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.     

On the coexistence of spin and lattice polarons in the La0.67−xEuxCa0.33MnO3 CMR system

The electrical and magnetic transport properties of the La_0.67−xEu_xCa_0.33MnO₃ system exhibit lowering of insulator to metal and paramagnetic to ferromagnetic transition temperature (T_C) with the increase of Eu concentration in addition to possessing CMR property. The temperature variation of electrical resistivity and magnetic susceptibility for x=0.21 is found to have two distinct regions in the paramagnetic state for T>T_P; one with the localization of lattice polaron in the high-temperature region (T>1.5T_P) satisfying the dynamics of variable range hopping (VRH) model and the other being the combination of the spin and lattice polarons in the region T_P<T<1.5T_P. The resistivity variation with temperature and magnetic field, the cusp in the resistivity peak and CMR phenomenon are interpreted in terms of coexistence of spin and lattice small polarons in the intermediate region (T_P<T<1.5T_P). The spin polaron energy in the La_0.46Eu_0.21Ca_0.33MnO₃ system is estimated to be 106.73±0.90 meV and this energy decreases with the increase of external magnetic field. The MR ratio is maximal with a value of 99.99% around the transition temperature and this maximum persists till T→0 K, at the field of 8 T.     

Electrical behavior of some silver-doped lanthanum-based CMR materials

With a view to understand the structural, magnetic and electrical properties of La_1−xAg_xMnO₃ (x=0.05-0.3), a series of samples were prepared by polyvinyl alcohol (PVA) gel route. It has been found that both the metal-insulator and ferro- to paramagnetic transition temperatures after increasing up to the composition x=0.20, are found to remain constant thereafter. The electrical resistivity vs. temperature plot of the sample x=0.10 is found to exhibit an insulating behavior below 36 K, while the sample, x=0.20 exhibits two peaks, and the observed behavior is explained on the basis of the phase separation model. The low-temperature (T<T_P), electrical resistivity data were analyzed by a theoretical model, ρ=ρ₀+ρ₂T²+ρ_4.5T^4.5, indicating the importance of grain/domain boundary effects, electron-electron and two-magnon scattering processes. The low-temperature resistivity data (T<50 K) were fitted to an equation, which is based on the combined effect of weak localization, electron-electron and electron-phonon scattering.     

Electronic transport and magnetoresistance of a heterojunction composed of La0.7Ce0.3MnO3 and 1 wt% Nb-doped SrTiO3

We experimentally studied the transport properties and magnetoresistance behavior of a La_0.7Ce_0.3MnO₃/SrTiO₃ (doped by 1 wt% Nb) junction. Based on the analyses of the current-voltage relations and the depletion width, we conclude that the dominant transport mechanism of the junction is tunneling. The magnetoresistance of the junction is negative throughout the whole bias voltage range (from −1 V to 0.4 V) and the whole temperature range (below 300 K). It is believed that the magnetic field depresses the junction resistance by reducing the depletion width of the junction.     

Thermoelectric power of potassium doped lanthanum manganites at low temperatures

The temperature-dependent resistivity and thermoelectric power of monovalent (K) doped La_1−xK_xMnO₃ polycrystalline pellets (x=0.05, 0.10 and 0.15) between 50 and 300 K are reported. K substitution enhances the conductivity of this system. Curie temperature (T_C) also increases from 260 to 309 K with increasing K content. In the paramagnetic region (T>T_C), the electrical resistivity is well represented by adiabatic polaron hopping, while in the ferromagnetic region (T<T_C), the resistivity data show a nearly perfect fit for all the samples to an expression containing, the residual resistivity, spin-wave and two-magnon scattering and the term associated with small-polaron metallic conduction, which involves a relaxation time due to a soft optical phonon mode. Small polaron hopping mechanism is found to fit well to the thermoelectric power (S) data for T>T_C whereas at low temperatures (T<T_C) in ferromagnetic region (S_FM), S_FM is well explained with the spin-wave fluctuation and electron–magnon scattering. Both, resistivity and thermopower data over the entire temperature range (50–300 K) are also examined in light of a two-phase model based on an effective medium approximation.     

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.     

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.     

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.     

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].     

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.     

Low field magneto-transport in LBSMO–PMMA composite

The low field magneto-transport has been measured as a function of temperature in the range 77–300 K and magnetic field; H?3.6 kOe for La_0.7Ba_0.2Sr_0.1MnO₃ (LBSMO)–x wt% PMMA composites where x=0, 2, 6 and 10. The X-ray diffraction (XRD) study reveals that no structural modification has occurred in the LBSMO in the composite. Scanning electron microscopy (SEM) investigation shows PMMA getting dispersed through the sample volume and some LBSMO grains appear to be coated with the polymer. The metal-like transition observed at ∼150 K in the virgin LBSMO sample disappears in the composite samples and the resistance shows an increase of about three orders of magnitude as the polymer concentration is increased to 10 wt%. Despite this huge increase in the resistance, the low field magneto-resistance (LFMR) shows an enhancement although smaller than the values commonly observed for other manganite-polymer composite systems. Spin polarized tunneling that causes LFMR seems to be enhanced in the composites.     

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.     

Effect of magnetic film thickness on rectifying properties of La0.8Sr0.2MnO3/TiO2 heterostructures

The La_0.8Sr_0.2MnO₃ (LSMO)/ TiO₂ heterostructures with different thicknesses of the LSMO films were successfully synthesized using the RF magnetron sputtering technique. Excellent rectifying characteristics are presented in all heterostructures in a wide temperature range. The differences of the diffusive potentials for three heterojunctions are very little at 300 K. The samples exhibit a high resistance that plays an important role on their rectifying properties. The diffusive potential decreases with increasing temperature. The result is attributed to both the reduction of the thickness of the deletion layer due to the thermal diffusion and the modulation of the interfacial electronic structure of the heterostructures. The metal-insulator (M-I) transition is observed clearly from the single LSMO layers and the LSMO/ TiO₂ p-n heterojunctions.     

Magnetoresistance in La1−xCaxMnO3 (0≤x<0.4)

The magnetic and transport properties of La_1−xCa_xMnO₃ (0≤x<0.4) have been systematically studied. The magnetoresistance (MR) maximum appears at x=0.2-0.25 and the temperature dependence of MR for x>0.25 shows a much broader profile than that of samples for x=0.2-0.25. Based on a scenario in which there is a short-range charge ordering (CO) state coexisting in the ferromagnetic state matrix for x>0.25, and the least or even no short-range CO state exists in samples for x=0.2-0.25, the above observations can be understood.     

Growth of single-phase c-axis aligned La1.2Ca1.8Mn2O7 films on SrTiO3 (001)

We report the growth of single phase, c-axis aligned thin films of La_1.2Ca_1.8Mn₂O₇ on SrTiO₃ (001) substrates using a controlled pulsed laser deposition method. In this method, constraint of epitaxy is utilized to stabilize the Ruddlesdon-Popper (RP) phase of La_1.2Ca_1.8Mn₂O₇. Oxygen ambient pressure and the rate of deposition play a very important role in influencing the epitaxial growth as well as maintaining phase purity of the material. The oxygen pressure inside the deposition chamber was very precisely controlled and varied during the layer-by-layer growth of the film. Films, prepared by our method, show excellent electrical and magnetic characteristics with a sharp metal-insulator transition at T_M-I=90 K, closely followed by a magnetic transition at T_C=91 K.     

Penetration of electromagnetic field through the La-Er-Ba manganite far above the magnetic phase transition temperature

Using the technique of penetration of electromagnetic waves through the bulk samples of La_0.60Er_0.07Ba_0.33MnO₃ manganite, it is shown that in this class of strongly correlated materials the local dynamic magnetic ordering is preserved at the temperature by 66 K above the Curie temperature where the static long-range magnetic order is absent. In this temperature range the dynamic magnetic permeability exceeds unity and is frequency dependent. The average lifetime of local ordered states is estimated.     

Epitaxial growth La0.67Ca0.33MnO3 thin film by radio frequency sputtering method

Perfect epitaxial growth of La_0.67Ca_0.33MnO₃ (LCMO) thin film has been achieved on (1 0 0) LaAlO₃ (LAO) single crystal substrate by radio frequency sputtering method. X-ray diffraction (XRD) and electron diffraction analysis indicates that La_0.67Ca_0.33MnO₃ film grows epitaxially on LaAlO₃ along [1 0 0] direction of the substrate. The resistivity variation with temperature of the film shows a sharp metal to semiconductor transition peak around 253 K, which is close to that of the target. The magnetoresistance (MR) also reveals high quality epitaxy film characteristic at low temperatures and near the metal to semiconductor transition temperature.     

Temperature dependence of the gap in the density of states near the Fermi level in a hole doped manganite

In this paper, we report a model-based quantitative analysis of temperature dependent scanning tunneling spectroscopy (STS) data taken on epitaxial thin films of the hole doped manganite La_0.7Ca_0.3MnO₃. The film, grown on lattice matched NdGaO₃ substrate, has a ferromagnetic transition temperature T_c=268 K. The analysis allows us to evaluate how the tunneling curve evolves across the transition temperature. We find that there is a gap Δ in the density of states (DOS), which peaks at T≈T_c. The gap closes in the ferromagnetic state following the evolution of the magnetization. The gap closing is gradual and not sudden at T=T_c. Above T_c the gap reduces from the peak value and reaches a limiting value of ≈75 meV for T/T_c≥1.1 which is close to the value of 60 meV seen from transport experiments.     

Localized insulator-conductor transformation of graphene oxide thin films via focused laser beam irradiation

By scanning a focused laser beam over graphene oxide (GO) film deposited on SiO₂/Si substrates, conductive strips as small as 1 μm can be patterned directly either as a channel in the insulating matrix, or as a stand-alone micro belt. The conductivity was increased by at least two orders of magnitude with the mobility estimated in the range of 1–10 cm²/V s. Raman mapping and X-ray photoelectron spectroscopy studies demonstrated the reduction of GO in the laser-irradiated area. The conductance of the patterned channel was independent of the change in oxide-electrode contact resistance of the graphene, and increased linearly with increasing channel width. Increasing irradiation power by repeated scanning initially increased the conductivity of the irradiated area and saturated at a conductivity of ∼36 S/cm. Partial oxidative burning combined with photothermal reduction was identified as the underlying mechanism for the enhancement of the conductivity after laser irradiation on the GO film. Oxidative burning can be controlled by varying the film thickness and laser power.