Polarized SSXANES study of spin ordering in ferromagnetic and paramagnetic phases of La1.2Sr1.65Ca0.15Mn2O7

Spin-selected polarized X-ray absorption near-edge structures (SSXANES) at the Mn K-edge from a bilayer La_1.2Sr_1.65Ca_0.15Mn₂O₇ single crystal have been studied with high resolution, both in the ferromagnetic (15 K) as well as paramagnetic phase (300 K). The orientation-dependent SSXANES spectra show unmistakable temperature dependence as the system makes the ferromagnetic to paramagnetic phase transition. The pre-edge structures are too intense to be ascribed to weak quadrupole transitions and are interpreted in terms of hybridization of Mn 3d orbitals with O2p and Mn 4p orbitals over and above similar onsite hybridization. The results also indicate possible existence of a small local (time-frozen) ferromagnetic ordering in the macroscopically disordered state. Need for further experimental and theoretical work on the SSXANES spectra from the bilayer system is emphasized.     

Correlation between extrinsic magnetoresistance and electroresistance in La0.6Pb0.4MnO3 thin films as revealed from current-voltage and ferromagnetic resonance studies

We have investigated magnetoresistance (MR) and electroresistance (ER) of well characterized La_0.6Pb_0.4MnO₃ (LPMO) films having two different crystallinity (i) (00l) oriented single-crystalline, SC, i.e. without any grain boundaries, and (ii) nanocrystalline, NC, with an average grain size of 17 nm. Both MR and ER were remarkably different for the two films, that is, (i) NC films exhibited a highest MR of ∼100% near the metal-insulator transition temperature; while for SC films the MR was in the range of 40-60%, (ii) NC films exhibited a finite ER, which increased monotonically with decreasing temperature; while in SC films ER was completely absent. Using current-voltage characteristic and ferromagnetic resonance studies we demonstrate that both enhanced MR and ER in NC films are extrinsic in nature and originate due to the presence of spin glassy grain boundaries.     

Electron spin resonance study of bulk and nanosized La0.875Sr0.125MnO3

The structural, transport and electron spin resonance properties of bulk and nanosized La_0.875Sr_0.125MnO₃ prepared by a sol-gel method have been investigated. The bulk sample has an orthorhombic structure and a ferromagnetic insulating ground state. The ESR spectra indicate the coexistence of the ferromagnetic insulating and ferromagnetic metallic phases below T_C. In addition to a sharp peak in the vicinity of T_C, another sharp peak close to is clearly observed in the intensity of the spectra, which may be correlated with the structural transition and orbital ordering at this temperature. For the nanosized sample, a drastically different behavior is found. With a rhombohedral structure down to 70 K, the nanosized sample shows a ferromagnetic metallic ground state. The ESR studies reveal the coexistence of the paramagnetic and ferromagnetic resonance signals. The resonance intensity shows a broad peak around 200 K, which may be due to the wide ferromagnetic transition in the nanoparticle.     

Low field magnetoresistance and conduction noise in layered manganite La1.4Ca1.6Mn2O7

Temperature dependence of conduction noise and low field magnetoresistance of layered manganite La_1.4Ca_1.6Mn₂O₇ (DLCMO) are reported and compared with the infinite layered manganite La_0.7Ca_0.3MnO₃ (LCMO). The double layered manganite was prepared using standard solid state reaction method and had a metal-insulator transition temperature (T_M-I) of 155 K. The temperature dependence of susceptibility showed evolution of ferromagnetic ordering at 168 K. The observed voltage noise spectral density (S_V) shows 1/f^α type of behaviour at all temperatures from 77 K to 300 K. In the ferromagnetic region (T<168 K), S_V/V² shows two peaks at 164 K and 114 K. The observed two peaks in normalised conduction noise of DLCMO is attributed to the excess noise generated due to setting up of short range 2D-ferromagnetic ordering and long range 3D-ferromagnetic ordering at two different temperatures T_C2 and T_C1. In temperature range between T_C1 and T_C2, the magnetoresistance (MR) showed a gradual increase with the magnetic field. The observed MR has been explained in the framework of the two phase model [ferromagnetic (FM) domains and paramagnetic (PM) regions].     

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.     

Large magnetoresistance induced by surface ferromagnetism in A-type antiferromagnetic La0.4Sr0.6MnO3 nanoparticles

Grain size effects on magnetic and transport properties for heavily Sr-doped A-type antiferromagnetic La_0.4Sr_0.6MnO₃ ceramics were studied. It was observed that with decrease in grain size, surface ferromagnetism could be introduced due to bond-breaking at surfaces. With decrease in grain size, the surface ferromagnetism was enhanced, and the phase transition order distinguished from the Arrott plot was a second one. The surface-induced ferromagnetism was insulating as judged from transport properties. With decrease in grain size, magnetoresistance was largely improved for both high magnetic and low magnetic fields. Under a 500 Oe magnetic field, the magnetoresistance is improved from 0.2%, 0.1%, 0.03% and 0.02% for the sample with grain size of 150 nm at 10, 100, 200 and 300 K, respectively, to 3%, 2.3%, 0.43% and 0.12% for the sample with grain size of 20 nm at 10, 100, 200 and 300 K. It was interesting to find that large magnetoresistance could be induced due to the surface ferromagnetism in A-type antiferromagnetic La_0.4Sr_0.6MnO₃ nanoparticles, which suggested that it was possible to search for manganites with relatively high low-field magnetoresistance in nanostructured A-type antiferromagnetic materials.     

Intrinsic inhomogeneity and non-linear conduction in charge-ordered Bi0.5Ca0.4Sr0.1MnO3

Systematic studies of X-ray, magnetic, electronic transport, and elastic properties have been performed on polycrystalline Bi_0.5Ca_0.4Sr_0.1MnO₃ sample. The sample exhibits charge ordering (CO) state below T_CO (=304 K), accompanied by a distinct maximum in magnetization. The softening of Young's modulus in the vicinity of T_CO indicates that there is a strong coupling of electron-phonon due to Jahn-Teller (JT) effect. The dynamic ferromagnetic spin correlations are observed at high temperatures above T_CO, which are replaced by antiferromagnetic (AFM) spin fluctuations at a concomitant CO transition. Below 32 K, a spin-glass (SG) state dominates at low temperatures. The voltage-current (V-I) characteristics measurement results indicate that the non-linear conduction starts above a threshold current, giving rise to a region of negative differential resistance (NDR). The origin of the non-linear conduction is discussed in view of current induced collapse of CO state associated with phase-separation mechanism.     

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.     

Electrical conduction through bond percolation in Nd0.67Sr0.33MnO3

We report our analysis of resistivity data on Nd_0.67Sr_0.33MnO₃ polycrystalline samples as a function of preparative conditions using a bond percolation model for a random mixture of metallic and insulating regions, assuming polaronic transport above and below the metal-insulator (M-I) transition temperature. Our analysis suggests that for oxygen deficient compounds the M-I transition that occurs at a lower temperature than the ferromagnetic transition arises from a percolation of the metallic regions. The temperature dependence of resistivity and thermopower suggests the existence of a bimodal distribution of conductivities.     

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.     

Electrical conductivity and low field magnetoresistance in polycrystalline La1−xKxMnO3 pellets prepared by pyrophoric method

Electrical conductivity and magnetoresistance of a series of monovalent (K) doped La_1−xK_xMnO₃ polycrystalline pellets prepared by pyrophoric method have been reported. K doping increases the conductivity as well as the Curie temperature (T_C) of the system. Curie temperature increases from 260 to 309 K with increasing K content. Above the metal-insulator transition temperature (T>T_MI), the electrical resistivity is dominated by adiabatic polaronic model, while in the ferromagnetic region (50<T<T_MI), the resistivity is governed by several electron scattering processes. Based on a scenario that the doped manganites consist of phase separated ferromagnetic metallic and paramagnetic insulating regions, all the features of the temperature variation of the resistivity between ∼50 and 300 K are described very well by a single expression. All the K doped samples clearly display the existence of strongly field dependent resistivity minimum close to ∼30 K. Charge carrier tunneling between antiferromagnetically coupled grains explains fairly well the resistivity minimum in monovalent (K) doped lanthanum manganites. Field dependence of magnetoresistance at various temperatures below T_C is accounted fairly well by a phenomenological model based on spin polarized tunneling at the grain boundaries. The contributions from the intrinsic part arising from DE mechanism, as well as, the part originating from intergrannular spin polarized tunneling are also estimated.     

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,electrical transport and electron spin resonance studies of ferromagnetic insulating manganites Nd0.85Na0.15MnO3

We have investigated the magnetic, electrical transport and electron spin resonance (ESR) properties of polycrystalline Nd_0.85Na_0.15MnO₃ prepared by sol–gel method. A ferromagnetic–paramagnetic (FM–PM) transition is observed around 110 K, which is not accompanied by a metal–insulator transition. The sample displays the complete PM state associated with the ESR spectra fitted by single Lorentzian line shape above 130 K. Below 130 K, ESR spectra become distorted and then linewidth increases rapidly, where short-range magnetic order develops and coexists with PM phase due to the inhomogeneous magnetic state. In addition, the large difference between the activation energies obtained from the resistivity and ESR parameters (peak-to-peak linewidth and line intensity) at the frame of adiabatic small polaron hopping model is pointed out for Nd_0.85Na_0.15MnO₃.     

Enhanced magnetoresistance in La0.82Sr0.18MnO3-π-conjugated semiconducting polymer heterostructure

We report a large enhancement (∼90%) in magnetoresistance in La_0.82Sr_0.18MnO₃ (LSMO) layers by incorporating a π-conjugated semiconducting polymer layer in between them. The epitaxial LSMO layers were deposited by DC magnetron sputtering on SrTiO₃ single crystal substrates and have FM transition temperature (T_C)∼310 K. A semiconducting polymer poly(3-octylthiophene) (P3OT) layer was deposited over the epitaxial LSMO layer by solution dip coating technique and with subsequent deposition of another epitaxial LSMO layer, forming a LSMO-P3OT-LSMO heterostructure. The effect of P3OT incorporation on magnetotransport properties of this heterostructure has been examined in the temperature range 77-350 K. Large MR enhancement observed near room temperature in the FM regime is explained in terms of efficient magnetic field dependent carrier injection at LSMO/P3OT interface.     

Charge and lattice dynamics of ordered state in La1/2Ca1/2MnO3: infrared reflection spectroscopy study

We report an infrared reflection spectroscopy study of La_1/2Ca_1/2MnO₃ over a broad frequency range and temperature interval which covers the transitions from the high temperature paramagnetic to ferromagnetic and, upon further cooling, to antiferromagnetic phase. The structural phase transition, accompanied by a ferromagnetic ordering at T_C=234 K, leads to enrichment of the phonon spectrum. A charge ordered antiferromagnetic insulating ground state develops below the Néel transition temperature T_N=163 K. This is evidenced by the formation of charge density waves and opening of a gap with the magnitude of 2Δ₀=(320±15) cm⁻¹ in the excitation spectrum. Several of the infrared active phonons are found to exhibit anomalous frequency softening. The experimental data suggest coexistence of ferromagnetic and antiferromangetic phases at low temperatures.     

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.     

Dynamic phase separation as revealed by the strong resistance relaxation in epitaxially shear-strained La0.67Ca0.33MnO3/NdGaO3(0 0 1) thin-films

Strong phase competitions between the ferromagnetic metal and the charge-ordered-insulator have been induced in a wide temperature range of 10-256 K for the shear-strained La_0.67Ca_0.33MnO₃/NdGaO₃(0 0 1) films. Based on various magnetotransport measurements, the mobility of phase boundaries was inferred to change dramatically with temperature. In the high temperature range where the phase boundaries are movable, strong relaxation in resistivity was observed, while at the frozen temperatures lower than 40 K it is weakened. The resistivities tend to relax in accordance with the phase transitions driven by the temperature or magnetic field in the phase separation (PS) background. Moreover, to our surprise, while the melting fields of the insulating phase varied with film thicknesses, for a given film however, they stay unchanged when started with different phase fractions produced by the field or thermal cycling. The results show a crucial role of the inherent strain state in determining PS and phase competitions in these epitaxial thin films.     

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.     

Effect of magnetic field on the TC and magnetic properties for the aligned MnBi compound

In the compound MnBi, a first-order transition from the paramagnetic to the ferromagnetic state can be triggered by an applied magnetic field and the Curie temperature increases nearly linearly with an increase in magnetic field by ∼2 K/T. Under a field of 10 T, T_C increases by 20 and 22 K during heating and cooling, respectively. Under certain conditions a reversible magnetic field or temperature induced transition between the paramagnetic and ferromagnetic states can occur. A magnetic and crystallographic H-T phase diagram for MnBi is given. Magnetic properties of MnBi compound aligned in a Bi matrix have been investigated. In the low temperature phase MnBi, a spin-reorientation takes place during which the magnetic moments rotate from being parallel to the c-axis towards the basal plane at ∼90 K. A measuring Dc magnetic field applied parallel to the c-axis of MnBi suppresses partly the spin-reorientation transition. Interestingly, the fabricated magnetic field increases the temperature of spin-reorientation transition T_s and the change in magnetization for MnBi. For the sample solidified under 0.5 T, the change in magnetization is ∼70% and T_s is ∼91 K.     

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.