Magnetic properties of the charge ordered Nd0.75Na0.25MnO3

Nd_0.75Na_0.25MnO₃ polycrystalline ceramic is prepared via sol-gel process and its magnetic properties and electron spin resonance (ESR) spectra have been investigated experimentally. As the compound is cooled from room temperature, a charge-ordered state first develops below 170 K. A high magnetic field melts the charge ordered state and stabilizes a ferromagnetic (FM) state below 170 K. A field induced transition, analogous to a spin flip transition, is observed between 40 and 170 K. The critical temperature for spin flip increases with increasing temperature. Below 130 K, the compound tends to be intrinsically inhomogeneous, i.e. FM clusters and paramagnetic domains coexist in this system at least, which is confirmed by ESR measurements. When the external magnetic field is zero, long range FM interaction is not developed in this system; however, a tendency of re-entrant FM transition is observed in this compound.     

Magnetic dynamics of charge ordered Nd0.80Na0.20MnO3 compound

The magnetic dynamics of charge ordered Nd_0.8Na_0.2MnO₃ compound was studied by measuring the temperature variation of magnetization for different magnetic fields up to 7 T and, the field variation of magnetization at different temperatures down to 5 K. This sample exhibits a charge-ordering transition at 180 K, followed by a weak ferromagnetic (FM) transition at around 100 K and a spin glass like transition below 40 K. Suppression of charge-ordering and spin glass like transition and increase in FM T_C were observed with an increase in magnetic field. A reversible metamagnetic transition above a threshold field (H_f) of 4.5 T was observed at 130 K, followed by a saturation magnetization of 3.2 μ_B/f.u. However at 5 K, an irreversible field induced first order phase transition from charge ordered state to FM state was observed at H_f=5 T. For comparison, the temperature and field variations of magnetization were studied on a FM compound from the same series with the composition Nd_0.90Na_0.10MnO₃. A clear FM transition with a T_C of 113 K and a saturation magnetization of 4.3 μ_B/f.u was observed.     

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.     

Effect of Y-doping on the magnetic and charge orderings in Nd2/3Ca1/3MnO3

The shifts of the magnetic and charge ordering transition temperatures caused by Nd substitution for Y in Nd_2/3Ca_1/3MnO₃ CMR narrow-band perovskite manganite have been studied. At low temperatures, three different long-range magnetic orderings consistent with a phase separation scenario have been observed in the doped compound (Nd_0.9Y_0.1)_2/3Ca_1/3MnO₃ by neutron-diffraction study: the antiferromagnetic orderings of PCE and DE types existing below ∼110 and ∼60 K, respectively, and the ferromagnetic one of B type existing below ∼42. Magnetic phase transformations temperatures as well as those of charge ordering have been found to be structural-dependent. Y-doping leads to the decrease of the anisotropy of the orthorhombic Pnma crystal lattice b/√2c, which causes a decrease of the indirect exchange parameters in the system and thus a decrease in the magnetic transformation temperatures for 20-30 K in the doped compound. Doping leads as well to the higher level of the coherent Jahn-Teller distortions of the MnO₆ octahedra in the 200-300 K temperature region, which results in the increase of the charge ordering temperature for ∼80 K.     

Effect of Ca doping on the magnetic properties of Nd0.5Sr0.5MnO3 studied by electron spin resonance

The magnetic properties of Ca-doped Nd_0.5Sr_0.5MnO₃ have been studied by electron spin resonance (ESR) and dc magnetization measurements. The antiferromagnetic order and charge order are found to occur separately at T_N=200 K and T_co=150 K, respectively. Compared to the undoped Nd_0.5Sr_0.5MnO₃, the ferromagnetic correlations are suppressed by doping of the small Ca²⁺ ion. In addition, the antiferromagnetic transition temperature is enhanced to 200 K, which can be explained by an increase of superexchange interaction between Mn³⁺ and Mn⁴⁺ ions as their distance decreases.     

Metastable states in phase separated electron doped Sm0.15Ca0.85MnO3

In order to study the mechanism behind the phase separation scenario in the Sm_0.15Ca_0.85MnO₃ compound, magnetization and resistivity measurements have been carried out in pulsed magnetic fields up to 50 T at temperatures 4.2 K<T<200 K. It is found that external magnetic field causes a collapse of a C-type AFM (P2₁/m) phase resulting in field-induced insulator-metal transition, which is irreversible below T₁=75 K. In zero field the content of a G-type phase in the mixed C-G state can vary from 10 to 17% at T=10 K. A set of metastable states with different volume ratios of G-type to C-type phases is observed below T₁ depending on the history of the sample. The obtained results indicate that the phase separation plays a dominant role for the electric and the magnetic properties of this material.     

Magnetic,electrical transport and electron spin resonance studies of Fe-doped manganite LaMn0.7Fe0.3O3+δ

We have investigated the magnetic, electrical transport and electron spin resonance (ESR) properties of polycrystalline Fe-doped manganite LaMn_0.7Fe_0.3O_3+δ prepared by sol–gel method. A typical cluster-glass feature is presented by DC magnetization and AC susceptibility measurements and a sharp but shallow memory effect was observed. Symmetrical Lorentzian lines of the Mn/Fe spectra were detected above 120 K, where the sample is a paramagnetic (PM) insulator. When the temperature decreases from 120 K, magnetic clusters contributed from ferromagnetic (FM) interaction between Mn³⁺ and Mn³⁺/Fe³⁺ ions develop and coexist with PM phase. At lower temperature, these FM clusters compete with antiferromagnetic (AFM) ones between Fe³⁺ ions, which are associated with a distinct field-cooled (FC) effect in characteristic of cluster-glass state.     

The relation between magnetoresistance and magnetocaloric effect in La0.85Ag0.15MnO3 manganite

We present the temperature dependence of La_0.85Ag_0.15MnO₃ resistivity in the temperature interval between 77 and 340 K and magnetic fields up to 26 kOe. We offer a method of separating tunnel magnetoresistance from total magnetoresistance. A change in both the magnetic entropy, which is caused by the magnetocaloric effect (MCE), and the magnetoresistance are shown to be connected through a simple relationship to La_0.85Ag_0.15MnO₃.     

Electronic and magnetic phase transitions in (Sm0.65Sr0.35)MnO3 induced by temperature and magnetic field

Temperature (4.2–260 K) and magnetic field (0–50 kOe) dependencies of the DC electrical resistance, DC magnetization, and AC magnetic susceptibility of (Sm_0.65Sr_0.35)MnO₃ prepared from high purity components have been studied. (Sm_0.65Sr_0.35)MnO₃ undergoes a temperature-induced transition between low-temperature ferromagnetic metallic and high-temperature paramagnetic insulating-like states. A magnetic field strongly affects this transition resulting in a metallic state and “colossal” magnetoresistance in the vicinity of the metal↔insulator transition. Magnetic and electric properties of (Sm_0.65Sr_0.35)MnO₃ are different compared to those reported earlier for similar composition, which is attributable to the purity of the starting materials and/or different process of synthesis. The character of phase transformations observed in (Sm_0.65Sr_0.35)MnO₃ is compared to that reported for Gd₅(Si_xGe_4−x) intermetallic alloys with a true first order phase transition.     

Magnetic properties of the novel nanocomposite (Zn0.15Ni0.85Fe2O4)0.15/(SiO2)0.85 at room temperature

The value of the effective magnetic anisotropy constant of the ferrimagnetic nanoparticles Zn_0.15Ni_0.85Fe₂O₄ embedded in a SiO₂ silica matrix, determined through ferromagnetic resonance (FMR), is much higher than the magnetocrystalline anisotropy constant. The higher value of the anisotropy constant is due to the existence of surface anisotropy. However, even if the magnetic anisotropy is high, the ferrimagnetic nanoparticles with a 15% concentration, which are isolated in a SiO₂ matrix, display a superparamagnetic (SPM) behavior at room temperature and at a frequency of the magnetization field equal to 50 Hz. The FMR spectrum of the novel nanocomposite (Zn_0.15Ni_0.85Fe₂O₄)_0.15/(SiO₂)_0.85, recorded at room temperature and a frequency of 9.060 GHz, is observed at a resonance field (B_0r) of 0.2285 T, which is substantially lower than the field corresponding to free electron resonance (ESR) (0.3236 T). Apart from the line corresponding to the resonance of the nanoparticle system, the spectrum also contains an additional weaker line, identified for a resonance field of ∼0.12 T, which is appreciably lower than B_0r. This line was attributed to magnetic ions complex that is in a disordered structure in the layer that has an average thickness of 1.4 nm, this layer being situated on the surface of the Zn_0.15Ni_0.85Fe₂O₄ nanoparticles that have a mean magnetic diameter of 8.9 nm.     

Magnetic resonances spectroscopy of nanosize particles La0.7Sr0.3MnO3

Using a co-precipitation method, perovskite-type manganese oxide La_0.7Sr_0.3MnO₃ nanoparticles (NPs) with particle size 12 nm were prepared. Detailed studies of both ⁵⁵Mn nuclear magnetic resonance and superparamagnetic resonance spectrum, completed by magnetic measurements, have been performed to obtain microscopic information on the local magnetic structure of the NP. Our results on nuclear dynamics provide direct evidence of formation of a magnetically dead layer, of the thickness ≈2 nm, at the particle surface. Temperature dependences of the magnetic resonance spectra have been measured to obtain information about complex magnetic properties of La_0.7Sr_0.3MnO₃ fine-particle ensembles. In particular, electron paramagnetic resonance spectrum at 300 K shows a relatively narrow sharp line, but as the temperature decreases to 5 K, the apparent resonance field decreases and the line width considerably increases. The low-temperature blocking of the NPs magnetic moments has been clearly observed in the electron paramagnetic resonances. The blocking temperature depends on the measuring frequency and for the ensemble of 12 nm NPs at 9.244 GHz has been evaluated as 110 K.     

Magneto-transport and ferromagnetic resonance studies of polycrystalline La0.6Pb0.4MnO3 thin films

To understand the nature of grain boundaries in polycrystalline materials, magneto-transport and ferromagnetic resonance measurement have been performed in polycrystalline La_0.6Pb_0.4MnO₃ (LPMO) thin films prepared by pulsed laser deposition. Films are found to undergo a semiconductor to metal transition at 230 K and re-enter into the semiconducting state below 130 K. Microwave absorption measurements carried out as function of applied field show two components of resonant absorption signal. First component is in accordance with ferromagnetic transition of grains at Curie temperature and the second component shows antiferromagnetic transition of grain boundaries at 160 K. An additional non-resonant absorption signal centered at zero field has also been observed that supports transition from conducting to insulating grain boundaries at ∼160 K. Further, temperature dependence of resistance in semiconducting state at low temperatures is in accordance with coulomb blockade model indicating insulating nature of AFM grain boundaries.     

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.     

Structural first-order transformation in La2/3Ba1/3MnO3: ESR study

We have studied by the electron-spin resonance (ESR) and static magnetic field techniques, the La_2/3Ba_1/3MnO₃ perovskite, which was previously shown to exhibit a martensitic phase transformation in the vicinity of T_s∼200 K [Physical Review B 68, 054109 (2003)], leading to its structural phase-segregated state. Resonant absorptions reveal that in the temperature interval from 100 K to 340 K the compound represents a mixture of two ferromagnetic phases possessing different magnetizations, in varying proportions depending on the temperature, and a small amount of a paramagnetic phase. The results agree well with the previous neutron diffraction study. Applied in the ESR experiments, magnetic fields (2–6 kOe) strongly affect the magnetization curves: even magnetic field as high as 700 Oe modifies the anomaly in the phase transformation region and removes the difference between the zero-field cooled and field-cooled magnetization curves, which implies that the difference in the magnetic susceptibility of the coexisting phases is small and the magnetic domain configuration can be easily changed.     

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.     

Magnetic resonance in crystalline La0.9Ca0.1MnO3: Comparative study of bulk and nanometer-sized samples

X-band electron magnetic resonance (EMR) measurements were done at 115?T?600 K on bulk and nanometer size-grain powder single-crystalline samples of La_0.9Ca_0.1MnO₃, in order to study an impact of structural inhomogeneity on magnetic ordering. For the nano-crystal sample, two superimposed EMR lines are observed below 240 K, while for bulk-crystal one, a second line emerges in narrow temperature interval below 130 K. Temperature dependences of resonance field and line width of the main and the secondary line are drastically different. EMR data and complementary magnetic measurements of bulk-crystal sample reveal mixed-magnetic phase, which agrees with the published phase diagram of bulk La_1−xCa_xMnO₃. In a marked contrast, the same analysis for nano-crystal sample shows two phases one of which is definitely ferromagnetic (FM) and other is likely such, or super paramagnetic. The data obtained are interpreted in terms of very different magnetic ground states in the two samples, that is attributed to different randomness of the indirect FM exchange interactions mediated by bound holes.     

The role of iron in the formation of the magnetic structure and related properties of La0.8Sr0.2Co1−xFexO3 (x=0.15, 0.2, 0.3)

La_0.8Sr_0.2Co_1−xFe_xO₃ (x=0.15, 0.2, 0.3) samples were studied by means of AC magnetic susceptibility, magnetization, magnetoresistance and ⁵⁷Fe Mössbauer spectrometry. Iron was found to take on a high spin 3d^5−α electronic state in each of the samples, where α refers to a partly delocalized 3d electron. The compounds were found to exhibit a spin-cluster glass transition with a common transition temperature of ∼53 K. The spin-cluster glass transition is visualized in the ⁵⁷Fe Mössbauer spectra as the slowing down of magnetic relaxation below ∼70 K, thereby showing that iron takes part in the formation of the glassy magnetic phase. The paramagnetic-like phase found at higher temperatures is identified below T_c≈195 K as being composed of weakly interacting, magnetically ordered nanosized clusters of magnetic ions in part with a magnetic moment oriented opposite to the net magnetic moment of the cluster. For each of the samples a considerable low-temperature negative magnetoresistance was found, whose magnitude in the studied range decreases with increasing iron concentration. The observed results obtained on the present compounds are qualitatively explained assuming that the absolute strengths of magnetic exchange interactions are subject to the relation ∣J_Co–Co∣<∣J_Fe–Co∣<∣J_Fe–Fe∣.     

Magnetic and magnetocaloric properties of Pr0.6−xEuxSr0.4MnO3 manganese oxides

Studies of the structural, magnetic and magnetocaloric properties of polycrystalline Pr_0.6−xEu_xSr_0.4MnO₃ (0≤x≤0.15) perovskite manganites were carried out. Substitution for praseodymium with europium, with smaller ionic radius, induces local distortion in the 〈Mn–O–Mn〉 bonds and consequently causes a random distribution in the magnetic exchange interactions. The competition between magnetic interactions leads to the appearance of an inhomogeneous magnetic state in our samples. Pr_0.6−xEu_xSr_0.4MnO₃ (x=0, 0.05, 0.1 and 0.15) polycrystalline samples were prepared using the solid–solid reaction method at high temperature. The compounds yielded are single phase and crystallize in the orthorhombic system with the Pnma space group. The substitution of Eu for Pr leads to a decrease of the Curie temperature T_C from 303 K for x=0.00 to 260 K for x=0.15. All of our compounds exhibit a large magnetic entropy change with a maximum around 2.2 J/kg K under a magnetic applied field change of 2 T for all compounds.     

Thermomagnetic transitions and coercivity mechanism in bulk composite Nd60Fe30Al10 alloys

The thermomagnetic behaviour (within the temperature range 553-300 K) for the bulk composite Nd₆₀Fe₃₀Al₁₀ alloy is described in terms of a transition from paramagnetic to superferromagnetic state at T=553 K, followed by a ferromagnetic ordering for T<473 K. For the superferromagnetic regime, the alloy thermomagnetic response was associated to a homogeneous distribution of magnetic clusters with mean magnetic moment and size of 1072 μ_B and 2.5 nm, respectively. For T<473 K, a pinning model of domain walls described properly the alloy coercivity dependence with temperature, from which the domain wall width and the magnetic anisotropy constant were estimated as being of ≈8 nm and ≈10⁵ J/m³, typical values of hard magnetic phases. Results are supported by microstructural and magnetic domain observations.