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.     

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.     

Magnetoresistance of La<Subscript>0.67</Subscript>Sr<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> epitaxial films grown on a substrate with low lattice mismatch

The structure, electrical resistivity, and magnetoresistance of La_0.67Sr_0.33MnO₃ heteroepitaxial films (120-nm thick) practically unstrained by lattice mismatch with the substrate were studied. A strong maximum of negative magnetoresistance of ≈27% (for μ₀H = 4 T) was observed at T ≈360 K. While the magnetoresistance decreased monotonically in magnitude with decreasing temperature, it was still in excess of 2% at 150 K. For T < 250 K, the temperature dependence of the electrical resistivity ρ of La_0.67Sr_0.33MnO₃ films is fitted well by the relation ρ = ρ₀ + ρ ₁(H)T^2.3, where ρ₀ = 1.1×10^?4 Ω cm, ρ₁(H = 0) = 1.8×10^?9 Ω cm/K^2.3, and ρ₁(μ₀H = 4 T)/ρ₁(H = 0) ≈0.96. The temperature dependence of a parameter γ characterizing the extent to which the electrical resistivity of the ferromagnetic phase of La_0.67Sr_0.33MnO₃ films is suppressed by a magnetic field (μ ₀H = 5 T) was determined.     

The 2<Superscript>1/3</Superscript> rule and other properties of ferromagnets near the temperature of the maximum of magnetic susceptibility

The behavior of the magnetization M and the magnetic susceptibility χ is theoretically analyzed for ferromagnets at the temperature T=T _m corresponding to the maximum of the function χ(T). Four new methods of determining the Curie temperature T_C with the use of the derived relationships are proposed. One of these methods is based on the relationship χ(T _m ) =2^1/3χ(T_C) (the 2^1/3 rule). The results are applied for processing experimental data obtained for lanthanum manganite of composition La_0.85Sr_0.15MnO₃.     

Response of the electrical resistivity and magnetoresistance of La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> films to biaxial tensile strains

The structure, electrical resistivity, and magnetoresistance of (50-nm)La_0.67Ca_0.33MnO₃ epitaxial films grown on a [(80 nm)Ba_0.25Sr_0.75TiO₃/La_0.3Sr_0.7Al_0.65Ta_0.35O₃] substrate with a substantial positive lattice misfit have been studied. The tensile biaxial strains are shown to account for the increase in the cell volume and in the relative concentration of Mn⁺³ ions in the manganite films as compared to those for the original material (33%). The peak in the temperature dependence of the resistivity ρ of La_0.67Ca_0.33MnO₃ films was shifted by 30–35 K toward lower temperatures relative to its position in the ρ(T) graph for a manganite film grown on (001)La_0.3Sr_0.7Al_0.65Ta_0.35O₃. For T < 150 K, the temperature dependences of ρ of La_0.67Ca_0.33MnO₃/Ba_0.25Sr_0.75TiO₃/La_0.3Sr_0.7Al_0.65Ta_0.35O₃ films could be well fitted by the relation ρ = ρ₀ + ρ₁T^4.5, where ρ₀ = 0.35 mΩ cm and the coefficient ρ₁ decreases linearly with increasing magnetic field. In the temperature interval 4.2–300 K, the magnetoresistance of manganite films was within the interval 15–95% (μ₀H = 5 T).     

Effect of a magnetic field on the thermal and kinetic properties of the Sm<Subscript>0.55</Subscript>Sr<Subscript>0.45</Subscript>MnO<Subscript>3.02</Subscript> manganite

The temperature and magnetic-field dependences of the heat capacity, thermal conductivity, thermopower, and electrical resistivity of the Sm_0.55Sr_0.45MnO_3.02 ceramic material are studied in the temperature range 77–300 K and in magnetic fields up to 26 kOe. It is revealed that the quantities under investigation exhibit anomalous behavior due to a magnetic phase transition at the Curie temperature T_C. An increase in the magnetic field strength H leads to an increase in the Curie temperature T_C and a jump in the heat capacity ΔC_p at T_C. The temperature dependences of the measured quantities are characterized by hystereses that are considerably suppressed in a magnetic field of 26 kOe and depend neither on the thermocycling range nor on the rate of change in the temperature. The thermal conductivity K at temperatures above T_C shows unusual behavior for crystalline solids (dK/dT>0) and, upon the transition to a ferromagnetic state, drastically increases as a result of a decrease in the phonon scattering by Jahn-Teller distortions. It is demonstrated that the hystereses of the studied properties of the Sm_0.55Sr_0.45MnO_3.02 manganite are caused by a jumpwise change in the critical temperature due to variations in the lattice parameters upon the magnetic phase transition.     

Response of the electrical resistivity of La<Subscript>0.67</Subscript>Ba<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript>(20 nm)/LaAlO<Subscript>3</Subscript>(001) films to magnetic field and variation in temperature

The structure, electrical resistivity, and magnetotransport parameters of 20-nm-thick epitaxial La_0.67Ba_0.33MnO₃ films grown by laser ablation on LaAlO₃(001) substrates are studied. The unit cell volume V _eff = 58.80 ų of the as-grown manganite films is found to be less than that for bulk La_0.67Ba_0.33MnO₃ crystals. Maximum values of the negative magnetoresistance MR(μ₀ H = 1 T) = ?0.27 for La_0.67Ba_0.33MnO₃ films are observed at a temperature of about 225 K. For 5 < T < 100 K, the film magnetoresistance depends only weakly on temperature and is on the order of ?0.1. At temperatures below 100 K and for 3 < μ₀ H < 5 T, the electrical resistivity of the as-grown films decreases linearly with increasing magnetic field.     

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.     

Adiabatic calorimetric study of the intense magnetocaloric effect and the heat capacity of (La<Subscript>0.4</Subscript>Eu<Subscript>0.6</Subscript>)<Subscript>0.7</Subscript>Pb<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript>

The temperature dependences of the intense magnetocaloric effect ΔT _AD(T, H) and the heat capacity C _p (T) of the (La_0.4Eu_0.6)_0.7Pb_0.3MnO₃ manganite are directly measured using adiabatic calorimetry. The experimental dependences ΔT _AD(T) are in satisfactory agreement with those calculated from the data on the behavior of the magnetization. The factors responsible for the absence of an anomaly in the experimental temperature dependence of the heat capacity C _p (T) in the range of the magnetic phase transition are discussed.     

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.     

Improved Scaling of the Magnetic Heat Capacity in La<Subscript>0.85</Subscript>Ag<Subscript>0.15</Subscript>MnO<Subscript>3</Subscript> Manganite

The heat capacity in a La_0.8 Ag_0.15 MnO₃ manganite has been measured near the Curie temperature T _C in applied magnetic fields up to 26 kOe to study the scaling critical behavior and to obtain the universality class. The conventional scaling fails in application to the manganites with a hysteresis and the strong sensitivity of T _C to a magnetic field. However, the application of the improved scaling procedure designed by us allows yielding the good scaling the magnetic heat =0.23 capacity in La_0.85Ag_0.15MnO₃, which may belong to a new universality class for systems with the strong spin-orbital coupling of t _2g -electrons, namely, double -Heisenberg with the critical exponent of the heat capacity α = ?0.23 and the critical exponent of the correlation radius v=0.7433. This new universality class is consistent with the crystal, magnetic and orbital symmetries for the La_0.85Ag_0.15MnO₃. Scaling failure in the vicinity of T _C in the range of t/H ^1/2ν ≈ [?0.033;0.024] is understood by finite-size and other disordering effects when T →T _C. It is remarkable that finite-size effect is consistent with grain size, L ≈ 50 μm, in the La_0.85Ag_0.15MnO₃. The correlation radius, Lt ^ν ≈ 30.28 Å, estimated from the finite-size effect is of the same order of magnitude with the sizes of the ferromagnetic fluctuations and drops in manganites.     

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.     

Electrical resistivity and magnetotransport properties of La<Subscript>0.67</Subscript>Ba<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> epitaxial films biaxially compressed by the substrate

The structure, electrical resistivity, and magnetoresistance of La_0.67Ba_0.33MnO₃(20 nm) films grown coherently on an La_0.3Sr_0.7Al_0.65Ta_0.35O₃(001) substrate with a lattice misfit of about 1% were studied. The rigid connection of the manganite layer with the bulk substrate brought about the unit cell distortion of the substrate (a _⊥/a _‖ = 1.02) and a decrease in the unit cell volume as compared to that of the corresponding bulk crystals (a _‖ and a _⊥ are the unit cell parameters measured in the substrate plane and along the surface normal, respectively). The temperature T _M ≈ 295 K, at which the electrical resistivity ρ of the (20 nm)La_0.67Ba_0.33MnO₃ films reached a maximum, was 40–45 K lower than that for the corresponding bulk crystals. The negative magnetoresistance (MR ≈ ?0.25 for μ₀ H = 1 T) attained a peak value at T _MR ≈ 270 K. The response of ρ to a magnetic field depended substantially on the angle between the current flow in the film and the direction of the magnetic field.     

The giant volume magnetostriction and colossal magnetoresistance in Eu<Subscript>0.55</Subscript>Sr<Subscript>0.45</Subscript>MnO<Subscript>3</Subscript> manganite

A doped manganite with the composition Eu_0.55Sr_0.45MnO₃ exhibits giant negative magnetostriction and colossal negative magnetoresistance at temperatures in the vicinity of the magnetic phase transformation (T～41 K). In the temperature interval 4.2 K≤T ≤40 K, the isotherms of magnetization, volume magnetostriction, and resistivity exhibit jumps at the critical field strength H_c1, which decreases with increasing temperature. At 70 K ≤T ≤120 K, the jumps on the isotherms are retained, but the shapes of these curves change and the H_c1 value increases with the temperature. At H<H_c1, the magnetoresistance is positive and exhibits a maximum at 41 K; at H>H_c1, the magnetoresistance becomes negative, passes through a minimum near 41 K and then reaches a colossal value. The observed behavior is explained by the existence of three phases in Eu_0.55Sr_0.45MnO₃, including a ferromagnetic (in which the charge carriers concentrate due to a gain in the s-d exchange energy) and two antiferromagnetic phases (of the A and CE types). The volumes of these phases at low temperatures are evaluated. It is shown that the colossal magnetoresistance and the giant volume magnetostriction are related to the ferromagnetic phase formed as a result of the magnetic-field-induced transition of the CE-type antiferromagnetic phase to the ferromagnetic state.     

Electrical resistivity and magnetotransport in La<Subscript>0.67</Subscript>Ba<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> films asymmetrically biaxially compressed by an NdGaO<Subscript>3</Subscript>(001) substrate

The La_0.67Ba_0.33MnO₃(40 nm) films are quasi-coherently grown on an NdGaO₃(001) substrate with an orthorhombic unit cell distortion of ～1.4%. The biaxial compressive stresses generated during nucleation and growth lead to a decrease in the unit cell volume of the grown layers. This, in turn, results in a decrease (by ～35 K) in the temperature of the maximum in the dependence of the electrical resistivity ρ of the layers on the temperature. For T < 150 K, the electrical resistivity ρ of the films increases in proportion to ρ₂ T ^4.5 and the coefficient ρ₂ decreases almost linearly with increasing magnetic field H. The negative magnetoresistance (≈?0.17 for μ₀ H = 1 T) reaches a maximum at temperatures close to room temperature. The response of the electrical resistivity ρ of the La_0.67Ba_0.33MnO₃(40 nm) films to the magnetic field depends on the crystallographic direction of the film orientation and the angle between H and I (where I is the electric current through the film).     

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.     

Heat capacity of the La<Subscript>0.9</Subscript>Ag<Subscript>0.1</Subscript>MnO<Subscript>3</Subscript> manganite near the curie temperature

The heat capacity of the La_0.9Ag_0.1MnO₃ manganite is measured in the temperature range 77–350 K and studied in detail in the vicinity of the Curie temperature for the first time. The regularities of the variation in the universal critical parameters in the vicinity of the phase transition point are established. The critical exponent and the amplitude of the heat capacity are calculated to be α = ?0.127 and A ⁺/A ^? = 1.146 with due regard for the scaling corrections. These parameters correspond to the critical behavior within the three-dimensional Heisenberg model. The size of ferromagnetic droplets in the paramagnetic range at T > T _C is estimated as ξ ≈ 19 Å. The results obtained are analyzed thoroughly and compared with theoretical data for a number of model systems.     

Multifrequency electron spin resonance study of the charge-ordered manganite Nd<Subscript>0.5</Subscript>Ca<Subscript>0.5</Subscript>MnO<Subscript>3</Subscript>

We performed multifrequency electron spin resonance (ESR) on the antiferromagnetic (T_N = 160 K) and charge-ordered (T _co = 250 K) insulating manganite Nd_0.5Ca_0.5MnO₃. Temperature (4–300 K) and frequency (9.4–285 GHz) dependence of the linewidth, intensity and position of the ESR line were studied. In the paramagnetic state we observe a single Lorentzian absorption line. For a given frequency, the ESR line position is temperature independent (close tog = 1.99). A strong linewidth broadening is observed below T_co. This indicates that there is no magnetic order in the temperature rangeT _cos>T >T _N but strong antiferromagnetic fluctuations are present. Below T_N, due to high-frequency and high-field ESR (up to 12 T) measurements, we were able to observe unexpected lines within the antiferromagnetic gap revealing the presence of a phase separation.     

Magnetization of La- and Ce-doped CaMnO<Subscript>3</Subscript> manganite single crystals in a strong magnetic field

Studies of the magnetization curves of electron-doped single-crystal manganites Ca_{1 ? x} Ln _x MnO₃ (Ln = La³⁺, Ce⁴⁺; x ≤ 0.12) in strong pulsed magnetic fields of up to 350 kOe have revealed a metamagnetic transition in Ca_0.9Ce_0.1MnO₃ in the temperature range 77–190 K. The critical transition fields increase to ～350 kOe with the temperature decreasing to 100 K. The spin polarization is ～50% of the theoretical value. These results are interpreted as due to “melting” of the orbital/charge ordering below the temperature T _OO/CO = 185 K = T _N (of the C type AFM phase); this entails a decrease in the volume of the ordered phase with localized carriers and an increase in the volume of the ferromagnetic phase with delocalized carriers. The temperature and field dependences of the magnetization are used to compare two manganite systems in the region of the two-phase magnetic state.     

Peculiarities of magnetic,galvanomagnetic, elastic,and magnetoelastic properties of Eu<Subscript>0.55</Subscript>Sr<Subscript>0.45</Subscript>MnO<Subscript>3</Subscript>

Magnetic, elastic, magnetoelastic, transport, and magnetotransport properties of the Eu_0.55Sr_0.45MnO₃ ceramics have been studied. A break was detected in the temperature dependence of electrical resistivity ρ(T) near the temperature of the magnetic phase transformation (41 K), with the material remaining an insulator down to the lowest measurement temperature reached (ρ=10⁶ Ω cm at 4.2 K). In the interval 4.2≤T≤50 K, the isotherms of the magnetization, volume magnetostriction, and ρ were observed to undergo jumps at the critical field H_C1, which decreases with increasing T. For 50≤T≤120 K, the jumps in the above curves persist, but the pattern of the curves changes and H_C1 grows with increasing T. The magnetoresistance Δρ/ρ = (ρ _H ?ρ_H=0)/ρ _H is positive for H<H_C1 and passes through a maximum at 41 K, where Δρ/ρ = 6%. For H>H_C1, the magnetoresistance is negative, passes through a minimum near 41 K, and reaches a colossal value of 3×10⁵ % at H=45 kOe. The volume magnetostriction is negative and attains a giant value of 4.5×10^?4atH=45 kOe. The observed properties are assigned to the existence of three phases in Eu_0.55Sr_0.45MnO₃, namely, a ferromagnetic (FM) phase, in which carriers are concentrated because of the gain in s-d exchange energy, and two antiferromagnetic (AFM) phases of the A and CE types. Their fractional volumes at low temperatures were estimated to be as follows: ～3% of the sample volume is occupied by the FM phase; ～67%, by the CE-type AFM phase; and ～30%, by the A-type AFM phase.