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.     

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.     

Improvement of refrigerant capacity of La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript> single crystal with a few percent Fe doping

Large low-field-induced magnetic entropy changes, ΔS _M, are observed in La_0.67Ca_0.33MnO₃ and La_0.67Ca_0.33Mn_0.96Fe_0.04O₃ single crystals. The peaks of ΔS _M broadened asymmetrically to high temperatures under higher magnetic fields for two materials should be attributed to the first-order magnetic phase transition at T _c. A small amount of iron doping results in an increase in the refrigerant capacity of the material though the magnetic entropy change decreases. The discovery of excellent magnetocaloric features of these single crystals in the low magnetic field can provide some ideas for exploring novel magnetic refrigerants operating under permanent magnet rather than superconducting one as magnetic field source. Supported by the State Key Project of Fundamental Research (Grant No. 2005CB724402), and the National Natural Science Foundation of China (Grant No. 50672126) Contributed by CHENG ZhaoHua     

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.     

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.     

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.     

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.     

Magnetic properties of nanoparticle La<Subscript>0.7</Subscript>Ca<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> under applied hydrostatic pressure

Pressure effects on magnetic properties of two La_0.7Ca_0.3MnO₃ nanoparticle samples with different mean particle sizes were investigated. Both the samples were prepared by the glycine-nitrate method: sample S—as-prepared (10 nm), and sample S₉₀₀—subsequently annealed at 900 °C for 2 h (50 nm). Magnetization measurements revealed remarkable differences in magnetic properties with the applied pressure up to 0.75 GPa: (i) for S sample, both transition temperatures, para-to-ferromagnetic T _C = 120 K and spin-glass-like transition T _f = 102 K, decrease with the pressure with the respective pressure coefficients dT _C/dP = −2.9 K/GPa and dT _f/dP = −4.4 K/GPa; (ii) for S₉₀₀ sample, para-to-ferromagnetic transition temperature T _C = 261 K increases with pressure with the pressure coefficient dT _C/dP = 14.8 K/GPa. At the same time, saturation magnetization M _S recorded at 10 K decreases/increases with pressure for S/S₉₀₀ sample, respectively. Explanation of these unusual pressure effects on the magnetism of sample S is proposed within the scenario of the combined contributions of two types of disorders present in the system: surface disorder introduced by the particle shell, and structural disorder of the particle core caused by the prominent Jahn–Teller distortion. Both disorders tend to vanish with the annealing of the system (i.e., with the nanoparticle growth), and so the behavior of the sample S₉₀₀ is similar to that previously observed for the bulk counterpart.     

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.     

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.     

The size effect on transport properties of colossal magnetoresistance materials La<Subscript>0.67</Subscript>Ca<Subscript>0.33</Subscript>MnO<Subscript>3</Subscript>

High quality La_0.67Ca_0.33MnO₃ (LCMO) film was deposited via a novel pulsed electron deposition technique on SrTiO₃(100) single crystal substrate. The micro-bridge with different widths was fabricated by using electron beam lithography (EBL) technique and their transport properties were studied. For the micro-bridges with width of 2 and 1.5 μm, the insulator-to-metal transition temperature (T _P) keeps unchanged compared with the film. For the micro-bridges with width of 1 μm, the T _P shifts towards the lower temperature by 50 K. When the width decreases down to 500 nm, the insulator-to-metal transition disappears. The magnetoresistance behavior of these micro-bridges was studied, and the results show that the low field magnetoresistance (LFMR) decreases and the high field magnetoresistances (HFMR) keep almost unchanged as the width of micro-bridge is reduced. Supported by the Key Project of the Natural Science Foundation of Zhejiang Province of China (Grant No. Z605131), the National Natural Science Foundation of China (Grant No. 60571029), and W. H. Tang was supported by the Creative Research Group of National Natural Science Foundation of China (Grant No. 60321001)     

Thermoelectric properties of La<Subscript>0.75</Subscript>Ca<Subscript>0.25</Subscript>MnO<Subscript>3</Subscript> manganite at ultrahigh pressures up to 20 GPa

Pressure dependences of the thermopower and electrical resistivity of the La_0.75Ca_0.25MnO₃ manganite are measured in the pressure range 0–20 GPa at room temperature. The absolute value of the thermopower increases in the pressure range 0–3 GPa and decreases at higher pressures. At the same time, the electrical resistivity decreases over the entire pressure range. It is found that the competing effect of the closing of the bandgap, which is determined by the activation energy for the thermopower, and the pressure broadening of the d bands is the cause of the observed behavior of the thermoelectric properties of La_0.75Ca_0.25MnO₃, which is untypical for the majority of dielectrics and semiconductors with single-band unipolar conductivity in the absence of phase transitions and is accompanied by a change in the sign of the pressure coefficient of the thermopower. The interrelation between the magnetic and thermoelectric properties of manganites under pressure is analyzed in the framework of the double exchange model. The causes of the considerable decrease in the pressure coefficients of the insulator-metal transition and Curie temperatures under pressure experimentally observed in manganites are discussed.     

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.     

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.     

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.     

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.     

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.     

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.     

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.     

High-frequency ultrasonic studies of the structural phase transition in an La<Subscript>0.875</Subscript>Sr<Subscript>0.125</Subscript>MnO<Subscript>3</Subscript> single crystal

The specific features of a phase transition from a disordered orbital state to an ordered orbital state in an La_0.875Sr_0.125MnO₃ single crystal are investigated using acoustic methods at a frequency f = 500 MHz. The phase transition is accompanied by a distortion of MnO₆ octahedra due to the cooperative Jahn-Teller effect and is a first-order phase transition, as judged from the sharp change observed in the damping of acoustic pulses, the acoustic wave velocity, and the temperature hysteresis. It is revealed that the parameters of the acoustic waves change significantly throughout the temperature range of existence of the cooperatively distorted structure. In an external magnetic field, the structural phase transition is shifted toward lower temperatures.