Magnetic ordering in La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript>x</Subscript>MnO<Subscript>3−<Emphasis Type="Italic">x</Emphasis>/2</Subscript> anion-deficient manganites

The structural, magnetic, and electrotransport properties of La_1?xSr_xMnO_{3? x/2}(0≤x≤0.30) manganites with perovskite structure are investigated experimentally as a function of oxygen deficiency. In the solid solutions La_1?xSr_xMnO₃, a change in the type of symmetry of the unit cell is observed at x=0.125. Samples with x≤0.125 are characterized by an O′-orthorhombic unit cell, whereas samples with x>0.125 are characterized by a rhombohedral unit cell. The structural properties of the anion-deficient solid solutions La_1?xSr_xMnO_3?x/2 are analogous to those of the stoichiometric system. It is assumed that, as the oxygen content decreases, La_{1? x}Sr_xMnO_3?x/2 anion-deficient solid solutions experience a series of successive magnetic phase transformations in the ground state: from an A-type (x=0) antiferromagnet to a cluster spin-glass-type inhomogeneous magnetic state (0.175>x≤0.30) through a two-phase (antiferromagnetic and ferromagnetic) state (0>x≤0.175). The anion-deficient solid solution with x=0.175 has the maximal value of the ferromagnetic component. As the oxygen deficiency increases, the resistivity of La_{1? x}Sr_xMnO_3?x/2 samples first decreases (up to a value of x=0.175), acquiring an activation character, and then increases (up to a value of x=0.30). In this case, none of the anion-deficient solid solutions exhibits a metal-semiconductor transition in the whole range of concentrations considered. A peak of magnetoresistance at a temperature below the point of magnetic ordering is observed only in the sample with x=0.175. The results of experiments carried out with a series of La_1?xSr_xMnO_3?x/2 anion-deficient solid solutions are summarized in the concentration diagrams of the spontaneous magnetic moment and the critical temperature of magnetic phase transitions. Hypothetical magnetic phase states are pointed out. The experimental results obtained can be interpreted in terms of the phase-separation model and the competition between ferromagnetic and antiferromagnetic indirect superex-change interactions. It is assumed that Mn³⁺-O-Mn³⁺ indirect superexchange interactions in the orbitally disordered phase are positive in the case of octahedral coordination of manganese ions and are negative when the coordination of at least one Mn³⁺ ion is pentahedral.     

Transport properties in La<Subscript>0.7−<Emphasis Type="Italic">x</Emphasis></Subscript>Gd<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> system

The influence of Gd doping at La-site on the electrical transport properties and the colossal magnetoresistance of La_0.7−x Gd _x Sr_0.3MnO₃ (x=0.00, 0.10, 0.15, 0.20, 0.30, 0.40, 0.50, 0.60, and 0.70) is studied. The experimental results indicate that the transport properties exhibit abnormal behavior under high doping condition. Forx=0.50, we find that a transition from metal to insulator occurs after the occurrence of insulator-metal transition nearT _c, which seldom occurs in ABO₃ structure. For samplesx=0.60 and 0.70, it exhibits insulator behavior far aboveT _c. These abnormal behaviors are attributed to different magnetic background, i.e. the system undergoes a transition from long range ferromagnetic order to the cluster-spin glass state and further to antiferromagnetic order.     

Magnetocaloric properties of La<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>K<Emphasis Type="Italic">x</Emphasis>MnO<Subscript>3</Subscript> manganites

A technology for obtaining single-phase ceramic samples of La_{1 − x} K _x MnO₃ manganites, as well as the dependence of their structure parameters on the potassium content, is described. The magnetocaloric effect in the samples has been measured by two direct methods, the classical method and the magnetic field modulation method, and has been calculated from the specific heat data. The values of the magnetocaloric effect obtained by these methods are significantly different. The observed discrepancies have been explained. Correlation between the doping level and the value of the effect has been found. It has been shown that the magnetic-field dependence of variation of the magnetic entropy near T _C in weak fields corresponds to theoretical calculations and that the value of the magnetocaloric effect in high magnetic fields can be predicted using this dependence.     

Colossal room-temperature magnetoresistance in thin La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Ag<Subscript>y</Subscript>MnO<Subscript>3</Subscript> epitaxial films

The first thin La_1?xAg_yMnO₃ epitaxial films (_y ≤ x) were grown on SrTiO₃ (110) substrates with silver present in the ionized state (Ag⁺) only. The Curie temperatures T_C of the compositions with x = y = 0.05, x = y = 0.1, and x = 0.3 and y = 0.27 crystallizing in the hexagonal structure \(R\bar 3c\) above or close to room temperature. The temperature dependences of electrical resistivity ρ and of magnetoresistance ¦Δρ/ρ/¦ = ¦(ρ_H ? ρ _H = 0)/ρ_H=0¦ pass through maxima near T_C, with the magnetoresistance being negative and reaching colossal values of ～7–20% in a magnetic field H = 8.2 kOe not only at T_C but also at room temperature. The magnetic moment per formula unit as derived from the saturation magnetization at T = 5 K is substantially smaller than expected for complete ferromagnetic ordering. The magnetization in fields of up to 6 kOe depends on the actual sample cooling conditions, and the hysteresis loop of a field-cooled sample is displaced along the H axis by ΔH. The above properties can be accounted for by the fact that the films are in a two-phase magnetic (ferromagnetic-antiferromagnetic) state induced by strong s-d exchange. The maximum value of Δ H was used to calculate the energy of exchange coupling between the ferromagnetic and antiferromagnetic parts of a sample.     

Thermal and magnetic properties of La<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>Pb<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript>

The thermodynamic and magnetic properties of the La_{1 − x} Pb _x MnO₃ (0.24 ≤ x ≤ 0.40) solid solution system were investigated in the temperature range of 4.2–340 K. All objects were ferromagnetics with Curie temperature T _C ≈ 320–340 K, which slowly increased with x. The M(T) behavior in the magnetic ordering region indicated a nonuniform ground state, due possibly to the competition of ferromagnetic and antiferromagnetic interactions. The increase in the saturation magnetic moment with x can be described by a simple model of the binary bonds in La_{1 − x} Pb _x MnO₃.     

Theory of the giant magnetoresistance in La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>A<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript>

To clarify the origin of the giant magnetoresistance (GMR) observed in La_1?x A _x MnO₃ (A²⁺=Sr²⁺, Pb²⁺, Ba²⁺ and Ca²⁺), we have investigated theoretically the electrical resistivity ρ of carriers in the background of Mn spins which interact with each other through the double exchange interaction. It has been found that extraordinarily large pin fluctuations caused by the instability of the ferromagnetic state are responsible for the transport anomalies including the GMR.     

Magnetic capacitance of the Gd<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>Bi<Subscript>1–<Emphasis Type="Italic">x</Emphasis></Subscript>FeO<Subscript>3</Subscript> thin films

The capacitance, inductance, and dissipation factor of the Gd _x Bi_1–x FeO₃ films were measured in the temperature range of 100 K < T < 800 K in magnetic fields of up to 8 kOe at frequencies of 0.1–100 kHz. The magnetic susceptibility maxima in the low-temperature region and dependences of the relaxation time and inductance on prehistory of the films cooled in zero and nonzero magnetic fields are established. The giant increase in magnetic capacitance in the external bias electric field is found. The results obtained are explained by the domain structure transformation in external electric and magnetic fields.     

Short-Range order of TlIn<Subscript>1–<Emphasis Type="Italic">x</Emphasis></Subscript>Sn<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>Te<Subscript>2</Subscript> thin films

The formation of the short-range order structure of amorphous nanometer-thick TlIn_1–x Sn _x Te₂ films (х = 0.02–0.09) obtained via vacuum deposition onto substrates of fresh KCl and KJ chips and celluloid at a temperature below Т = 213 K is studied by high-energy electron diffraction. Both freshly deposited films and films held in vacuum (10^–2 Pa) at room temperature in darkness for several months are studied. The effect of the tin concentration on the interatomic distances, the coordination numbers, and the time of amorphous phase stability of TlIn_1–x Sn _x Te₂ films due to a great spread in bond lengths and bond angles is established.     

Spin-glass like behaviors in La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Tb<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> perovskite

A series of samples of La_1−x Tb _x MnO₃ (0⩽x⩽0.15) are prepared. The static and dynamic magnetizations of La_1−x Tb _x MnO₃ have been investigated. The results indicate that the spins with the short-range order are frozen into random direction at low enough temperatures which leads to the samples exhibiting the spin-glass like behavior. It is considered that the spin-glass like behavior originates from the competition between ferromagnetic double exchange among Mn³⁺ and Mn²⁺ and antiferromagnetic superexchange among Mn³⁺ and Mn³⁺, as well as Tb³⁺ and Tb³⁺.     

Polarization characteristics of graded thick Ba<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>TiO<Subscript>3</Subscript> films

The barium strontium titanate ceramics Ba_{1 − x} Sr _x TiO₃ with a spatially variable composition has been prepared according to the thick film technology (tape casting). The strontium content over the film thickness is varied from 0 to 30 mol %. The structure and polarization characteristics of the samples prepared have been investigated. It has been found that the polarization characteristics of multilayer structures are determined by the ratio between the thicknesses of layers with different compositions and by their properties. No shift of the hysteresis loops in the graded thick Ba_{1 − x} Sr _x TiO₃ ( _x = 0–0.3) films has been revealed. The results obtained have been analyzed in the framework of modern theoretical approaches.     

Magnetocaloric effect in sandwich structures of La<Subscript>1–<Emphasis Type="Italic">x</Emphasis> </Subscript>K<Subscript> <Emphasis Type="Italic">x</Emphasis> </Subscript>MnO<Subscript>3</Subscript> manganites

This paper reports on the results of the investigation into the magnetocaloric properties of sandwich structures of La_1–xK_xMnO₃ manganites with x = 0.11 (LKM11), 0.13 (LKM13), and 0.15 (LKM15) in magnetic fields of up to 18 kOe. The results of the analysis of the field and temperature dependences of the magnetocaloric effect in the structures LKM11 + LKM13 and LKM13 + LKM15 have demonstrated that the use of sandwich structures increases the efficiency of magnetic cooling in a magnetic field of 18 kOe by 45%.     

Non-linear optical properties of (Pb<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>)TiO<Subscript>3</Subscript> thin films

Thin films of (Pb_1−x Sr _x )TiO₃, x=0,0.5,1.0 have been prepared on glass substrates by the chemical-solution method using the spin-coating technique. The optical nonlinearity in the visible spectral region is investigated using short (5 ns) laser pulses at the off-resonant wavelength of 532 nm employing the open aperture z-scan technique. It is found that the third order nonlinear absorption is dependent on the lead content of the films, with the compositions x=0, 0.5 exhibiting large values (β∼10⁻⁷ m/W), thereby suggesting the possible use of these materials as optical limiters. No optical nonlinearity is observed for the composition with x=1.0.     

Magnetic phase transitions in Nd<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Ca<Emphasis Type="Italic">x</Emphasis>MnO<Subscript>3</Subscript> manganites

The magnetic properties of manganites of the Nd_1?xCa_xMnO₃ system with x≤0.15 have been studied. It is shown that, in the 0.06≤x≤0.1 interval, the results can be interpreted using a model according to which the concentrational transition from a weakly ferromagnetic (WFM) state (x=0) to a ferromagnetic (FM) state (x>0.15) proceeds via a mixture of the exchange-coupled FM and WFM phases. In the vicinity of T=9 K, samples with 0.06≤x≤0.1 exhibit a spontaneous magnetic phase transition involving reorientation of the magnetization vectors of the WFM and the exchange-coupled FM phases. In the temperature interval between 5 and 20 K, a sample with the composition Nd^0.92Ca^0.08MnO^2.98 exhibits metamagnetic behavior. Magnetic phase diagrams in the H?T and T?x coordinates are presented. The appearance of the spin-reorientation transitions is explained in terms of the magnetic analog of the Jahn-Teller effect with allowance for the fact that, according to the neutron diffraction data, the magnetic moments of neodymium ions in the FM phase are parallel to the magnetic moments of manganese ions.     

Hall effect in La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript>x</Subscript>MnO<Subscript>3</Subscript> crystals

A study of the temperature dependences of the ordinary and anomalous Hall coefficients and of the Hall mobility of carriers in single crystals of the ferromagnetic manganites La_1?xSr_xMnO₃ (x=0.15, 0.20, 0.25) was carried out in the temperature interval from 85 to 400 K. The nature of the carriers and the conduction mechanisms in these compounds are discussed.     

The magnetic properties of nanosized La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Ca<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> (0.5 ≤ <Emphasis Type="Italic">x</Emphasis> ≤ 0.8)

Magnetic properties of La_1−x Ca _x MnO₃ (0.5 ≤ x ≤ 0.8) samples with an equivalent average particle size ~50 nm prepared by a sol–gel method were investigated. The charge ordering (CO) transition that is observed in the bulks disappears and the ferromagnetic (FM) transition occurs in all the prepared samples. For all the samples, the spontaneous magnetization (M _S) value is much lower than the corresponding theoretic value, which shows that the majority of the sample is antiferromagnetic (AFM). However, the M _S value is much larger than the corresponding value reported by some other groups. The invisible of CO transition and the large M _S value can be attributed to the good connection among the adjacent particles. Moreover, the exchange bias (EB) phenomenon is observed except the x = 0.5 sample. With x increasing, the M _S value decreases and the EB field increases, which can be understood by considering the coexistence of FM phase with Mn³⁺–Mn⁴⁺ spin clusters in the shell and the AFM phase in the core of the nanoparticles.     

Evolution of magnetooptical and transport properties of La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Ag<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> films depending on silver concentration

Evolution of optical, magnetooptical, and transport properties of La_1?x Ag _x MnO₃/SrTiO₃ epitaxial films depending on the silver concentration (x = 0.05, 0.10, 0.15, and 0.25) is studied. The highest values of the Curie temperature (T _C ≈ 317 K), magnetoresistance (～16%), magnetotransmission (～8%), and transverse Kerr effect (δ ～ 20 × 10^?3) are attained for a concentration x = 0.10 of Ag⁺ ions. Comparison of the temperature dependences of the transmission of IR radiation, resistivity, magnetotransmission, magnetoresistance, and Kerr effect indicates electronic and magnetic inhomogeneity of the films in spite of saturation of films with silver. This feature of the film state is explained using the concepts of epitaxial stresses and metastable point defects.     

Heat capacity and magnetocaloric properties of La<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>K<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> manganites

The magnetocaloric effect and the heat capacity of La_{1 − x} K _x MnO₃ (x = 0.1, 0.15, 0.175) ceramic samples have been studied at temperatures in the range 77–350 K and in magnetic fields of up to 27 kOe. The technique for preparing the samples has been described. The heat capacity anomalies related to the ferromagnetic-paramagnetic magnetic phase transition have been revealed and interpreted. It has been demonstrated that the change in the magnetic entropy ΔS calculated from the data on the heat capacity C _p and direct measurements of the magnetocaloric effect ΔT reaches values that are of practical interest.     

Relationship between the magnetoresistance and the magnetocaloric effect in La<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>Ag<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> manganites

A generalized expression relating the magnetoresistance of manganites La_{1 − x} Ag _x MnO₃ with the change in the magnetic entropy has been proposed. The correct inclusion of the acting mechanisms of appearance of the magnetoresistance is shown to lead to adequate agreement between the experimental and calculated values of ΔS _M .     

Magnetic Properties of a Layered Cobaltite Sr<Subscript>1–<Emphasis Type="Italic">x</Emphasis></Subscript>Y<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>CoO<Subscript>3–δ</Subscript> (<Emphasis Type="Italic">x</Emphasis> = 0.1)

The structure, the magnetic and magnetotransport properties of perovskite Sr_0.9Y_0.1CoO_2.63 have been studied. The sample is shown to have a two-phase structure. The main phase has a tetragonally distorted unit cell and is described by space group I4/mmm. The broadening of the reflections with indices corresponding to doubling unit cell parameter c indicates the absence of the rigorous translation symmetry along axis c. The existence of the broadened superstructure reflection observed in the diffraction pattern at small angles at temperature lower than 400 K is explained by the existence of the monoclinic phase whose content is significantly lower than that of the tetragonal phase, but is dominant in the Sr_0.8Y_0.2CoO_3–δ composition. The spontaneous magnetization appears as the monoclinic phase forms. The magnetic structure is mainly G-type antiferromagnetic with magnetic moments 1.5μ_B in the layers of CoO₆ octahedra and 2μ_B in the anion-deficit CoO_{4 + γ} layers. The conduction of the Sr_0.9Y_0.1CoO_2.63 composition has a semiconducting character. The magnetoresistance is 57% in a field of 14 T at a temperature of 5 K and strongly decreases with the temperature increase.     

Magnetic-field-induced change in optical transmission spectra of Hg<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>Cd<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>Te epitaxial films

The optical transmission spectra of epitaxial Hg_{1 − x} Cd _x Te films with a gradient of the band gap have been studied experimentally. The possibility of transforming the spectra after exposure of the samples to a homogeneous magnetic field has been demonstrated. This effect is possibly caused by the dependence of the magnetization of the Hg_{1 − x} Cd _x Te films on the composition gradient of the solid solution.