Superspin-glass like behavior of nanoparticle La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> obtained by mechanochemical milling

Single-phase perovskite compound La_0.7Ca_0.3MnO₃ was synthesised by a high-energy ball milling in a single step processing. Structure and morphology characterizations revealed nanoparticle nature of this mixed valent manganite with the average particle diameter of 9 nm. Comprehensive set of magnetic measurements showed that the system can be described as an ensemble of interacting magnetic nanoparticles where each particle possesses high magnetic moment, i.e., superspin. Furthermore, magnetic behavior showed contributions from both superspin-glass (SSG) and superparamagnetic (SP) states, and the prevailing properties depended on the experimental conditions. It was established that SSG state dominated in low magnetic fields up to 500 Oe while in higher applied fields suppression of collective behavior occurred and individual characteristics of nanoparticles prevailed. It was also concluded that the applied method of synthesis produced system with high magnetic anisotropy as well as with the large nanoparticle shell whose thickness amounts 30% of a particle diameter.     

Spin-glass dynamics in interacting nanoparticle system La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> obtained by mechanochemical milling

Spin dynamics in mechanochemically obtained nanoparticle manganite La_0.70Ca_0.30MnO₃ was investigated in this study by means of a series of AC and DC magnetic measurements. AC susceptibility indicates the presence of sizeable interparticle interactions, yielding collective magnetic behavior. The related properties were probed by experiments in weak DC field: memory effects were analyzed in both field-cooled (FC) and zero field-cooled (ZFC) regimes, while, after ZFC aging, magnetic relaxation was recorded. The system appears to be sensitive to magnetothermal history, in analogy with spin-glass-like compounds. The analysis of the data indicates the occurrence of slow dynamics in an ensemble of strongly interacting super spins.     

Giant magnetorefractive effect in La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> films

Complex experimental investigations of the structural, optical, and magneto-optical properties (magnetotransmission, magnetoreflection, and transversal Kerr effect, as well as the magnetoresistance, of La_0.7Ca_0.3MnO₃ epitaxial films indicate that magnetoreflection and magnetotransmission in manganite films can reach giant values and depend strongly on the magnetic and charge homogeneity of the films, their thickness, and spectral range under investigation. It has been shown that the optical enhancement of the magnetorefractive effect occurs in thin films as compared to manganite crystals. In the region of the minimum of the reflectance near the first phonon band, the resonance-like magnetorefractive effect has been observed, which is accompanied by change of the sign of the magnetoreflection. A model based on the theory of the magnetorefractive effect has been proposed to qualitatively explain this behavior.     

Hysteresis of magnetoresistance in granular La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> at low temperatures

The magnetoresistance of granular La_0.7Ca_0.3MnO₃ is studied experimentally over wide ranges of temperatures and magnetic fields. The emphasis is on anomalously large hysteresis of magnetoresistance at low temperatures (T = 4.2 K). The observed ρ(H) dependence can be qualitatively explained by spin-dependent tunneling of electrons through the dielectric boundaries of conducting granules characterized by a wide spread in the magnetic-moment magnitudes.     

Magnetorefractive effect in La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> in the infrared spectral range

The reflection and magnetic reflection spectra, magnetic resistance, electrical properties, and equatorial Kerr effect in La_0.7Ca_0.3MnO₃ crystals have been complexly investigated. The measurements have been performed in wide temperature and spectral ranges in magnetic fields up to 3.5 kOe. It has been found that magnetic reflection is a high-frequency response in the infrared spectral range to the colossal magnetore-sistance near the Curie temperature. Correlation between the field and temperature dependences of the magnetic reflection and colossal magnetoresistance has been revealed. The previously developed theory of the magnetorefractive effect for metallic systems makes it possible to explain the experimental data at the qualitative level. Both demerits of the theory of the magnetorefractive effect in application to the magnets and possible additional mechanisms responsible for the magnetic reflection are discussed.     

Elastic properties of a La<Subscript>0.5</Subscript>Pr<Subscript>0.2</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> single crystal

The temperature dependences of the velocity of longitudinal sound and internal friction in the ferromagnetic La_0.5Pr_0.2Ca_0.3MnO₃ single crystal with magnetic first-order phase transition were studied. It was found that the sound velocity decreases by ≈20% in transition from the ferromagnetic to paramagnetic state. In the paramagnetic region, the extended temperature hysteresis of the sound velocity and the internal friction was observed. It was shown that La_0.5Pr_0.2Ca_0.3MnO₃ has two paramagnetic phases with different sound velocities.     

Unipolar resistive switching in high-resistivity Pr<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> junctions

We report the first demonstration of laser forward transfer using a real-time reconfigurable mask based on a spatial light modulator. The ability to dynamically change the projected beam shape and size of a coherent light source, in this case a 355-nm pulsed UV laser, represents a significant technological advancement in laser direct-write processing. The application of laser transfer techniques with adaptive control of the laser beam pattern is unique and represents a paradigm shift in non-lithographic processing. This work describes how the size and shape of an incident laser beam can be dynamically controlled in real time with the use of a digital micromirror device (DMD), resulting in laser-printed functional nanomaterials with geometries identical to those of the projected beam. For applications requiring additive non-lithographic techniques, this novel combination, which relies on the laser forward transfer of variable, structured voxels, represents a dramatic improvement in the capabilities and throughput of laser direct-write processes.     

Two-phase paramagnetic-ferromagnetic state of La<Subscript>0.7</Subscript>Pb<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> single-crystal lanthanum manganite

Two phases, paramagnetic and ferromagnetic, were shown by the magnetic resonance method to coexist below the temperature T _C in La_0.7Pb_0.3MnO₃ single crystals exhibiting colossal magnetoresistance. The magnetic resonance spectra were studied in the frequency range 10–78 GHz. The specific features in the behavior of the spectral parameters were observed to be the strongest at the temperatures corresponding to the maximum magnetoresistance in the crystals. The concentration ratios of the paramagnetic and ferromagnetic phases in the samples were found to be sensitive to variations in temperature and external magnetic field. This behavior suggests realization of the electronic phase separation mechanism in the system under study.     

Magnetotransport characteristics of strained La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> epitaxial manganite films

The electrical and magnetic characteristics of La_0.7Sr_0.3MnO₃ (LSMO) epitaxial manganite films are investigated by different methods under conditions when the crystal structure is strongly strained as a result of mismatch between the lattice parameters of the LSMO crystal and the substrate. Substrates with lattice parameters larger and smaller than the nominal lattice parameter of the LSMO crystal are used in experiments. It is shown that the behavior of the temperature dependence of the electrical resistance for the films in the low-temperature range does not depend on the strain of the film and agrees well with the results obtained from the calculations with allowance made for the interaction of electrons with magnetic excitations in the framework of the double-exchange model for systems with strongly correlated electronic states. Investigations of the magneto- optical Kerr effect have revealed that an insignificant (0.3%) orthorhombic distortion of the cubic lattice in the plane of the NdGaO₃(110) substrate leads to uniaxial anisotropy of the magnetization of the film, with the easy-magnetization axis lying in the substrate plane. However, LSMO films on substrates (((LaAlO₃)_0.3+(Sr₂AlTaO₆)_0.7)(001)) ensuring minimum strain of the films exhibit a biaxial anisotropy typical of cubic crystals. The study of the ferromagnetic resonance lines at a frequency of 9.76 GHz confirms the results of magnetooptical investigations and indicates that the ferromagnetic phase in the LSMO films is weakly inhomogeneous.     

Microstructural evolution and electrical properties of La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> thin films grown on SrTiO<Subscript>3</Subscript> substrates by excimer-laser assisted metal-organic deposition

Thin films of La_0.7Ca_0.3MnO₃ were successfully grown epitaxially on (100) single-crystal SrTiO₃ substrates by excimer-laser assisted metal-organic deposition. Initial amorphous LCMO thin films were obtained by metal-organic deposition at 500 °C. Crystallization and epitaxial growth of the films was achieved using a KrF pulsed laser irradiation while the film/substrate samples were kept at 500 °C. High resolution transmission electron microscopy observations on cross-sections demonstrate the formation mechanism of the epitaxial films. The crystallization process starts at the LCMO/STO interface and grows by increasing the number of laser shots. A fully crystallized film was obtained after 5 min of irradiation. The film/substrate interface was found to be sharp and abrupt. The temperature dependence of the resistance R(T) shows various behaviors, starting from insulating to semiconducting and metal–insulator transition material during the formation of the manganite film. The oxygen content was also improved by increasing the irradiation time. Promising values of the temperature coefficient of resistance were obtained from these manganite films for prospect integration in silicon based microbolometric devices. PACS 81.15.-z; 81.15.Np; 73.61.-r; 71.30.+h     

Elastic properties of La<Subscript>0.82</Subscript>Ca<Subscript>0.18</Subscript>MnO<Subscript>3</Subscript> single crystal

The temperature dependences of the velocity of longitudinal sound waves and the internal friction in a La_0.82Ca_0.18MnO₃ single crystal with the Curie temperature T _C = 181 K have been studied. As temperature decreases, the single crystal is shown to undergo the transition from the pseudocubic O* to the Jahn–Teller O’ phase at T ~ 254 K and the reverse transition from O’ to O* phase at T ~ 84 K. The velocity of sound and the internal friction in the O’ phase are found to be significantly smaller than those in the O* phase.     

Elastic and magnetic properties of the La<Subscript>0.6</Subscript>Pr<Subscript>0.1</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> single crystal

The temperature dependences of the velocity of longitudinal sound, internal friction, and magnetization of the single crystal with the nominal composition La_0.6Pr_0.1Ca_0.3MnO₃ have been measured. It has been found that the substitution of praseodymium for lanthanum in La_0.7Ca_0.3MnO₃ leads to a decrease in the velocity of sound and to an increase in the spontaneous magnetization. The method of determining the Curie temperature distribution function during a first-order transition has been proposed. It has been shown that, in the crystal under study, this function is asymmetric.     

Current-induced Conductance Jumps in Mechanically Controllable Junctions of La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> Manganites

The magnetic switching processes in mechanically controllable junctions (MCJ), made from high-quality single crystals of La_0.7Sr_0.3MnO₃, are studied as a function of the DC current (up to 10⁹ A/cm²) passing through the nanoconstriction. The current-voltage (I-V) curves of the MCJ are typical for an electron tunnelling process. By fitting I-V curves to the Simmons model, the barrier width (1 - 1.6) nm and height (0.4 - 1.7) eV of the junctions and their effective tunnel area (1-10) × 10^?11 cm² were estimated. Based on the close relation between transport properties and the magnetization in manganese compounds, we interpret the jumps in the conductance of MCJ, by integer multiples of e²/h, as due to the configuration reorientation of the magnetization of the Mn-ions clusters at the constriction surfaces.     

Kinetics of magnetization reversal in a thin La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> manganite film

The kinetics of magnetization reversal of a thin LSMO film has been studied for the first time. It is shown that the magnetic domain structure critically depends on the conditions of structure formation. In the demagnetized state (after zero-field cooling from T _c ), a maze-like domain microstructure with perpendicular magnetization is formed in the film. However, after field cooling and/or saturating magnetization by a field of arbitrary orientation, the [110] direction of spontaneous magnetization in the film plane is stabilized; this pattern corresponds to macrodomains with in-plane magnetization. Further film magnetization reversal (both quasi-static and pulsed) from this state is implemented via nucleation and motion of 180° “head-to-head” domain walls. Upon pulse magnetization reversal, the walls “jump” at a distance proportional to the applied field strength and then undergo thermally activated drift. All dynamic characterisitcs critically depend on the temperature when the latter varies around the room temperature.     

Positive magnetoresistance of La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript>/C Composites at room temperature

Two-phase composites xLa_0.7Sr_0.3MnO₃/(100–x)C (x = 5–85 mass %) have been synthesized. The magnetoresistive properties of these materials in magnetic fields from 0 to 15 kOe have been investigated. It has been shown that, at room temperature, the positive isotropic magnetoresistance for samples with x = 50–60 mass % reaches 15%.     

A sonochemical-assisted synthesis and annealing temperature effect of La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> nanoparticles

This paper reports on the sonochemical-assisted synthesis of La_0.7Sr_0.3MnO₃ (LSMO) nanoparticles (NPs) which have a single-crystalline perovskite structure. The average particle size of LSMO NPs was controlled from about 40 to 120 nm by changing the annealing temperatures from 750 to 1050°C. The particle size, electrical resistivity, and ferromagnetic transition temperature of LSMO NPs were strongly dependent on the annealing temperature. A substantial decrease in resistivity and an enhancement in the insulator–metal transition temperature were found on increasing the annealing temperature. Furthermore, the enhancement in magnetization and paramagnetic–ferromagnetic (PM–FM) transition temperatures was observed as the annealing temperature increases.     

Effect of an interface boundary on the magnetooptical and magnetotransport properties of La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript>/La<Subscript>0.67</Subscript>Sr<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> heterostructures

The optical, magnetooptical (Kerr effect and magnetotransmission), and magnetotransport properties of La_2/3Ca_1/3MnO₃/La_2/3Sr_1/3MnO₃ and La_2/3Ca_1/3MnO₃/SrTiO₃/La_2/3Sr_1/3MnO₃ heterostructures on SrTiO₃ substrates are studied. The contribution of the interface boundary to the magnetotransmission is typical of a material with a transitional composition. It is found that a 2-nm-thick SrTiO₃ spacer does not influence the shape and position of the magnetotransmission peak in a field normal to the surface of the heterostructure but increases the contribution of the upper layer to the magnetotransmission in the Voigt geometry and also enhances the magnetoresistance that is due to the tunneling of spin-polarized carriers through the spacer. The Kerr spectra taken of the heterostructures are typical of single-layer single-crystal films.     

Structural and magnetic phase transitions in Pr<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> at high pressures

The crystal structure and Raman spectra of Pr_0.7Ca_0.3MnO₃ manganite at high pressures of up to 30 GPa and the magnetic structure at pressures of up to 1 GPa have been studied. A structural phase transition from the orthorhombic phase of the Pnma symmetry to the high-pressure orthorhombic phase of the Imma symmetry has been observed at P ∼ 15 GPa and room temperature. Anomalies of the pressure dependences of the bending and stretching vibrational modes have been observed in the region of the phase transition. A magnetic phase transition from the initial ferromagnetic ground state (T _C = 120 K) to the A-type antiferromagnetic state (T _N = 140 K) takes place at a relatively low pressure of P = 1 GPa in the low-temperature region. The structural mechanisms of the change of the character of the magnetic ordering have been discussed.     

Magnetotransport properties of La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> with different grain sizes

The magnetotransport and magnetoresistive (MR) properties of manganese-based La_0.67Ca_0.33MnO₃ perovskite with different grain sizes are reported. The electrical resistivity was measured as a function of temperature in magnetic fields of 0.5 and 1 T. The insulator–metal transition temperature, T _IM, shifted to a higher temperature with the application of the magnetic field. In zero field, T _IM is almost constant (∼271 K) for all samples except for the sample with the largest grain size, where T _IM=265 K. The temperature dependence of resistivity was fitted with several equations in the metallic (ferromagnetic) region and the insulating (paramagnetic) region. The density of states at the Fermi level, N(E _F), and the activation energy of electron hopping were estimated by fitting the resistivity versus temperature curves. The ρ–T ² curves are nearly linear in the metallic regime, but the ρ–T ^2.5 curves exhibit a deviation from linearity. The variable range hopping model and small polaron hopping model fit the data well in the high-temperature region, indicating the existence of the Jahn–Teller distortion that localizes the charge carriers. MR was found to increase with an increase in the magnetic field, an effect which is attributed to the intergrain spin tunneling effect.     

Pressure-induced antiferromagnetism in La<Subscript>0.75</Subscript>Ca<Subscript>0.25</Subscript>MnO<Subscript>3</Subscript> manganite

The crystal and magnetic structures of La_0.75Ca_0.25MnO₃ manganite are studied under high pressures up to 4.5 GPa in the temperature range 12–300 K by the neutron diffraction method. At normal pressure and temperature T _C = 240 K, a ferromagnetic state is formed in La_0.75Ca_0.25MnO₃. At high pressures P ≥ 1.5 GPa and at temperatures T < T _N ≈ 150 K, a new A-type antiferromagnetic state appears. A further increase in pressure leads to an increase in the volume fraction of the antiferromagnetic phase, which coexists with the initial ferromagnetic phase. The effect of high pressure causes a considerable increase in T _C with the slope dT _C /dP ≈ 12 K/GPa. Calculations performed in the framework of the double exchange model with allowance for the electron-phonon interaction make it possible to explain this pressure dependence of T _C on the basis of experimental data.