been studied. The low-field magnetoresistance of double-layered manganite, in the temperature regions between T_M1 and T_C2, has been found to follow 1/T⁵. The observed behaviour of temperature dependence of resistivity and low-field magnetoresistance has been explained in terms of two-phase model where ferromagnetic domains exist in the matrix of paramagnetic regions in which spin-dependent tunneling of charge carriers occurs between the ferromagnetic correlated regions. Based on the two-phase model, the dimension of these ferromagnetic domains inside the paramagnetic matrix has been estimated as ∼12 Å.     

Synthesis of magnetoresistive La0.7Sr0.3MnO3 nanoparticles by an improved chemical coprecipitation method

La_0.7Sr_0.3MnO₃ nanoparticles were prepared by a simple chemical coprecipitation route. Structural, magnetoresistance (MR), and magnetic properties were investigated. Rietveld refinement of X-ray powder diffraction result shows that the sample is single-phase with the space group of R3¯C. The result of field-emission scanning electronic microscopy shows that most of the grain sizes are distributed from 50 to 200 nm. The composition determined by energy-dispersive spectroscopy is the stoichiometry of La_0.7Sr_0.3MnO₃. The ferromagnetic to paramagnetic transition is sharp with Curie temperature T_C=367 K, which further confirms that the sample is single-phase. The steep change in MR at low fields is attributed to the alignment of the magnetization, while the high-field MR is due to the grain boundary effect.     

Low temperature magnetoresistance in La1.32Sr1.68Mn2O7 layered manganite under hydrostatic pressure

The La_1.32Sr_1.68Mn₂O₇ layered manganite system has been studied by the low temperature electrical resistance and magnetoresistance under hydrostatic pressure up to 25 kbar. We have observe both, a Curie temperature (T_C) and a metal-insulator transition (T_MI) at 118 K in the ambient pressure. The applied pressure shifts the T_MI to higher temperature values and induces a second metal-insulator transition (T²_MI) at 90 K, in the temperature dependence of resistivity measurements. Also, the pressure suppresses the peak resistance abruptly at T_C. When an external field of 5 T is applied, we have observed a large negative magnetoresistance of 300% at the transition temperature and a 128% at 4.5 K. However, the increased pressure decreases the magnetoresistance ratio gradually. When the pressure reaches its maximum available value of 25 kbar, the magnetoresistance ratio decreases at a rate of 1.3%/kbar. From our experimental results, the decrease of magnetoresistance ratio with pressure is explained by the pressure induced canted spin state which is not favor for the spin polarized intergrain tunneling in layered manganites.     

Magnetic phase coexistence in Tb- and Sr-doped La0.7Ca0.3MnO3 manganite:A temperature-dependent neutron diffraction study

We report the results of the temperature-dependent neutron diffraction measurements on the nearly half-doped (La_0.325Tb_0.125)(Ca_0.3Sr_0.25)MnO₃ manganite sample. The simultaneous doping of magnetic Tb³⁺ and divalent Sr²⁺ in the La_0.7Ca_0.3MnO₃ system results into a large A-site size disorder. Rietveld refinement of neutron diffraction data reveal that the single phase sample crystallizes in a distorted orthorhombic structure. Increased 〈r_A〉 value affects the transport behavior that results into an insulating-like behavior of the sample. Under application of 1 T field sample exhibit insulating-like behavior while insulator-metal transition (T_IM) is exhibited under 5 and 8 T fields. Variable range hoping (VRH) mechanism of charge carriers is exhibited in the insulating region. Field cooled and zero field cooled magnetization measurement shows the Curie temperature (T_C)~47 K. The refinement of the ND data collected at various temperatures below 300 K shows that there is no structural phase transition in the compound. Around 100 K, a magnetic peak appears at lower angle that can be ascribed to the presence of the A-type antiferromagnetic (AFM) phase. Two more peaks are observed around 50 K at lower angles that can be fitted in CE-type antiferromagnetic phase. Splitting of the peaks at lower temperatures is the signature of orbital ordering in the presently studied nearly half-doped manganite system. Results of the detailed structural analysis of the temperature-dependent ND measurements on (LaTb)_0.45(CaSr)_0.55MnO₃ sample has been discussed in the light of coexisting A-type and CE-type antiferromagnetic phases present in the sample at low temperature.     

The transport and magnetic properties of La–Pb–Mg–Mn–O manganites at low temperatures

The structure, transport properties and the magnetoresistance behavior in the temperature interval 77–400 K of the perovskite-like lanthanum manganites La_0.6Pb_0.4−xMg_x+yMnO₃ (x=0, 0.1, 0.2 and y=0, 0.2) were investigated. Polycrystalline bulk samples were prepared by sol–gel self-combustion and subsequent heat treatment at 1000 °C for different times, 40, 80, 160 and 320 min. All manganites exhibit a peak in the resistivity around 200–250 K, below the ferromagnetic ordering temperature (320–330 K). An isotropic and negative magnetoresistance has been observed in all compounds. Magnetoresistance MR exhibits a peak in the temperature range 130–150 K, below SC–metal transition temperature. Magnitude of MR at the peaks was nearly 27% in the magnetic field of 2 T. At room temperature, a magnetoresistance of 9.5% for La_0.6Pb_0.2Mg_0.2MnO₃ composition was obtained. Longer heat treatment time enhanced the magnetorezistive properties.     

Effect of pressure and magnetic field on bilayer La1.25Sr1.75Mn2O7 single crystal

We report the temperature dependence of susceptibility for various pressures, magnetic fields and constant magnetic field of 5 T with various pressures on La_2−2xSr_1+2xMn₂O₇ single crystal to understand the effectiveness of pressure and magnetic field in altering the magnetic properties. We find that the Curie temperature, T_c, increases under pressure (dT_c/dP=10.9 K/GPa) and it indicates the enhancement of ferromagnetic phase under pressure up to 2 GPa. The magnetic field dependence of T_c is about 26 K for 3 T. The combined effect of pressure and constant magnetic field (5 T) shows dT_c/dP=11.3 K/GPa and the peak structure is suppressed and broadened. The application of magnetic field of 5 T realizes 3D spin ordered state below T_c at atmospheric pressure. Both peak structure in χ_c and 3D spin ordered state are suppressed, and changes to 2D-like spin ordered state by increase of pressure. These results reveal that the pressure and the magnetic field are more competitive in altering the magnetic properties of bilayer manganite La_1.25Sr_1.75Mn₂O₇ single crystal.     

Magnetoimpedance in La0.67Pb0.33MnO3 manganite prepared by sol–gel method

In the present work, manganite La_0.67Pb_0.33MnO₃ was prepared by the sol–gel method. The difference between metal–insulator transition temperature T_MI (217 K) and Curie temperature T_c (342 K) in the sol–gel nanocrystalline manganite is mainly due to the grain boundary effect. The breaking of Mn–O–Mn bonds and strong scattering at the grain boundary cumber the transport. At room temperature 300 K, impedance and resistance increase with increasing frequency of ac currents. The observed dc magnetoresistance in sol–gel La_0.67Pb_0.33MnO₃ is related to the spin-polarized inter-grain tunneling and spin-dependent scattering at grain boundaries. The sol–gel manganite shows the magnetoimpedance characteristics, which are different from those of traditional sintered manganites and metallic giant magnetoimpedance materials. For sol–gel La_0.67Pb_0.33MnO₃ at low frequencies, the impedance experiences a peak under a low longitudinal field. In contrast, at high frequencies the peak phenomenon disappears, and the impedance drops sharply with low fields, which is due to the inter-grain or grain boundary effect. The permeability also sensitively varies with an application of transverse field. The magnetoimpedance effect in sol–gel nanocrystalline manganite is influenced by both field-induced permeability change and dc magnetoresistance.     

Large negative magnetoresistance in thiospinel CuCrZrS4

We report on large negative magnetoresistance observed in ferromagnetic thiospinel compound CuCrZrS₄. The electrical resistivity increased with decreasing temperature according to the exp(T₀/T)^1/2, an expression derived from variable range hopping with strong electron-electron interaction. The resistivity under a magnetic field was expressed by the same form with the characteristic temperature T₀ decreasing with increasing magnetic field. Magnetoresistance ratio ρ(T,0)/ρ(T,H) is 1.5 for H=90 kOe at 100 K and increases divergently with decreasing temperature reaching 80 at 16 K. Results of magnetization measurements are also presented. A possible mechanism of the large magnetoresistance is discussed.     

Low temperature magnetization and magnetoresistance studies on the layered manganite system La1.2Sr1.8Mn2−xRuxO7 (x=0, 0.1, 0.5, 1.0)

We report the detailed results of magnetization and magnetoresistance measurements in the Ru doped layered manganite system La_1.2Sr_1.8Mn_2−xRu_xO₇ (x=0, 0.1, 0.5, 1.0). High-resolution measurements of magnetization and magnetoresistance were carried out as functions of temperature, magnetic field and time. We find evidence for the existence of competing ferromagnetic and antiferromagnetic interactions resulting in the formation of a frustrated spin-glass-like state at low temperatures. The time dependent magnetization follows the relation very well. We find that Ru doping enhances the coercive field and drives the system towards a magnetically mixed phase at low temperatures. Large negative magnetoresistance values are observed in all samples and at low temperatures the magnetoresistance varies as the square root of the applied magnetic field.     

Increase in Tc and spin glass transition in La0.9Ca0.1Mn1−yCryO3 (y=0, 0.1 and 0.2)

We report on the structural, frequency dependent ac susceptibility, dc magnetization and magnetoresistance (MR) measurements on polycrystalline samples of La_0.9Ca_0.1Mn_1−yCr_yO₃ (y=0, 0.1 and 0.2) prepared by sol-gel technique. For y=0, a paramagnetic to ferromagnetic transition is observed at T_c=136 K. Both for y=0.1 and 0.2, T_c increases from 136 to 180 K. For y=0, the imaginary part of the ac susceptibility shows a broad transition at T_f<T_c which does not depend very much on the frequency. However, for y=0.1 and 0.2, the frequency dependence resembles that of a spin glass. Though all the three samples show a semi-conducting behavior between 300 and 5 K, a negative MR is observed corresponding to T_c and T_f. The value of MR decreases for the Cr substituted samples.     

Room temperature ferromagnetism and magnetotransport properties of the layered manganite system La1.2Ba1.8Mn2−xRuxO7 (0≤x≤1.0)

The dc magnetization and ac susceptibility measurements on two dimensional layered manganite La_1.2Ba_1.8Mn₂O₇ samples reveal the occurrence of ferromagnetism above room temperature with ferromagnetic (FM) to paramagnetic (PM) transitions at 338 K. The bifurcation temperatures shown by the zero-field cooled (ZFC) and field cooled (FC) dc magnetization curves at high temperatures shift towards lower temperatures as the applied field is increased from 100 to 2500 Oe. The data are suggestive of a large magnetic anisotropy due to the strong competing ferromagnetic and antiferromagnetic interactions resulting in a spin-glass-like state. Ru doping is found to enhance the ferromagnetism and metallicity of the system in a remarkable way. The magnetoresistance (MR) values obtained are very high and about 40% even at 260 K for the undoped sample.     

Synthesis, structural and transport properties of nanocrystalline La1−xBaxMnO3 (0.0≤x≤0.3) powders

Nanocrystalline La_1−xBa_xMnO₃ (0.0≤x≤0.3) manganites have been prepared by a simple and instantaneous solution combustion method, which is a low temperature initiated synthetic route to obtain fine-grained powders with relatively high surface area. The phase purity and crystal structure of the combustion products are carried out by powder X-ray diffraction. The as-made nanopowders are in cubic phase. On calcination to 900 °C, barium doped manganites retain cubic phase, whereas barium free manganite transformed to rhombohedral phase. The scanning electron microscope (SEM) results revealed that the combustion-derived compounds are agglomerated with fine primary particles. The doped manganites have surface area in the range 24-44 m²/g. The surface area of the manganites increases with barium content, whereas it decreases on calcination. Both undoped and doped lanthanum manganites show two active IR vibrational modes at 400 and 600 cm⁻¹. The low temperature resistivity measurements have been carried out by four-probe method down to 77 K. All the samples exhibit metal-insulator behaviour and metal-insulator transition temperature (T_M-I) in the range 184-228 K and it is interesting to note that, as the barium content increases the T_M-I shifts to lower temperature side. The maximum T_M-I of 228 K is observed for La_0.9Ba_0.1MnO₃ sample.     

Effect of Al doping on the magnetic and electrical properties of layered perovskite La1.3Sr1.7Mn2−xAlxO7

The effect of Al substitution for Mn site in layered manganese oxides La_1.3Sr_1.7Mn_2−xAl_xO₇ on the magnetic and electrical properties has been investigated. It is interesting that all the samples undergo a similar and complex transition with lowing temperature; they transform from the two-dimensional short-range ferromagnetic order at T*, then enter the three-dimensional long-range ferromagnetic state at T_C, at last they display the canted antiferromagnetic state below T_N. T*, T_C and T_N are all reduced with Al content. Resistivity increases sharply with increasing Al concentration, and the metal-insulator transition disappears when x reaches 10%. Additionally, magnetoresistance (MR) effect is weakened. Al substitution dilutes the magnetic active Mn-O-Mn network and weakens the double exchange interaction, and further suppresses FM ordering and metallic conduction. Owing to the anisotropic interaction in the layered perovskite, the magnetic and electrical properties are more sensitive to Al doping level than those in ABO₃-type perovskite.     

Heat capacity of EuMnO3 and Eu0.7A0.3MnO3 (A=Ca,Sr) compounds

We carried out the heat capacity calculation of the magnetoresistance compounds EuMnO₃ and Eu_0.7A_0.3MnO₃ (where A=Ca and Sr) as a function of temperature from 5 to 100 K, using the Rigid Ion Model (RIM). The results on heat capacity for EuMnO₃ and Eu_0.7A_0.3MnO₃ (A=Ca and Sr) obtained by us are in good agreement with the measured values. Although strong electron–phonon interactions are present in these compounds but the lattice part of the specific heat also deserves proper attention. The parent compound EuMnO₃ exhibits two magnetic transitions at 35 and 47 K due to weak ferromagnetic (FM) component and antiferromagnetic (AF) ordering. In addition, we have reported cohesive energy (φ), molecular force constant (f), compressibility (β), Restrahalen frequency (υ₀), Debye temperature (θ_D) and Gruneisen parameter (γ) in the temperature range 5 K?T?100 K.     

Emission Mössbauer studies of the magnetoresistive compound, La0.7Sr0.3MnO3

The magnetic behavior of the Sr_0.3 manganite is studied using a local microprobe, ⁵⁷Co. In contrast with Ca substituted manganites, a much larger fraction of the material exhibits short-range order with superparamagnetic-like behavior even at 80 K. The differences in behavior are attributed to the large mismatch between the ionic radii of La⁺³ and the divalent substituent Sr⁺², which introduces anharmonicity in local vibrations. In common with all other compounds exhibiting negative bulk magnetoresistivity, the Sr_0.3 compound also exhibits very marked softening of lattice as one approaches T_c from below. Application of an external magnetic field results in coalescing of nanosized magnetic clusters to form larger ones with better alignment of spins.     

Highly cation-deficient manganese perovskite, La1−xMn1−yO3 with x=y

Oxidative (δ>0) nonstoichiometry in the perovskite ‘LaMnO_3+δ’ has been known to be manifested not with O interstitials but rather with cation vacancies of equal amounts at the two cation sites, La and Mn, i.e. La_1−xMn_1−yO₃ with x=y. Here, we report the fabrication of samples with record-high cation-vacancy concentrations (x>0.12 or δ>0.4) by means of a variety of high-pressure oxygenation techniques. Linear (negative) dependence of the cell volume on x was observed within the whole x range investigated, down to 56.9 Å³ (per formula unit) for a sample oxygenated at 5 GPa and 1100 °C using Ag₂O₂ as an excess oxygen source. With increasing degree of cation deficiency in La_1−xMn_1−xO₃, the ferromagnetic transition temperature was found to follow a bell shape with respect to x exhibiting a maximum of ∼250 K about x≈0.1. For moderately oxygenated samples large magnetoresistance effect was evidenced.     

Magnetic phases in lanthanum-strontium manganite-cobaltite La1.25Sr0.75MnCoO6

Two methods—the solid-phase high-temperature (1300 °C) and the liquid-phase low-temperature (750 °C) routes—were used to synthesize the complex oxide La_1.25Sr_0.75MnCoO₆, which has the structure of rhombohedral perovskite and is characterized by a disordered distribution of Mn and Co in structural sites. It was found by means of X-ray absorption near edge spectroscopy (XANES) at the K-edge that mixed valence states of Co²⁺/Co³⁺ and Mn³⁺/Mn⁴⁺, exist in both phases. Measurements of dc magnetization and real (χ′) and imaginary (χ″) parts of the ac susceptibility showed that the magnetic properties of these oxides are determined by a ferromagnetic transition at T_C=217 K and a frequency-dependent transition at T_g<100 K. The high frequency dependence of T_g is indicative of the cluster-glass behavior of La_1.25Sr_0.75MnCoO₆ (7 5 0) at T<T_C within the ferromagnetic state.     

Structural and magnetic phase diagram and room temperature CMR effect of La1−xAgxMnO3

The study of the structural and magnetic phase diagram of the manganites La_1−xAg_xMnO₃ shows similarity with the La_1−x′Sr_x′MnO₃ series, involving a metallic ferromagnetic domain at relatively high temperature (≈300 K). The Ag-system differs from the Sr-one by a much smaller homogeneity range (x≤1/6) and the absence of charge ordering. But the most important feature of the Ag-manganites deals with the exceptionally high magnetoresistance (−25%) at room temperature under 1.2 T, that appears for the composition x=1/6. The latter is interpreted as the coincidence of the optimal double exchange condition (Mn³⁺:Mn⁴⁺=2) with T_max=300 K (maximum of the ρ(T) curve in zero field).     

Magnetic properties and charge ordering in Pr0.75Na0.25MnO3 manganite

The structural and magnetic properties of Pr_0.75Na_0.25MnO₃ have been investigated experimentally. At room temperature, the compound shows paramagnetic characteristic. Along with decreasing temperature, a peak appears in the magnetization versus temperature curve around 220 K. To clarify whether this peak is associated with the ordering arrangement of Mn³⁺ and Mn⁴⁺ ions, electron diffraction experiments were carried out below and above 220 K respectively. Only basic Brag diffraction spots can be observed at high temperatures, however, superlattice diffraction appears below 220 K. This provides direct evidence for the existence of charge ordering in Pr_0.75Na_0.25MnO₃. We find the Mn³⁺ and Mn⁴⁺ cations form zigzag chains in a-c plane by analyzing the diffraction patterns. Combining with the magnetization measurements and the results of electron spin resonance, we confirm the antiferromagnetic phase and ferromagnetic component coexist in Pr_0.75Na_0.25MnO₃ below 120 K.