Magnetic state of the structural separated anion-deficient La<Subscript>0.70</Subscript>Sr<Subscript>0.30</Subscript>MnO<Subscript>2.85</Subscript> manganite

The results of neutron diffraction studies of the La_0.70Sr_0.30MnO_2.85 compound and its behavior in an external magnetic field are stated. It is established that in the 4–300 K temperature range, two structural perovskite phases coexist in the sample, which differ in symmetry (groups R[`3]cR\bar 3c and I4/mcm). The reason for the phase separation is the clustering of oxygen vacancies. The temperature (4–300 K) and field (0–140 kOe) dependences of the specific magnetic moment are measured. It is found that in zero external field, the magnetic state of La_0.70Sr_0.30MnO_2.85 is a cluster spin glass, which is the result of frustration of Mn³⁺-O-Mn³⁺ exchange interactions. An increase in external magnetic field up to 10 kOe leads to fragmentation of ferromagnetic clusters and then to an increase in the degree of polarization of local spins of manganese and the emergence of long-range ferromagnetic order. With increasing magnetic field up to 140 kOe, the magnetic ordering temperature reaches 160 K. The causes of the structural and magnetic phase separation of this composition and formation mechanism of its spin-glass magnetic state are analyzed.     

Critical behavior of La<Subscript>0.825</Subscript>Sr<Subscript>0.175</Subscript>MnO<Subscript>2.912</Subscript> anion-deficient manganite in the magnetic phase transition region

For La _0.825 ³⁺ Sr _0.175 ² +Mn³⁺O _2.912 ^2? anion-deficient manganite, the specific magnetization, the dynamic magnetic susceptibility, and the heat capacity are investigated. This material is found to be an inhomogeneous ferromagnet below the Curie point T _C ≈ 122 K, which is much lower than the Curie point determined for the stoichiometric composition (T _C ≈ 268 K). An increase in magnetic field by two orders of magnitude leads to an increase in the Curie temperature by ΔT ≈ 12 K. The presence of oxygen vacancies leads to the frustration of a part, namely, V _fr ≈ 22%, of the indirect Mn³⁺-O-Mn³⁺ exchange interactions, but the spin glass state is not realized. The ferromagnetic matrix of the material under study is characterized by a scatter in the exchange interaction intensities. The heat capacity is found to exhibit an anomalous behavior. Based on the Banerjee magnetic criterion, it is established that the ferromagnet-paramagnet transition observed for La _0.825 ³⁺ Sr _0.175 ²⁺ Mn³⁺O _2.912 ^2? anion-deficient manganite is a second-order thermodynamic phase transition. The mechanism and origin of the critical behavior of the system under investigation are discussed.     

Magnetic properties of La0.70Sr0.30MnO2.85 anion-deficient manganite under hydrostatic pressure

The magnetic properties of La_0.70Sr_0.30MnO_2.85 anion-deficient manganite are studied experimentally under hydrostatic pressure. The results show that, in the whole pressure range under investigation (0–1 GPa), the sample is a spin glass with a smeared phase transition to the paramagnetic state. It is found that the spin glass state arises from the frustration of the exchange coupling of the ferromagnetic clusters embedded in the antiferromagnetic matrix. The fraction of the sample volume occupied by the ferromagnetic phase is found to be V _fer ～ 13%. Under hydrostatic pressure, the freezing temperature T _f of the magnetic moments of the ferromagnetic clusters increases at a rate of 4.30 K/GPa and the magnetic ordering temperature T _MO increases at a rate of 12.90 K/GPa. In addition, the ferromagnetic part of the sample increases by ΔV _fer ～ 5%. The enhancement of the ferromagnetic properties of La_0.70Sr_0.30MnO_2.85 anion-deficient manganite under hydrostatic pressure is explained by the redistribution of oxygen vacancies and a decrease in the unit-cell parameters.     

Frustrated exchange interactions formation at low temperatures and high hydrostatic pressures in La<Subscript>0.70</Subscript>Sr<Subscript>0.30</Subscript>Mn<Subscript>O2.85</Subscript>

The magnetic and thermal properties of the anion-deficient La_0.70Sr_0.30MnO_2.85 manganite are investigated in wide temperature (4–350 K) range, including under hydrostatic pressure (0–1.1 GPa). Throughout the pressure range investigated, the sample is spin glass with diffused phase transition into paramagnetic state. It is established, that spin glass state is a consequence of exchange interaction frustration of the ferromagnetic clusters embeded into antiferromagnetic clusters. The magnetic moment freezing temperature T _f of ferromagnetic clusters increases under pressure, freezing temperature dependence on pressure is characterized by derivative value ∼4.5 K/GPa, while the magnetic ordering T _MO temperature dependence is characterized by derivative value ∼13 K/GPa. The volume fraction of sample having ferromagnetic state is V _fer ∼ 13% and it increases under a pressure of 1.1 GPa by ΔV _fer ≈ 6%. Intensification of ferromagnetic properties of the anion-deficient La_0.70Sr_0.30MnO_2.85 manganite under hydrostatic pressure is a consequence of oxygen vacancies redistribution and unit cell parameters decrease. The most likely mechanism of frustrated exchange interactions formation is discussed.     

Metal-insulator transition in a radiation-disordered La<Subscript>0.85</Subscript>Sr<Subscript>0.15</Subscript>MnO<Subscript>3</Subscript> manganite

The temperature dependences of the electrical resistivity ρ(T) and the ac magnetic susceptibility χ(T, H = 0) are thoroughly investigated for a perovskite-like lanthanum manganite, namely, La_0.85Sr_0.15MnO₃, which is preliminarily exposed to neutron irradiation with a fluence _F = 2 × 10¹⁹ cm^?2 and then annealed at different temperatures ranging from 200 to 1000°C. The results of the electrical resistance measurements demonstrate that neutron irradiation of the samples leads to the disappearance of the low-temperature insulating phase. As the annealing temperature increases, the insulating phase is not restored and the manganite undergoes a transformation into a metallic phase. Analysis of the magnetic properties shows that, under irradiation, the ferromagnet-paramagnet phase transition temperature T_C decreases and the magnetic susceptibility is reduced significantly. With an increase in the annealing temperature, the phase transition temperature T_C and magnetic susceptibility χ(_{T, H} = 0) increase and gradually approach values close to those for an unirradiated sample. This striking difference in the behavior of the electrical and magnetic properties of the radiation-disordered La_0.85Sr_0.15MnO₃ manganite is explained qualitatively.     

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.     

Features of acoustic wave propagation near the structural phase transition in the La<Subscript>0.875</Subscript>Sr<Subscript>0.125</Subscript>MnO<Subscript>3</Subscript> manganite

Features of the phase transition from the disordered state to the ordered orbital state in a La_0.875Sr_0.125MnO₃ single crystal, caused by the cooperative Jahn-Teller effect, have been investigated. A significant change in the acoustic wave parameters in the entire range of cooperative distortion of the structure is revealed. Application of an external magnetic field shifts the structural phase transition to low temperatures.     

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.     

Phase separation in a manganite La<Subscript>0.95</Subscript>Ba<Subscript>0.05</Subscript>MnO<Subscript>3</Subscript> crystal

The structure and magnetic states of a crystal of lightly doped manganite La_0.95Ba_0.05MnO₃ were studied using thermal-neutron diffraction, magnetic measurements, and electrical resistance data in a wide temperature range. It is shown that, in terms of its magnetic properties, the orthorhombic crystal is characterized by two order parameters, namely, antiferromagnetic (T _N = 123.6 K) and ferromagnetic (T _C = 136.7 K). The results obtained differ in detail from known information on the manganites La_0.95Ca_0.05MnO₃ and La_0.94Sr_0.06MnO₃. Two models of the magnetic state of the La_0.95Ba_0.05MnO₃ crystal are discussed, one of which is a model of a canted antiferromagnetic spin system and another is associated with the phase separation of the manganite. Arguments are advanced in favor of the coexistence in this crystal of the antiferromagnetic phase (about 87%) with a Mn⁴⁺ ion concentration of 0.048 and the 1/16-type charge-ordered ferromagnetic phase (about 13%) with a Mn⁴⁺ ion concentration of 0.0625. The specific features of the manganite studied are due to self-organization of the La_0.95Ba_0.05MnO₃ crystal lattice caused by the relatively large barium ion size.     

Acoustic and magnetic properties of La<Subscript>0.825</Subscript>Sr<Subscript>0.175</Subscript>MnO<Subscript>3</Subscript> lanthanum manganites

This paper reports on measurements of the acoustic, magnetic, and electrical properties and on an x-ray microprobe analysis of a La_0.825Sr_0.175MnO₃ single-crystal sample. The acoustic studies were made with a pulsed acoustic spectrometer operating on a 770-MHz carrier. The studies revealed anomalies in the damping coefficients and sound velocity near 300, 200 K, and the Curie temperature T_C (283 K) where the colossal magnetoresistance occurs. The effect of a magnetic field on the magnetic texture of lanthanum manganites cooled below T_C, observed earlier in samples of other composition, is confirmed. In addition, a region was found wherein the magnetic susceptibility of an unclamped sample behaves anomalously. The electrical resistivity was observed to decrease substantially below T_C; this effect exhibits a hysteretic pattern in the interval 200–180 K.     

Phase separation of the spin system in the La<Subscript>0.93</Subscript>Sr<Subscript>0.07</Subscript>MnO<Subscript>3</Subscript> crystal

The magnetic state of the manganite La_0.93Sr_0.07MnO₃ in the range 4.2–290 K was studied using elastic neutron scattering. The magnetic state of this compound was found to occupy a particular place in the La_1?xSr_xMnO₃ solid-solution system, in which the antiferromagnetic type of order (LaMnO₃, T_N=139.5 K) switches to ferromagnetic ordering (La_0.9Sr_0.1MnO₃, T_C=152 K) with increasing x. In the transition state, this compound contains large-scale spin configurations of two types. A fractional crystal volume of about 10% is occupied by regions of the ferromagnetic phase with an average linear size of 200 Å, while the remainder of the crystal is a phase with a nonuniform canted magnetic structure. Arguments are presented for the phase separation of the La_0.93Sr_0.07MnO₃ spin system being accounted for by Mn⁴⁺ ion ordering.     

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.     

Raman measurements on thin films of the La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> manganite: a probe of substrate-induced effects

We report on a Raman study of the phonon spectrum of La _0.7Sr_0.3MnO₃ thin films epitaxially grown on LaAlO₃. The spectrum, as a function of film thickness d, does not change over the 1000–100 ? range, whereas a strong hardening of the phonon frequencies of both bending and stretching modes is apparent in ultra-thin films (d<100 ?) where substrate-induced effects are remarkable. This behaviour, which appears to be related with the measured d-dependence of the insulator-to-metal transition temperature, is ascribed to co-operative effects of MnO₆ octahedra rotation and charge-localization. Raman spectroscopy proves to be a simple and powerful tool to monitor subtle structural modifications hardly detectable with conventional diffraction techniques in ultra-thin films.     

Magnetocaloric effect in the Sm<Subscript>0.55</Subscript>Sr<Subscript>0.45</Subscript>MnO<Subscript>3</Subscript> manganite

The magnetocaloric effect ΔT has been studied by a direct method in two samples of the manganite Sm_0.55Sr_0.45MnO₃, namely, a single crystal (sample A) and a ceramic sample (sample C). The temperature dependences of the ΔT effect of both samples exhibit a maximum at T _max = 143.3 K for the sample A and T _max = 143 K for the sample C. In these maxima, the values of the ΔT effect are 0.8 and 0.4 K in the magnetic field H = 14.2 kOe for the samples A and C, respectively. In addition, the ΔT(T) curve of the sample A has a minimum at T _min = 120 K, in which ΔT = −0.1 K. The maximum value of the ΔT effect increases with an increase in the magnetic field H in the range of magnetic fields up to 14.2 kOe, and the rate of this increase at H > 8 kOe is higher than that at H < 8 kOe. These features of the ΔT effect are explained by the presence of ferromagnetic and antiferromagnetic A- and CE-type clusters in the samples.     

The magnetic and hyperthermia studies of bare and silica-coated La<Subscript>0.75</Subscript>Sr<Subscript>0.25</Subscript>MnO<Subscript>3</Subscript> nanoparticles

The magnetic nanoparticles of La_0.75Sr_0.25MnO₃ perovskite manganite with a controlled size were prepared via sol–gel procedure, followed by thermal treatment and subsequent mechanical processing of the resulting raw product. The prepared materials were structurally studied by the XRD and TEM methods and probed by DC magnetic measurements. The nanoparticles of the mean crystallite sizes 11–40 nm exhibit T _C in the range of ≈310–347 K and the sample possessing 20-nm crystallites was identified as the most suitable for hyperthermia experiments. In order to obtain a colloidally stable suspension and prevent toxic effects, the selected magnetic cores were further encapsulated into silica shell using tetraethoxysilane. The detailed magnetic studies were focused on the comparison of the raw product, the bare nanoparticles after mechanical processing and the silica-coated nanoparticles, dealing also with effects of size distribution and magnetic interactions. The heating experiments were carried out in an AC field of frequencies 100 kHz–1 MHz and amplitude 3.0–8.9 kA m⁻¹ on water dispersions of the samples, and the generated heat was deduced from their warming rate taking into account experimentally determined thermal losses into surroundings. The experiments demonstrate that the heating efficiency of the coated nanoparticles is generally higher than that of the bare magnetic cores. It is also shown that the aggregation of the bare nanoparticles increases heating efficiency at least in a certain concentration range.     

Crystal and magnetic structures and physical properties of the Sm<Subscript>0.37</Subscript>Sr<Subscript>0.63</Subscript>MnO<Subscript>3</Subscript> manganite

The ¹⁵²Sm_0.37Sr_0.63MnO₃ manganite is investigated using neutron diffraction. The parameters of the crystal and magnetic structures of the manganite are determined. The diffraction data are compared with the transport and magnetic characteristics of this compound. A comparison is performed between the ¹⁵²Sm_0.37Sr_0.63MnO₃ and ¹⁵²Sm_0.45Sr_0.55MnO₃ manganites. Although these compounds differ insignificantly in the strontium doping level, are homogeneous antiferromagnets, and do not exhibit a colossal negative magnetoresistance, they have different crystal symmetries (tetragonal I4/mcm and orthorhombic Pnma), differ in the type of spin ordering (C-type antiferromagnetic and A-type antiferromagnetic ordering), are characterized by different orbital polarizations (\(d_{3z^2 - r^2 } \) and \(d_{x^2 - y^2 } \)), and possess one-and two-dimensional magnetic and transport properties, respectively. The critical concentration range in which samarium strontium manganites undergo a concentration structural transition from the orthorhombic to tetragonal crystal symmetry with a change in the type of orbital and magnetic order is revealed.     

Study of mechanochemically prepared nanocrystalline La<Subscript>0.8</Subscript>Sr<Subscript>0.2</Subscript>MnO<Subscript>3</Subscript>

The nanocrystalline La_0.8Sr_0.2MnO₃ (LSM) is prepared by varying the revolutions per minute and milling time of planetary monomill during the mechanochemical method. The LSM forms in a relatively shorter milling time with an increase in the milling speed from 250 to 600 rpm. The structural phase transition from orthorhombic to rhombohedral phase in the LSM prepared by ball milling at the speed 250 rpm for 36 h is seen due to sintering it at 700 °C for 4 h. The crystallite size reduces with the increase in both the milling speed and the milling time individually or combined. The microhardness (HV) and sintered density increase with the reduction in the crystallite size. The temperature-activated transition temperature is suppressed by reducing the grain size in the nanometer range. The electrical dc conductivity increases with the reduction in the grain/crystallite size.     

Acoustical investigations of a La<Subscript>0.75</Subscript>Sr<Subscript>0.25</Subscript>MnO<Subscript>3</Subscript> single crystal

The acoustical, resistive, and magnetic properties of a La_0.75Sr_0.25MnO₃ lanthanum manganite single crystal are investigated in the temperature range involving the second-order magnetic phase transition. The acoustical measurements are performed by the pulse-echo method in the frequency range 14–90 MHz. It is found that, as the temperature decreases, the velocity of a longitudinal acoustic wave propagating along the [111] axis in the single crystal drastically increases at temperatures below the critical point of the magnetic phase transition. No dispersion of the acoustic velocity is revealed. A sharp increase in the acoustic velocity is accompanied by the appearance of an acoustical absorption peak. The observed effects are discussed with due regard for the interaction of acoustic waves with the magnetic moments of the manganese ions.     

Magnetotransport properties of nano-constriction array in La<Subscript>0.67</Subscript>Sr<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> film

Nano-constriction array in La_0.67Sr_0.33MnO₃ film was fabricated by using ion beam etching masked by a monolayer of packed and ordered array of SiO₂ microspheres. Nano-constrictions of around 50 nm in width were fabricated. The low field magnetoresistance (LFMR) exhibited in the samples were observed to be current dependent and the I-V characteristics of the film were found to be nonlinear. These observations were attributed to the co-existence of the ferromagnetic regions and the nano-constricted region of weakened ferromagnetic coupling where Mn³⁺-O-Mn⁴⁺ bond were distorted due to the ion beam bombardment. The spin polarized bias current would strengthen local ferromagnetic coupling when passing through this nano-constricted regions. This current effect is relatively large comparing to the external magnetic field to the drop of resistance.     

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.