Evidence of glassy ferromagnetic phase and kinetic arrest of electronic phase in Sm0.35Pr0.15Sr0.5MnO3 manganites

The effect of doping of rare earth Pr³⁺ ion as a replacement of Sm³⁺ in Sm_0.5Sr_0.5MnO₃ is investigated. Temperature dependent dc and ac magnetic susceptibility, resistivity, magnetoresistance measurements on chemically synthesized (Sm_0.5−xPr_x)Sr_0.5MnO₃ show various unusual features with doping level x=0.15. The frequency independent ferromagnetic to paramagnetic transition at higher temperature (∼191 K) followed by a frequency dependent reentrant magnetic transition at lower temperature (∼31 K) has been observed. The nature of this frequency dependent reentrant magnetic transition is described by a critical slowing down model of spin glasses. From non-linear ac susceptibility measurements it has been confirmed that the finite size ferromagnetic clusters are formed as a consequence of intrinsic phase separation, and undergo spin glass-like freezing below a certain temperature. There is an unusual observation of a 2nd harmonic peak in the non-linear ac susceptibility around this reentrant magnetic transition at low temperature (∼31 K). Arrott plots at 10 and 30 K confirm the existence of glassy ferromagnetism below this low temperature reentrant transition. Electronic- and magneto-transport measurements show a strong magnetic field—temperature history dependence and strong irreversibility with respect to the sweeping of magnetic field. These results are attributed to the effect of phase separation and kinetic arrest of the electronic phase in this phase separated manganite at low temperatures.     

Structural, magnetic and magnetotransport behavior of La0.7SrxCa0.3−xMnO3 compounds

A systematic investigation of the structural, magnetic and electrical properties of a series of nanocrystalline La_0.7Sr_xCa_0.3−xMnO₃ materials, prepared by high energy ball milling method and then annealed at 900 °C has been undertaken. The analysis of the XRD data using the Win-metric software shows an increase in the unit cell volume with increasing Sr ion concentration. The La_0.7Sr_xCa_0.3−xMnO₃ compounds undergo a structural orthorhombic-to-monoclinic transition at x=0.15. Electric and magnetic measurements show that both the Curie temperature and the insulator-to-metal transition temperature increase from 259 K and 253 K correspondingly for La_0.7Ca_0.3MnO₃ (x=0) to 353 K and 282 K, respectively, for La_0.7Sr_0.3MnO₃ (x=0.3). It is argued that the larger radius of Sr²⁺ ion than that of Ca²⁺ is the reason to strengthen the double-exchange interaction and to give rise to the observed increase of transition temperatures. Using the phenomenological equation for conductivity under a percolation approach, which depends on the phase segregation of ferromagnetic metallic clusters and paramagnetic insulating regions, we fitted the resistivity versus temperature data measured in the range of 50-320 K and found that the activation barrier decreased with the raising Sr²⁺ ion concentration.     

Electron-doped Sm1−xSrxMnO3 perovskite manganites: Crystal and magnetic structures and physical properties

We present the results of a study of electron-doped Sm_1−xSr_xMnO₃ (x>0.5) perovskite manganites by combining high-resolution neutron powder diffraction with measurements of resistivity, magnetization and magnetic susceptibility. Although investigated Sm_0.45Sr_0.55MnO₃ and Sm_0.37Sr_0.63MnO₃ compounds belonging to the same phase diagram area differ significantly in the strontium content, they are homogeneous antiferromagnetic (AF) insulators and do not exhibit CMR. They have different crystallographic symmetries (orthorhombic Pbnm and tetragonal I4/mcm, respectively) in the entire temperature range under study (1.5-288 K), differ in the type of spin ordering at low temperatures (AF-A and AF-C), are characterized by different orbital polarizations (d_x²_−y² and d_3z²_−r²), and possess two- and one-dimensional magnetic properties, respectively. The lack of magnetoresistance for these compositions is explained by the lack of coexisting magnetic phases involving double exchange ferromagnetism, in contrast to what is observed for the magnetoresistive Sm_1−xSr_xMnO₃ compounds, that is with x?0.52.     

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.     

Double metal-insulator peaks and effect of Sm substitution on magnetic and transport properties of hole-doped La0.85Ag0.15MnO3

La_0.85−xSm_xAg_0.15MnO₃ (x=0−0.2) ceramics were prepared using the conventional solid-state synthesis method to investigate the effect of Sm³⁺ substitution on magnetic and electrical transport properties. Magnetic susceptibility versus temperature measurements showed all samples exhibit ferromagnetic to paramagnetic transition with Curie temperature, T_c decreasing from 283 K (x=0) to 164 K (x=0.2) with increasing Sm³⁺. The observed slope in susceptibility, χ′ versus temperature curves below T_c indicates the possible presence of FM and AFM phases in the metallic region. In addition, a deviation from the Curie-Weiss law above T_c in 1/χ′ versus T curves indicates the existence of a Griffith's phase in the x=0.05−0.2 samples due to the Sm³⁺ ion substitution. The Griffith temperature, T_G was found to decrease from 295 K (x=0.05) to 229 K (x=0.2). Electrical resistivity measurements of the samples in zero field showed transition from metallic behavior to insulating behavior as the temperature was increased. For x=0, two metal-insulator, MI transition peaks were observed at T_p1=282 K and at T_p2=250 K. Both peaks shifted to lower temperatures with the increase in Sm³⁺. The relative resistivity of the first peak to the second peak decreases with increasing Sm³⁺ for x>0.05 while at x=0.2 the T_p1 peak was strongly suppressed. Magnetoresistance, MR was observed to weaken with Sm³⁺ substitution. The metallic region of the ρ(T) curve of the x=0−0.15 samples was fitted to the model of electron-electron and electron-magnon scattering while the insulating region was fitted to the variable range hopping, VRH model. The resistivity behavior indicated that the substitution of Sm³⁺ weakened the double exchange process and enhanced the Jahn-Teller effect. Our results indicated that the T_p1 peak is strongly related to the double-exchange mechanism while the T_p2 peak is suggested to originate from magnetic inhomogeneity.     

The structure and magnetotransport properties of La2/3Sr1/3MnO3/Ba(La)TiO3 composites

The effect of Ba(La)TiO₃ doping on the structure and magnetotransport properties of La_2/3Sr_1/3MnO₃(LSMO)/xBa(La)TiO₃ (x=0.0, 1.0, 5.0 mol%) have been investigated. The X-ray diffraction patterns and microstructural analysis show that BaTiO₃ and LSMO phases exist independently in BaTiO₃-doped composites. The metal-insulator transition temperature (T_MI) decreases whereas the maximum resistivity increases very quickly by the increase of BaTiO₃ doping level. The partial substitution of Ba by La(0.35 mol%) results in a decrease in resistivity of LSMO/xBa(La)TiO₃ composites. Magnetoresistance of BaTiO₃-doped composites decreases monotonously in the temperature range 200-400 K in a magnetic field of 5 T, which is completely different from that of LSMO compound. The value of MR decreases at low field (H<1 T) and increases at high fields (H>1 T) with increasing the BaTiO₃ doping level at low temperatures below 280 K. These investigations reveal that the magnetotransport properties of LSMO/xBa(La)TiO₃ composites are dominated by spin-dependent scattering and tunneling effect at the LSMO/BaTiO₃/LSMO magnetic tunnel junction.     

Enhancement of magnetoresistances at room temperature in YSZ doping La0.67Sr0.33MnO3 system

The temperature dependence of the resistance of composite samples (1−x)La_0.67Sr_0.33MnO₃+xYSZ with different YSZ doping level x was investigated at magnetic fields 0-3 T, where YSZ represents yttria-stabilized zirconia. Results show that the YSZ dopant does not only adjust the metal-insulator transition temperature, but also increases the magnetoresistance effect. With increase of YSZ doping level for the range of x<2%, the metal-insulator transition temperature values T_P of the composites decrease, but T_P increases with increase of x further for the range of x>2%. Meanwhile, in the YSZ-doped composites, a broad metal-insulator transition temperature region was found at zero and low magnetic field, which results in an obvious enhanced magnetoresistance in the temperature range 10-350 K. Specially, a larger magnetoresistance value was observed at room temperature at 3 T, which is encouraging with regard to the potential application of magnetoresistance materials.     

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.     

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).     

Enhanced low-field-magnetoresistance and electro-magnetic behavior of La0.7Sr0.3MnO3/BaTiO3 composites

We report the structural, magentoresistance and electro-magnetic properties of ferromagnet–ferroelectric–type (1−x)La_0.7Sr_0.3MnO₃/xBaTiO₃ (with x=0.0%, 3.0%, 6.0%, 12%, 15.0% and 18.0%, in wt%) composites fabricated through a solid-state reaction method combined with a high energy milling method. The insulator–metal transition temperature shifts to a lower temperature and resistivity increases while the feromagnetic–paramagnetic transition temperature remains almost unchanged with the increase of BaTiO₃ content. Magnetoresistance of the composites at an applied magnetic field H=3 kOe is enhanced in the wide temperature ranges with the introduction of BaTiO₃, which could be explained by the enhanced spin polarized tunneling effect induced by the introduction of BaTiO₃. The low-field magnetoresistance of the composite is analyzed in the light of a phenomenological model based on the spin polarized tunneling at the grain boundaries. Furthermore, the temperature dependence of resistivity for this series has been best-fitted by using the adiabatic small polaron and variable range hopping models. These models may be used to explain effect of BTO on the electronic transport properties on high temperature paramagnetic insulating region.     

Structural,magnetic and electrical properties of Co1−xZnxFe2O4 synthesized by co-precipitation method

Nanoparticles of Co_1−xZn_xFe₂O₄ with stoichiometric proportion (x) varying from 0.0 to 0.6 were prepared by the chemical co-precipitation method. The samples were sintered at 600 °C for 2 h and were characterized by X-ray diffraction (XRD), low field AC magnetic susceptibility, DC electrical resistivity and dielectric constant measurements. From the analysis of XRD patterns, the nanocrystalline ferrite had been obtained at pH=12.5–13 and reaction time of 45 min. The particle size was calculated from the most intense peak (3 1 1) using the Scherrer formula. The size of precipitated particles lies within the range 12–16 nm, obtained at reaction temperature of 70 °C. The Curie temperature was obtained from AC magnetic susceptibility measurements in the range 77–850 K. It is observed that Curie temperature decreases with the increase of Zn concentration. DC electrical resistivity measurements were carried out by two-probe method from 370 to 580 K. Temperature-dependent DC electrical resistivity decreases with increase in temperature ensuring the semiconductor nature of the samples. DC electrical resistivity results are discussed in terms of polaron hopping model. Activation energy calculated from the DC electrical resistivity versus temperature for all the samples ranges from 0.658 to 0.849 eV. The drift mobility increases by increasing temperature due to decrease in DC electrical resisitivity. The dielectric constants are studied as a function of frequency in the range 100 Hz–1 MHz at room temperature. The dielectric constant decreases with increasing frequency for all the samples and follow the Maxwell–Wagner's interfacial polarization.     

Discussion again of the magnetic and transport property of Ag-doped LaMnO3

Samples La_1−aAg_aMnO₃ (0.05?a?0.50) were sol–gel fabricated. A part of Ag was found to dissociate and run off the samples in sintering process when sintering temperature exceeds 700 °C, resulting in a composite of La_1−xAg_xMnO₃ and MnO₂/Mn₂O₃. The magnetic and transport properties of the composite have been studied. The sample with the nominal composition La_0.7Ag_0.3MnO₃ was found to show the greatest magnetoresistance in the sample group. Detailed analysis on average Mn valence reveals a composite of (La_0.985Ag_0.015MnO₃)_0.776[(MnO₂)_0.590(Mn₂O₃)_0.410]_0.224. Its MR ratio at room temperature exceeds 24% under a field of 1.8 T. A conductivity leap has been observed around a=0.30. It suggests a kind of field-induced fluctuation in percolation in the samples investigated.     

Effect of Cr doping on the magnetic and electrical transport properties of charge-ordered Bi0.5Ca0.5MnO3

An experimental study on the magnetic and electrical transport properties of the manganites Bi_0.5Ca_0.5Mn_1−xCr_xO₃ (BCMCO) (0≤x≤0.12) is carried out. The results show that Cr doping can suppress the charge-ordering transition, favoring the ferromagnetic clusters. For x=0.12, the charge-ordering transition disappears but a very broad paramagnetic-ferromagnetic-like transition is detected at the Curie temperature T_C=72.6 K. It is caused by phase separation or coexistence of the charge-ordering and ferromagnetic phase. Moreover, the critical Cr content to destroy charge ordering phase in BCMCO does not match the general monotonous tendencies shown by Cr-doped Re_0.5Ca_0.5MnO₃ (Re-rare-earth). These differences are ascribed to the fact that the ground state in BCMCO differs markedly from the ferromagnetic metallic phase in Cr-doped Re_0.5Ca_0.5MnO₃ compounds.     

Large enhancement of room temperature magnetoresistance in Ag-added La0.67(Ca0.65Ba0.35)0.33MnO3

The electrical and magnetoresistant properties of La_0.67(Ca_0.65Ba_0.35)_0.33MnO₃/Ag_x (abbreviated by LCBMO/Ag_x) have been studied. The results show that Ag addition causes a decrease of resistivity dramatically and especially induces a large enhancement of room temperature magnetoresistance (MR). The room temperature MR ratio for x=0.27 sample in 10 kOe magnetic field is 41%, almost 20 times larger than that for x=0 sample. This enhancement is related to that the Curie temperature (T_c) of the sample is near room temperature, as well as the significant reduction of resistivity. The good fits of experimental results for x=0.27 sample to Brillouin function indicate that the MR behavior in the Ag added LCBMO is induced by the spin-dependent hopping of the electrons between the spin clusters, which is an intrinsic property of the CMR materials.     

Effect of monovalent metal substitution on the magnetocaloric effect of perovskite manganites Pr0.5Sr0.3M0.2MnO3 (M=Na,Li, K and Ag)

The influence of monovalent doping on the magnetocaloric effect (MCE) and refrigerant capacity or relative cooling power (RCP) of Pr_0.5Sr_0.3M_0.2MnO₃ (M=Na, Li, K and Ag) materials has been investigated. A large magnetocaloric effect was inferred over a wide range of temperature around the second order paramagnetic–ferromagnetic transition. The maximum magnetic entropy changes (ΔS_M) reached 1.8, 2.2, 1.6 and 2.1 J/kg K and the relative cooling power (RCP) approached 58.9, 59.3, 69.6 and 54.6 J/kg for Na, Li, K and Ag doped materials in the magnetic change of 15 kOe, respectively. According to the results determined by the Maxwell relation, the magnetic entropy change fits well with the Landau theory of phase transition above T_C for Pr_0.5Sr_0.3Li_0.2MnO₃. The large magnetic entropy change induced by low magnetic field suggested that these materials are beneficial for practical applications.     

Electroresistive and magnetoresistive properties of Nd0.7Sr0.3MnO3 after quenching under pressure of 9 GPa

Polycrystalline Nd_0.7Sr_0.3MnO₃ was quenched from 1300 K to 300 K and 80 K after it had been subjected to a high quasihydrostatic pressure of 9 GPa. Such high pressure and high temperature treatment (HPT) results in significant changes of the crystallochemical parameters—Mn-O lengths and Mn-O-Mn angles within unchanged lattice symmetry of the Pnma-type. A strong increase of the resistivity and a large decrease of the FM-PI transition temperature were detected for the Nd_0.7Sr_0.3MnO₃ HPT treated samples. The intrinsic characteristic T_MI(T_C) (T_MI is the metal-insulator and T_C is the ferromagnetic-paramagnetic transition temperature) correlates with the change of the Mn-O(1)-Mn angle, which is consistent with the double exchange model of the ferromagnetic metallic state in manganites. Remarkable electroresistive (ER) and magnetoresistive (MR) effects appear after HPT treatment, which were not present in the starting Nd_0.7Sr_0.3MnO₃ sample. The structure sensitive properties such as resistivity, MR and ER effects correlate with the change of the nanograin sizes after HPT treatment. Nonlinear current-voltage characteristics showing a hysteresis appear for HPT treated samples at low temperatures. The transport in granular Nd_0.7Sr_0.3MnO₃ samples is likely defined by spin-dependent scattering of charge carriers inside the ferromagnetic metallic grains with embedded small charged isolating islands and by jumping over charged insulating barriers at the intergrain boundaries, which can be strongly affected by the external electric and magnetic fields.     

Ferromagnetic-to-antiferromagnetic transition in (Hf1−xTix)Fe2 intermetallic compounds induced by geometrical frustration of the Fe(2a) sites

The ferromagnetic-to-antiferromagnetic transition in the hexagonal (Hf_1−xTi_x)Fe₂ (0?x?1) intermetallic compounds has been investigated by ⁵⁷Fe Mössbauer spectroscopy. At 10 K, the transition occurs within rather narrow concentration limits, around x=0.55–0.65. We found that the key factor governing the unexpected quick change of the magnetic structure is the magnetic frustration of the Fe(2a) sites. The magnetic frustration is caused by the noncollinearity of the Fe(6h) magnetic sublattice. The noncollinearity arises from the rotation of the magnetic moments due to the competition between the ferromagnetic exchange interactions and the antiferromagnetic Fe(6h)–Ti–Fe(6h) interaction. In the compounds with x=0.4–0.6, the temperature transitions to the antiferromagnetic state are observed. As an example, the Hf_0.4Ti_0.6Fe₂ compound is completely antiferromagnetic above 200 K.     

Study on the phase separation of La0.7Sr0.3MnO3 nanoparticles by electron magnetic resonance

In this work, the technique of electron magnetic resonance (EMR) is used to measure the magnetic resonant spectra of La_0.7Sr_0.3MnO₃ nanoparticles synthesized by sol–gel routes with three different gelation agents (S1: Urea+citric acid; S2: citric acid, and S3: Urea+tri-sodium citrate). The purpose of this study is to investigate the influence of synthesis conditions on the magnetic properties of nanoparticles. Our ESR results show that Curie temperatures of La_0.7Sr_0.3MnO₃ nanoparticles with different gelation agents are slightly different (T_c∼340 to 360 K) and possess both paramagnetic (PM) and ferromagnetic (FM) phases in the temperature below T_c. Besides, a sharp FM–PM transition indicates that the combined agent of Urea+tri-sodium citrate creates a better quality in CMR nanomagnets.     

Analysis of low temperature specific heat in Nd0.5Sr0.5MnO3 and R0.5Ca0.5MnO3 (R=Nd,Sm, Dy and Ho) compounds

We report on the specific heat C(T) of doped manganites Nd_0.5Sr_0.5MnO₃, Nd_0.5Ca_0.5MnO₃, Sm_0.5Ca_0.5MnO₃, Dy_0.5Ca_0.5MnO₃ and Ho_0.5Ca_0.5MnO₃ in the temperature range 2?T?300 K using modified rigid ion model (MRIM). The present specific heat results are in general satisfactory agreement with experimental data except at very low temperatures (i.e. T?12 K). Also a sharp peak observed in the experimental results for these compounds around 5 K could not be revealed by our computed results as they arise due to Schottky-like anomaly. Besides, we have reported the cohesive and the thermal properties of these compounds. The results obtained by us are discussed in detail.     

Effects of ZnO film thickness on electrical and magnetoresistance characteristics of La0.8Sr0.2MnO3/ZnO heterostructures

The La_0.8Sr_0.2MnO₃/ZnO heterostructures with different thicknesses of ZnO films are fabricated by using RF magnetron sputtering technique. The heterojunctions exhibit excellent rectifying properties at 300 K. At low temperatures the temperature dependent junction resistance exhibits a metal-insulator transition like behavior. A magnetic field strongly impacts on electrical characteristics of La_0.8Sr_0.2MnO₃/ZnO p-n junctions, i.e., depressing the junction resistance greatly and driving the metal-insulator transition temperature (T_MI) towards higher temperatures. Large magnetoresistance is observed below T_MI, and it increases with increasing magnetic field and almost saturates at 5 T, i.e., above −90% at 100 K and 5 T.