Critical behavior in Co-doped manganites La0.67Pb0.33Mn1−xCoxO3 (0≤x≤0.08)

The critical properties of perovskite manganite La_0.67Pb_0.33Mn_1−xCo_xO₃ (0≤x≤0.08) around the paramagnetic-ferromagnetic phase transition are investigated through various techniques such as the modified Arrott plot, Kouvel-Fisher method and critical isotherm analysis. Though the nature of this transition was found to be in second order, the estimated critical exponents β (0.233≤β≤0.368), γ (1.03≤γ≤1.40) and δ (4.32≤δ≤5.54) are in between the theoretically predicted values for three-dimensional Heisenberg and tricritical mean-field model. This model suggests the coexistence of the short-range and long-range ferromagnetic orders around the critical temperature. The values of the critical exponents obtained from different methods and the well-obeyed scaling behavior confirm that the calculated exponents are unambiguous and purely intrinsic to the system.     

Critical parameters near the ferromagnetic-paramagnetic phase transition in La0.7A0.3(Mn1−xbx)O3 (A=Sr; B=Ti and Al; x=0.0 and 0.05) compounds

The critical parameters provide important information concerning the interaction mechanisms near the paramagnetic-to-ferromagnetic transition. In this paper, we present a thorough study for the critical behavior of La_0.7A_0.3(Mn_1−xB_x)O₃ (A=Sr; B=Ti and Al; x=0.0 and 0.05) polycrystalline samples near ferromagnetic-paramagnetic phase transition temperature by analyzing isothermal magnetization data. We have analyzed our dc-magnetization data near the transition temperature with the help of the modified Arrot plot, Kouvel-Fisher method. We have determined the critical temperature T_C and the critical parameters β, γ and δ. With the values of T_C, β and γ, we plot M×(1−T/T_C)^−β vs. H×(1−T/T_C)^−γ. All the data collapse on one of the two curves. This suggests that the data below and above T_C obey scaling, following a single equation of state. Critical parameters for x=0 and x_Ti=0.05 samples are between those predicted for a 3D-Heisenberg model and mean-field theory and for x_Al=0.05 samples the values obtained for the critical parameters are close to those predicted by the mean-field theory.     

Critical behavior and magnetic entropy change in the La0.6Sr0.4Mn0.8Fe0.1Cr0.1O3 perovskite

Critical behavior in the La_0.6Sr_0.4Mn_0.8Fe_0.1Cr_0.1O₃ ceramics was studied using magnetization methods. Results show that the paramagnetic–ferromagnetic transition is of second order. Based on the critical behavior analysis using the Banerjee criterion and the Kouvel–Fisher method, we find the critical exponents: β=0.395±0.010, γ=1.402±0.010, and δ=5.208±0.007, for which the magnetic interaction is satisfied within the three-dimensional Heisenberg model. Results indicate the presence of short-range interactions. The magnetic entropy change (−ΔS_M) reached maximum values of 1.75, 1.45, 1.15, 0.8 and 0.43 J Kg⁻¹ K⁻¹ under a magnetic field variation of 5, 4, 3, 2 and 1 T, respectively. Nevertheless, these (−ΔS_M) values are much low for any potential application at this moment. The nature of this phenomenon is discussed in relation to the characteristics of the magnetic phase transition and critical exponents.     

Magnetic properties of R2Fe17−xGax (R=Y and Gd) compounds

The magnetic properties of Y₂Fe_17−xGa_x for 3≤x≤7 and Gd₂Fe_17−xGa_x for 5≤x≤7 have been investigated using ⁵⁷Fe Mössbauer spectroscopy. These compounds have the rhombohedral Th₂Zn₁₇ structure. X-ray diffraction analysis of aligned powders shows that the easy direction of magnetization is parallel to the c-axis in Y₂Fe₁₀Ga₇ and Gd₂Fe₁₀Ga₇ and is perpendicular to the c-axis in Y₂Fe₁₄Ga₃, Y₂Fe₁₂Ga₅, Gd₂Fe₁₂Ga₅ and Gd₂Fe₁₁Ga₆. Mössbauer studies indicate that those samples are ordered ferromagnetically. The ⁵⁷Fe hyperfine field decreases with increasing Ga content. This decrease results from the decreased magnetic exchange interactions resulting from Ga substitution. The average isomer shift, δ, for R₂Fe_17−xGa_x (R=Y and Gd) at room temperature is positive and the magnitude of δ increases with increasing Ga content.     

Structural,magnetic and magnetocaloric properties of AMn1−xGaxO3 compounds with 0≤x≤0.2

Structural, magnetic and magnetocaloric properties of manganites series with the AMn_1−xGa_xO₃ (A=La_0.75Ca_0.08Sr_0.17 and x=0, 0.05, 0.1 and 0.2) composition have been investigated to shed light on Ga-doping influence. Solid-state reaction method was used for preparation. From XRD study, all samples are found single phase and crystallize in the orthorhombic structure with the Pnma space group. The variation of the magnetization M vs. temperature T, under an applied magnetic field of 0.05 T, reveals a ferromagnetic–paramagnetic transition for all samples. The experimental results indicate that T_C decreases from 336 to 135 K with increasing Ga substitution. Magnetocaloric effect (MCE) was estimated, in terms of isothermal magnetic entropy change (−ΔS_M), using the M(T, μ₀H) data and employing the thermodynamic Maxwell equation. The maximum entropy change and Relative Cooling Power (RCP) show non-monotonic behaviors with increasing the concentration of Gallium. In fact, the maximum value of ΔS_Mmaxof AMn_1−xGa_xO₃ for x=0.00 and 0.2 samples is found to be, respectively, 2.87 and 1.17 J/kg/K under an applied magnetic field change of 2 T. For the same applied magnetic field (μ₀H=2 T), the RCP values are found to vary between 97.58 and 89 J/kg.     

A study on magnetoelastic properties of Tb3 (Fe28−xCox) V1.0 (x=0, 3, 6) compounds

In this work, The magnetoelastic properties of polycrystalline samples of Tb₃ (Fe_28−xCo_x) V_1.0 (x=0, 3, 6) intermetallic compounds are investigated by means of linear thermal expansion and magnetostriction measurements in the temperature range of 77–515 K under applied magnetic fields up to 1.5 T. The linear thermal expansion increases with the Co content. The well-defined anomalies observed in the linear thermal expansion coefficients for Tb₃ (Fe_28−xCo_x) V_1.0 (x=0, 3, 6) compounds are associated with the magnetic ordering temperature for x=0 and spin reorientation temperatures for x=3, 6. Below transition temperatures, the value of the longitudinal magnetostriction (λ_Pa) at 1.6 T increases with Co content.     

Magnetic/structural phase diagram and enhanced giant magnetoresistance in Zn-doped antiperovskite compound Ga1−xZnxCMn3

The structural, magnetic and electrical transport properties of Zn-doped antiperovskite compounds Ga_1−xZn_xCMn₃ (0≤x≤0.30) have been investigated. After partial substitution of Zn for Ga, the Curie temperature increases monotonously and the ground antiferromagnetic (AFM)-ferromagnetic intermediate (FI) phase transition is gradually suppressed. With increasing the doping level x, the saturated magnetizations decreases gradually firstly for x≤0.20, then increases with increasing x. The electrical transport properties of Ga_1−xZn_xCMn₃ are studied at different magnetic fields. Enhanced giant magnetoresistance (GMR) was observed around the AFM-FI transition. With increasing x, the maximal values and peak widths of GMR increase. Particularly, for x=0.20, GMR reaches a maximum value of 75%, spanning a temperature range of 80 K at 50 kOe and displays the behavior of strongly depending on the magnetization history. The possible origins are discussed.     

Phase separation, ferromagnetism and magnetic irreversibility in La1−xSrxMn1−yFeyO3

Magnetic susceptibility, χ(T), is investigated in ceramic La_1−xSr_xMn_1−yFe_yO₃ (LSMFO) samples with x=0.3 and y=0.15−0.25. A ferromagnetic (FM) transition observed in LSMFO is accompanied with an appreciable decrease of the transition temperature with increasing y, which is connected to breaking of the FM double-exchange interaction by doping with Fe. Strong magnetic irreversibility, observed in low (B=10 G) field, gives evidence for frustration of the magnetic state of LSMFO. The FM transition, which is expanded with increasing B, is more pronounced in the samples with y=0.15-0.20 and broadens considerably at y=0.25, where the irreversibility is increased. Well above the transition, χ(T) exhibits a Curie-Weiss asymptotic behavior, yielding very large values of the effective Bohr magneton number per magnetic ion, incompatible with those of Mn or Fe single ions. At y=0.15 and 0.20 a critical behavior of χ⁻¹(T)∼(T/T_C−1)^γ in the region of the FM transition is characterized by influence of two different magnetic systems, a 3D percolative one with γ₌γ_p≈1.8 and T_C=T_C^(p), and a non-percolative 3D Heisenberg spin system, with γ=γ_H≈1.4 and T_C=T_C^(H), where T_C^(p)<T_C^(H). At y=0.25 the percolative contribution to the critical behavior of χ(T) is not observed. The dependence of χ on T and y gives evidence for phase separation, with onset already near the room temperature, leading to generation of nanosize FM particles in the paramagnetic host matrix of LSMFO. The ferromagnetism of LSMFO is attributable to percolation over the system of such particles and generation of large FM clusters, whereas the frustration is governed presumably by a system of smaller weakly-correlated magnetic units, which do not enter the percolative FM clusters.     

Magnetic properties and room-temperature magnetocaloric effect in the doped antipervoskite compounds Ga1−xAlxCMn3 (0≤x≤0.15)

We report the effects of Al doping on the structure, magnetic properties, and magnetocaloric effect of antiperovskite compounds Ga_1−xAl_xCMn₃ (0≤x≤0.15). Partial substitutions of Al for Ga enhance the Curie temperature (from 250 K for x=0.0 to 312 K for x=0.15) and the saturation magnetization. On increasing the doping level x, the maximum values of the magnetic entropy change (−ΔS_M) decreases while the temperature span of −ΔS_M vs. T plot broadens. Furthermore, the relative cooling power (RCP) is also studied. For 20 kOe, the RCP value tends to saturate at a high doping level (for x=0.12, 119 J/kg at 296 K). However, at 45 kOe, the RCP value increases quickly with increasing x (for x=0.15, 293 J/kg at 312 K). Considering the relatively large RCP and inexpensive raw materials, Ga_1−xAl_xCMn₃ may be alternative candidates for room-temperature magnetic refrigeration.     

Magnetic phase diagram simulation of La1−xCaxMnO3 system by using Monte Carlo, Metropolis algorithm and Heisenberg model

This work presents a critical temperature study of La_1−xCa_xMnO₃ manganites in bulk by means of Monte Carlo method thermal activated magnetic properties. The analysis was carried out for stoichiometries in the range of 0≤x≤1. The model is based on a three-dimensional classical Heisenberg-Hamiltonian involving the presence of Mn^3+eg, Mn^3+eg′ and Mn⁴⁺ ions, and their nearest neighbor interaction. For this modeling, simple cubic lattice samples of size L³, with L=6, 15 and 30 were used. The values of exchange parameters were determined by using LaMnO₃ (x=0), La_0.5Ca_0.5MnO₃ and CaMnO₃ (x=1) phases. Relationships between exchange parameters and anisotropy constants for different hole densities were found. Results of transition temperatures for each phase showed good agreement with experimental reports, especially for L=30 and L→∞.     

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.     

Room temperature magnetic entropy change and magnetoresistance in La0.70(Ca0.30−xSrx)MnO3:Ag 10% (x=0.0−0.10)

The magnetic and magnetocaloric properties of polycrystalline La_0.70(Ca_0.30−xSr_x)MnO₃:Ag 10% manganite have been investigated. All compositions are crystallized in single phase orthorhombic Pbnm space group. Both, the insulator–metal transition temperature (T^IM) and Curie temperature (T_c) are observed at 298 K for x=0.10 composition. Though both T^IM and T_c are nearly unchanged with Ag addition, the MR is increased. The MR at 300 K is found to be as large as 31% with magnetic field change of 1 T, whereas it reaches up to 49% at magnetic field of 3 T for the La_0.70Ca_0.20Sr_0.10MnO₃:Ag_0.10 sample. The maximum entropy change (ΔS_Mmax) at near its T_c (300.5 K) is 7.6 J kg⁻¹ K⁻¹ upon the magnetic field change of 5 T. The La_0.70Ca_0.20Sr_0.10MnO₃:Ag_0.10 sample having good MR (31%^1 T, 49%^3 T) and reasonable change in magnetic entropy (7.6 J kg⁻¹.K⁻¹, 5 T) at 300 K can be a potential magnetic refrigerant material at ambient temperatures.     

Magnetic and charge ordering properties of Bi0.6−xEuxCa0.4MnO3 (0.0≤x≤0.6)

We have studied structure, magnetic and transport properties of polycrystalline Bi_0.6−xEu_xCa_0.4MnO₃ (x=0.0, 0.1, 0.2, 0.3, 0.4, 0.5 and 0.6) perovskite manganites. Magnetic measurements show that the charge-ordering temperature (T_CO) decreases with increasing x up to x=0.4 and then slightly increases with further increasing x up to x=0.6. Further, the antiferromagnetic (AFM) ordering temperature (T_N) decreases with increasing x. At T<T_N a transition to metamagnetic glass like state is also seen. Eu doping also leads to enhancement in the magnetic moment and a concomitant decrease in resistivity up to x=0.2 and then an increase in resistivity up to x=0.5. We propose that the local lattice distortion induced by the size mismatch between the A-site cations and 6s² character of Bi³⁺ lone pair electron are responsible for the observed variation in physical properties.     

Magnetic properties and Griffiths singularity in La0.45Sr0.55 Mn1−xCoxO3

The magnetic properties and the Griffiths singularity were investigated in Mn-site doped manganites of La_0.45Sr_0.55Mn_1−xCo_xO₃ (x=0, 0.05, 0.10 and 0.15) in this work. The parent sample La_0.45Sr_0.55MnO₃ undergoes a paramagnetic-ferromagnetic transition at T_C=290 K and a ferromagnetic-antiferromagnetic transition at T_N=191 K. The doping of Co ions enhances the ferromagnetism and suppresses the antiferromagnetism. The enhanced ferromagnetism results from the fact that the Co doping enhances the Mn³⁺-Mn⁴⁺ double-exchange interaction and induces the Co²⁺-Mn⁴⁺ ferromagnetic superexchange interaction. Detailed investigation on the magnetic behavior above T_C exhibits that the Griffiths singularity takes place in this series of Mn-site doped compounds. The correlated disorder induced by the Co ionic doping, together with the phase competition from the ferromagnetic and the antiferromagnetic interactions among Mn ions, is responsible for the Griffiths singularity.     

Non-Fermi-liquid behavior in UCu4+xAl8−x compounds

We report on experimental studies of the Kondo physics and the development of non-Fermi-liquid scaling in UCu_4+xAl_8−x family. We studied 7 different compounds with compositions between x=0 and 2. We measured electrical transport (down to 65 mK) and thermoelectric power (down to 1.8 K) as a function of temperature, hydrostatic pressure, and/or magnetic field.Compounds with Cu content below x=1.25 exhibit long-range antiferromagnetic order at low temperatures. Magnetic order is suppressed with increasing Cu content and our data indicate a possible quantum critical point at x_cr≈1.15. For compounds with higher Cu content, non-Fermi-liquid behavior is observed. Non-Fermi-liquid scaling is inferred from electrical resistivity results for the x=1.25 and 1.5 compounds. For compounds with even higher Cu content, a sharp kink occurs in the resistivity data at low temperatures, and this may be indicative of another quantum critical point that occurs at higher Cu compositions.For the magnetically ordered compounds, hydrostatic pressure is found to increase the Néel temperature, which can be understood in terms of the Kondo physics. For the non-magnetic compounds, application of a magnetic field promotes a tendency toward Fermi-liquid behavior. Thermoelectric power was analyzed using a two-band Lorentzian model, and the results indicate one fairly narrow band (10 meV and below) and a second broad band (around hundred meV). The results imply that there are two relevant energy scales that need to be considered for the physics in this family of compounds.     

Magnetic and related properties of the solid solution CeCuxGa4−x

Physical properties of polycrystalline samples of CeCu_xGa_4−x (x = 0.2–1.4), crystallizing in the tetragonal BaAl₄-type structure (space group I 4/mmm), were studied by means of X-ray powder diffraction, magnetization, specific heat, electrical resistivity and magnetoresistivity measurements in wide temperature and magnetic fields ranges. The unit-cell volume of the system was found to decrease with increasing x (in total by about 4%) but the magnetic moments of Ce³⁺ ions remain localized in the whole x-range studied. The alloys exhibit ferromagnetic order at low temperatures, which manifests itself as distinct and relatively sharp anomalies in all the temperature characteristics measured. The ordering temperature decreases with increasing the Cu content from 5.5(1) K for x = 0.2 down to 1.35(5) K for x = 1.4, and the electrical transport properties of the system show some features characteristic of Kondo lattices.     

Magnetic and magnetoelastic properties of Zn-doped cobalt-ferrites—CoFe2−xZnxO4 (x=0, 0.1, 0.2, and 0.3)

Cobalt-ferrite (CoFe₂O₄) based materials are suitable candidates for magnetomechanical sensor applications owing to a strong sensitivity of their magnetostriction to an applied magnetic field. Zn-doped cobalt-ferrites, with nominal compositions CoFe_2−xZn_xO₄ (x=0–0.3), were synthesized by auto-combustion technique using Co- , Fe- , and Zn-nitrate as precursors. X-ray spectra analysis and Transmission electron microscopy studies revealed that the as-prepared powders were comprised of nano-crystalline (∼25–30 nm) cubic-spinel phase with irregularly-shaped grains morphology along with minor impurity phases. Calcination (800 °C for 3 h) of the precursor followed by sintering (1300 °C for 12 h) resulted in a single phase cubic-spinel structure with average grain size ∼2–4 μm, as revealed from scanning electron micrographs. The magnitude of coercive field decreases from ∼540 Oe for x=0 to 105 Oe for x=0.30. Saturation magnetization initially increases and peaks to ∼87 emu/g for x=0.2 and then decreases. The peak value of magnetostriction monotonically decreases with increasing Zn content in the range 0.0–0.3; however the piezomagnetic coefficient (dλ/dH) reaches a maximum value of 105×10⁻⁹ Oe⁻¹ for x=0.1. The observed variation in piezomagnetic coefficient in the Zn substituted cobalt ferrite is related to the reduced anisotropy of the system. The Zn-doped cobalt-ferrite (x=0.1) having high strain derivative could be a potential material for stress sensor application.     

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.     

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.