Nature of the low-energy excitations of a charge-ordered phase of La<Subscript>0.25</Subscript>Ca<Subscript>0.75</Subscript>MnO<Subscript>3</Subscript> manganites

The nature of the low-energy excitations of polycrystalline and nanostructured La_0.25Ca_0.75MnO₃ samples has been analyzed in order to investigate the mechanisms of charge ordering in manganites. It has been found that the electrodynamic response spectra of La_0.25Ca_0.75MnO₃ in the energy range of 0.5 to 90 meV and the temperature range of 5 to 300 K have no resonance features that could be attributed to the collective excitations of the charge-ordered phase. It has been shown that the absorption lines observed at frequencies of 20–40 and 80–100 cm^–1 are attributed to usual acoustic phonons becoming optically active owing to the structure phase transition and the appearance of a fourfold superstructure with a quadruple period along the crystallographic a axis. The suppression of the superstructure has been revealed in samples with nanocrystallites (≤40 nm). This suppression indicates a relatively weak coupling of the charge and magnetic order parameters with the phonon subsystem.     

Pressure-induced structural transformations,orbital order and antiferromagnetism in La<Subscript>0.75</Subscript>Ca<Subscript>0.25</Subscript>MnO<Subscript>3</Subscript>

High pressure evolution of structural, vibrational and magnetic properties of La_0.75Ca_0.25MnO₃ was studied by means of X-ray diffraction and Raman spectroscopy up to 39 GPa, and neutron diffraction up to 7.5 GPa. The stability of different magnetic ground states, orbital configurations and structural modifications were investigated by LDA + U electronic structure calculations. A change of octahedral tilts corresponding to the transformation of orthorhombic crystal structure from the Pnma symmetry to the Immaone occurs above P ~ 6 GPa. At the same time, the evolution of the orthorhombic lattice distortion evidences an appearance of the e _g d _{x² ? z²} orbital polarization at high pressures. The magnetic order in La_0.75Ca_0.25MnO₃ undergoes a continuous transition from the ferromagnetic 3D metallic (FM) ground state to the A-type antiferromagnetic (AFM) state of assumedly 2D pseudo-metallic character under pressure, that starts at about 1 GPa and extends possibly to 20–30 GPa.     

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.     

Structure and magnetoresistance of La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> films grown coherently on (001)NdGaO<Subscript>3</Subscript>

40-to 120-nm-thick (001)La_0.67Ca_0.33MnO₃ films grown through laser evaporation on (001)NdGaO₃ were studied. The lattice parameters of the La_0.67Ca_0.33MnO₃ films measured in the substrate plane (a_∥=3.851 Å) and along the normal to its surface (a_⊥=3.850 Å) practically coincided with that of the pseudocubic neodymium gallate. The unit-cell volume of the La_0.67Ca_0.33MnO₃ film was slightly smaller than that of stoichiometric bulk samples. The position of the maximum in the temperature dependence of electrical resistivity did not depend on the thickness of the La_0.67Ca_0.33MnO₃ film. The negative magnetoresistance (MR≈?0.25, H=0.4 T) of La_0.67Ca_0.33MnO₃ films reached a maximum at 239–244 K.     

Response of the electrical resistivity and magnetoresistance of La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> epitaxial films to biaxial compressive mechanical (001) or (110) strains

The behavior of the electrical resistivity and magnetoresistance of 40-to 120-nm-thick La_0.67Ca_0.33MnO₃ films grown on differently oriented lanthanum aluminate substrates was studied. The cell volume in thin (40 nm) La_0.67Ca_0.33MnO₃ films grown coherently on (001)LaAlO₃ was found to be substantially smaller. Mechanical stress relaxation in biaxially strained La_0.67Ca_0.33MnO₃ films is accompanied by an increase in the cell volume. The temperatures at which the electrical resistivity and magnetoresistance in biaxially strained La_0.67Ca_0.33MnO₃ films were maximum can differ by 60–70 K from those observed in bulk single crystals.     

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).     

Elastic and kinetic properties of single-crystal La<Subscript>0.75</Subscript>Ba<Subscript>0.25</Subscript>MnO<Subscript>3</Subscript>

An experimental study of the temperature behavior of longitudinal sound velocity, internal friction, electrical resistivity, and thermopower of single-crystal La_0.75Ba_0.25MnO₃ is reported. A structural transition accompanied by a large jump (18%) in the sound velocity was found to occur at T _S ≈170 K. Within the interval 156–350 K, the temperature dependences of the sound velocity and internal friction reveal a temperature hysteresis. An internal-friction peak due to relaxation processes was detected. The metallic and semiconducting regions are separated by a transition domain about 80 K wide lying below the Curie temperature T _C =300 K.     

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.     

Size effect in nanocrystalline manganites La<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript><Emphasis Type="Italic">A</Emphasis><Subscript>x</Subscript>MnO<Subscript>3</Subscript> (<Emphasis Type="Italic">A</Emphasis>=Ag,Sr)

Nanocrystalline samples of the manganites La_0.9Ag_0.1MnO₃, La_0.7Ag_0.3MnO₃, and La_0.7Sr_0.3MnO₃ were synthesized through pyrolysis and isothermally annealed. The atomic, subatomic, and magnetic structures of these manganites were studied using magnetic, x-ray, and neutron diffraction measurements. Increasing the annealing temperature from 600 to 1200°C coarsens the grains from 30–40 to 600–700 nm in size. All the samples studied have rhombohedral structure and are ferromagnets. The Curie temperature decreases for the samples doped by silver and increases for the samples doped by strontium as the anneal temperature is increased. The magnetization of the Mn ions increases with nanoparticle size in all the three systems, which indicates the presence of a size effect.     

Nature of EPR line asymmetry in La<Subscript>0.70</Subscript>Ca<Subscript>0.25</Subscript>Ba<Subscript>0.05</Subscript>MnO<Subscript>3</Subscript>

It was pointed out in some works that asymmetry of an electron paramagnetic resonance (EPR) line is generally caused by both the electrical conduction and the nondiagonal elements of the dynamic susceptibility of a magnetic subsystem. Direct measurements of the temperature dependences of the conductivity and the EPR line shape in a La_0.70Ca_0.25Ba_0.05MnO₃ sample showed that the conduction makes the predominant contribution to the EPR line asymmetry.     

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.     

Intrinsic metastability of low doped manganites: La<Subscript>0.8</Subscript>Ca<Subscript>0.2</Subscript>MnO<Subscript>3</Subscript> case

Transport properties of phase separated La_0.8Ca_0.2MnO₃ crystals in the aged highly resistive metastable state were studied. It was found that the coexistence of different ferromagnetic phases at low temperatures is sensitive to electric current/field. In a contrast with the previously studied low resistivity metastable states the high resistivity state exhibits positive magnetoresistance and significant current dependence of the resistivity even at temperatures much higher than the Curie temperature. Application of current pulses results in appearance of zero bias anomaly in the current dependent conductivity. Similarly to the low resistivity metastable states the memory of the resistivity can be erased only after heating of the sample to T_e ≈360 K. After one year storage at room temperature the La_0.8Ca_0.2MnO₃ samples show clear signatures of aging. The aged samples spontaneously evolute towards high resistivity states. The results are discussed in the context of a coexistence of two ferromagnetic phases with different orbital order and different conductivity. The metallic ferromagnetic phase seems to be less stable giving rise to the experimentally observed electric field effects and aging.     

High-precision measurements of the compressibility and the electrical resistivity of bulk <Emphasis Type="Italic">g</Emphasis>-As<Subscript>2</Subscript>Te<Subscript>3</Subscript> glasses at a hydrostatic pressure up to 8.5 GPa

High-precision studies of the volume and the electrical resistivity of g-As₂Te₃ glasses at a high hydrostatic pressure up to 8.5 GPa at room temperature are performed. The glasses exhibit elastic behavior in compression only at a pressure up to 1 GPa, and a diffuse structural transformation and inelastic density relaxation (logarithmic in time) begin at higher pressures. When the pressure increases further, the relaxation rate passes through a sharp maximum at 2.5 GPa, which is accompanied by softening the relaxing bulk modulus, and then decreases, being noticeable up to the maximum pressure. When pressure is relieved, an unusual inflection point is observed in the baric dependence of the bulk modulus near 4 GPa. The polyamorphic transformation is only partly reversible and the residual densification after pressure release is 2%. In compression, the electrical resistivity of the g-As₂Te₃ glasses decreases exponentially with increasing pressure (at a pressure up to 2 GPa); then, it decreases faster by almost three orders of magnitude in the pressure range 2–3.5 GPa. At a pressure of 5 GPa, the electrical resistivity reaches 10^–3 Ω cm, which is characteristic of a metallic state; this resistivity continues to decrease with increasing pressure and reaches 1.7 × 10^–4 Ω cm at 8.1 GPa. The reverse metal–semiconductor transition occurs at a pressure of 3 GPa when pressure is relieved. When the pressure is decreased to atmospheric pressure, the electrical resistivity of the glasses is below the initial pressure by two–three orders of magnitude. Under normal conditions, both the volume and the electrical resistivity relax to quasi-equilibrium values in several months. Comparative structural and Raman spectroscopy investigations demonstrate that the glasses subjected to high pressure have the maximum chemical order. The glasses with a higher order have a lower electrical resistivity. The polyamorphism in the As₂Te₃ glasses is caused by both structural changes and chemical ordering. The g-As₂Te₃ compound is the first example of glasses, where the reversible metallization under pressure has been studied under hydrostatic conditions.     

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.     

Pressure-induced modifications of crystal and magnetic structure of oxygen deficient La<Subscript>0.7</Subscript>Sr<Subscript>0.3</Subscript>MnO<Subscript>3-d</Subscript> manganites

The crystal and magnetic structures of the oxygen deficient manganites La_0.7Sr_0.3MnO_3-d (d = 0.15, 0.20) have been studied by means of powder neutron diffraction over the 0–5.2 GPa pressure and 10–290 K temperature ranges. La_0.7Sr_0.3MnO_2.85 exhibits a coexistence of rhombohedral and tetragonal (I4/mcm) crystal structures and below T_g ~ 50 K a spin glass state is formed. La_0.7Sr_0.3MnO_2.80 exhibits a tetragonal (I4/mcm) crystal structure. Below T_g ~ 50 K a phase separated magnetic state is formed, involving coexistence of C-type AFM domains with spin glass domains. In both compounds the crystal structure and magnetic states remain stable upon compression. The factors leading to the formation of different magnetic states in La_0.7Sr_0.3MnO_3-d (d = 0.15, 0.20) and their specific high pressure behavior, contrasting with that of the stoichiometric A_0.5Ba_0.5MnO₃ (A = Nd, Sm) compounds showing pressure-induced suppression of the spin glass state and the appearance of the FM state, are analysed.     

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.     

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.     

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.     

Effect of high pressure on the crystal and magnetic structures of La<Subscript>0.5</Subscript>Ca<Subscript>0.5</Subscript>CoO<Subscript>3</Subscript> cobaltite

The atomic and magnetic structures of La_0.5Ca_0.5CoO₃ cobaltite have been studied by the neutron diffraction technique at high pressures of up to 4 GPa in the 10- to 300-K temperature range. The pressure dependences of the structural parameters have been obtained. The Curie temperature increases with the pressure with the coefficient dT _C/dP = 1 K/GPa, demonstrating the stability of the ground ferromagnetic (FM) state. The pressure dependence of the ground FM state in La_0.5Ca_0.5CoO₃ is in drastic contrast with that for La_{1 − x} Ca _x CoO₃ at a lower calcium content (x < 0.3). For the latter compound, the pressure suppressed the ground FM state and a large negative pressure coefficient of the Curie temperature (dT _C/dP ∼ −10 K/GPa) was observed. The nature of such a phenomenon is analyzed in the framework of the double exchange model also taking into account the changes in the electron configuration of Co³⁺ ions.     

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).