Size of the interpolated cation and hole carrier density: two key parameters for the optimisation of colossal magnetoresistive properties of Pr-based manganites

The exploration of the magnetic and transport properties of four series of manganese perovskites, Pr_0.7Ca_0.34−xA_xMnO_3−δ (A=Sr, Ba), Pr_0.7−xLa_xCa_0.3 MnO_3−δ and Pr_0.66Ca_0.34−x Sr_xMnO_3−δ has allowed four phases with colossal magnetoresistive (CMR) properties to be isolated: Pr_0.7Ca_0.25Sr_0.025MnO_3−δ and Pr_0.66Ca_0.26Sr_0.08MnO_3−δ that exhibit a variation of resistance of 2.5. 10⁷% and 10⁹% at μ₀ H=5 T for T=88 K and 50 K respectively, Pr_0.58La_0.12Ca_0.3 MnO_3−δ that exhibits a variation of 6.10⁶% for μ₀ H=5 T at T=80 K and Pr_0.7Ba_0.025Ca_0.275MnO_3−δ for which a resistance variation of 5.10⁹%, at T=50 K, for μ₀ H=5 T is evidenced. for each compound of this series except the barium phase, one observes that the temperature T_max, which corresponds to the resistance maximum on the R(T) curves in zero magnetic field, increases dramatically as the mean size of the interpolated cations increases, and that the CMR effect correlatively decreases dramatically. The comparison of the two series Pr_0.7Ca_0.3−xSr_xMnO_3−δ and Pr_0.66Ca_0.34−xSr_xMnO_3−δ shows also the crucial role of the hole carrier density: for a same mean ionic radius of the interpolated cation T_max is decreased of about 50 K by introducing 0.034 hole per Mn mole.     

Magnetic studies of colossal magnetoresistance perovskites on macroscopic,mesoscopic and microscopic length scales

We have investigated magnetic correlations in various CMR manganites on macroscopic, mesoscopic and microscopic length scales by carrying out DC magnetization, neutron depolarization, and neutron diffraction measurements. We present here the effect of substituting Mn with Fe and La with Dy in the ferromagnetic La_0.7−xCa_xMnO₃ (x ∼ 0.3–0.33) compounds. Neutron diffraction has been used in order to characterize the long-range magnetic order and its gradual suppression by the substitution. Neutron depolarization study has been carried out in order to bridge the gap in our understanding regarding the nature of magnetic correlation obtained from the macroscopic and microscopic measurements. In particular, our study on La_0.67Ca_0.33Mn_0.9Fe_0.1O₃ has established the fact that a true double exchange mediated spin-glass is insulating. In another study of La-site ionic size effect and its disorder in (La_1−x Dy _x )_0.7Ca_0.3MnO₃, we have investigated the evolution of the length scale of magnetic ordering with a possible microscopic explanation and the results have been compared with that for the light rare earth substituted compounds.     

Transport and Magnetic Properties of Eu and Sr Doped Manganite Compound La0.7Ca0.3MnO3

The effect of simultaneous increase in carrier density and size-disorder on the transport and magnetic properties of La_0.7Ca_0.3MnO₃ has been investigated by studying the (La_{0.7 − 2x} Eu _x )(Ca_0.3Sr _x )MnO₃ (0.05 ≤ x ≤ 0.2) (LECSMO) compounds. These compounds have been compared with standard La_{1 − x} Ca _x MnO₃ (0.3 ≤ x ≤ 0.5) (LCMO) in which carrier density alone varies. In LECSMO, the insulator-metal transition temperature (T _p) decreases from 180 K for x = 0.05 to 80 K for x = 0.15 sample vis-à-vis ∼240 K for x = 0.35 to ∼225 K for x = 0.45 in LCMO system. Similarly, the Curie temperature (T _C) in LECSMO, decreases from 205 K for x = 0.05 to 75 K for x = 0.2 sample against 240 K for x = 0.35 to ∼220 K for x = 0.45 in LCMO system. Also, in LCMO the T _C and T _p are coincident whereas, in LECSMO system, with increasing x there is an increasing disparity between the two. At 5 K, in the metallic region, a large MR (>90%) is observed in x = 0.15 sample and is discussed in terms of phase segregation and inter-grain magnetoresistance.     

La0.33Pr0.34Ca0.33MnO3薄膜的应变效应

采用脉冲激光沉积法分别在(100)LaAlO₃和(100)SrTiO₃基片上生长了La_0.33Pr_0.34Ca_0.33MnO₃薄膜,并通过磁测量和电输运测量对生长在不同基片上的La_0.33Pr_0.34Ca_0.33MnO₃薄膜的物性进行了研究.结果表明,基片和薄膜之间的压应力导致La_{关键词： 钙钛矿锰氧化物 相分离 电荷有序}     

Effect of isovalent doping of manganite (La1?xPrx)0.7Ca0.3MnO3 films (0≤x≤1) on their optical, magnetooptical, and transport properties near the metal-insulator transition

The optical, magnetooptical, and electric properties of epitaxial (La_1−x Pr_x)_0.7Ca_0.3MnO₃ films (0≤x≤1) grown by MOCVD on LaAlO₃ and SrTiO₃ substrates were studied. It is shown that the decrease in the average cation radius resulting from isovalent substitution of the Pr for La ions brings about a lowering of the Curie temperature, the metal-insulator transition temperature, and the temperatures of the maxima in magnetotransmission (MT) and magnetoresistance (MR). These temperatures depend only weakly on the substrate type. Substitution of La by Pr does not change the shape of the spectral response of the transverse Kerr effect. For concentrations x≤0.50, the maximum values of the Kerr effect and of the MT vary insignificantly, which should be assigned to the existence of a singly connected ferromagnetic metallic region at low temperatures. In films with x=0.75, the presence of ferromagnetic metallic drops in an antiferromagnetic insulating matrix was revealed. The totality of the experimental data obtained suggest that nanoscopic magnetic and electronic nonuniformities exist both in films with a singly connected metallic region and in an x=1 film, which is an antiferromagnetic insulator. __________ Translated from Fizika Tverdogo Tela, Vol. 46, No. 7, 2004, pp. 1203–1213. Original Russian Text Copyright ? 2004 by Sukhorukov, Loshkareva, Gan’shina, Kaul’, Gorbenko, Mostovshchikova, Telegin, Vinogradov, Rodin.     

Experimental evidence for a magnetic two-phase state in manganites

It is found that samples of manganites La_0.9Sr_0.1MnO₃ (single crystal), Eu_0.7A_0.3MnO₃ (A=Ca, Sr; ceramics), and La_0.1Pr_0.6Ca_0.3MnO₃ and La_0.84Sr_0.16MnO₃ (thin epitaxial films) that are either field-cooled (in a magnetic field) or zero-field-cooled differ in low-temperature magnetization, and the hysteresis loop of field-cooled samples exhibits a displacement. This displacement signifies that a ferro-antiferromagnetic state occurs in these samples. The exchange integral J～10^?6 eV is calculated from this displacement, which describes the exchange Mn-O-Mn coupling through the interface ferromagnetic droplet-antiferromagnetic matrix. The magnetoresistance and volume magnetostriction of La_1?x Sr_xMnO₃ single crystals exhibit similar dependences on x, temperature, and the magnetic field in the vicinity of the Curie point, which points to the fact that these dependences are due to the same reason, namely, the occurrence of a magnetic two-phase ferro-antiferromagnetic state caused by strong s-d exchange.     

Interfacial spin interactions of ferromagnetic and antiferromagnetic manganite bilayers

A pulsed laser deposition technique was used to grow ferromagnetic La_0.7Sr_0.3MnO₃ (LSMO) films on antiferromagnetic La_0.33Ca_0.67MnO₃ (LCMO) and Pr_0.7Ca_0.3MnO₃ (PCMO) films in bilayer forms. The LSMO film on the PCMO layer had a more elongated out-of-plane lattice than that on the LCMO layer. The former had a lower ferromagnetic transition temperature (320 K) than the latter (350 K). The enhanced low-temperature magnetoresistance of the LSMO/PCMO bilayer suggests that the spin frustration is stronger at this bilayer than in the LSMO/LCMO bilayer. These differences indicate that strain state and defect concentration play important roles in governing interfacial spin interactions.     

La0.3Ca0.7Mn1－xVxO3体系的有序相和再入型自旋玻璃行为研究

通过对La_0.3Ca_0.7Mn_1－xV_xO₃(x=0.05,0.10,0.134,0.20)体系的M-T曲线、ρ-T曲线、ESR谱的测量,研究了Mn位掺V对La_0.3Ca_0.7MnO₃体系电荷序和自旋序的影响.结果表明,当0.05≤x≤0.134时, 体系存在电荷有序(CO)相,其自旋序随温度降低发生顺磁(PM)-电荷有序(CO)-反铁磁(AFM)变化.当x＝0.20时,CO相逐步融化,在40 K发生自旋玻璃转变,表现出再入型的自旋玻璃行为,低温下的基态存在着多种复杂的磁相互作用之间的竞争机理. 关键词： 电荷有序 自旋序 相分离 再入型自旋玻璃行为     

Ti/Pr0.7Ca0.3MnO3/La0.67Sr0.33MnO3/Pt异质结电致电阻效应的改善

采用脉冲激光沉积技术制备了Ti/Pr_0.7Ca_0.3MnO₃/Pt和Ti/Pr_0.7Ca_0.3MnO₃/La_0.67Sr_0.33MnO₃/Pt异质结并研究了La_0.67Sr_0.33MnO₃功能插层对异质结电致电阻特性的影响. 实验结果表明La_0.67Sr_0.33MnO₃功能层的引入有效提高了器件的电阻转变特性,尤其是电阻转变率和疲劳性得到了极大的改善. 对La_0.67Sr_0.33MnO₃插层改善电致电阻转变特性的机理进行了定性的分析. 关键词： 电致电阻效应 电阻转变比率 疲劳特性     

Structural, magnetic and magnetotransport behavior of La0.7SrxCa0.3−xMnO3 compounds

A systematic investigation of the structural, magnetic and electrical properties of a series of nanocrystalline La_0.7Sr_xCa_0.3−xMnO₃ materials, prepared by high energy ball milling method and then annealed at 900 °C has been undertaken. The analysis of the XRD data using the Win-metric software shows an increase in the unit cell volume with increasing Sr ion concentration. The La_0.7Sr_xCa_0.3−xMnO₃ compounds undergo a structural orthorhombic-to-monoclinic transition at x=0.15. Electric and magnetic measurements show that both the Curie temperature and the insulator-to-metal transition temperature increase from 259 K and 253 K correspondingly for La_0.7Ca_0.3MnO₃ (x=0) to 353 K and 282 K, respectively, for La_0.7Sr_0.3MnO₃ (x=0.3). It is argued that the larger radius of Sr²⁺ ion than that of Ca²⁺ is the reason to strengthen the double-exchange interaction and to give rise to the observed increase of transition temperatures. Using the phenomenological equation for conductivity under a percolation approach, which depends on the phase segregation of ferromagnetic metallic clusters and paramagnetic insulating regions, we fitted the resistivity versus temperature data measured in the range of 50-320 K and found that the activation barrier decreased with the raising Sr²⁺ ion concentration.     

Size of the interpolated cation and hole carrier density: two key parameters for the optimisation of colossal magnetoresistive properties of Pr-based manganites

The exploration of the magnetic and transport properties of four series of manganese perovskites, Pr_0.7Ca_0.34?xA_xMnO_3?δ (A=Sr, Ba), Pr_0.7?xLa_xCa_0.3 MnO_3?δ and Pr_0.66Ca_0.34?x Sr_xMnO_3?δ has allowed four phases with colossal magnetoresistive (CMR) properties to be isolated: Pr_0.7Ca_0.25Sr_0.025MnO_3?δ and Pr_0.66Ca_0.26Sr_0.08MnO_3?δ that exhibit a variation of resistance of 2.5. 10⁷% and 10⁹% at μ₀ H=5 T for T=88 K and 50 K respectively, Pr_0.58La_0.12Ca_0.3 MnO_3?δ that exhibits a variation of 6.10⁶% for μ₀ H=5 T at T=80 K and Pr_0.7Ba_0.025Ca_0.275MnO_3?δ for which a resistance variation of 5.10⁹%, at T=50 K, for μ₀ H=5 T is evidenced. for each compound of this series except the barium phase, one observes that the temperature T_max, which corresponds to the resistance maximum on the R(T) curves in zero magnetic field, increases dramatically as the mean size of the interpolated cations increases, and that the CMR effect correlatively decreases dramatically. The comparison of the two series Pr_0.7Ca_0.3?xSr_xMnO_3?δ and Pr_0.66Ca_0.34?xSr_xMnO_3?δ shows also the crucial role of the hole carrier density: for a same mean ionic radius of the interpolated cation T_max is decreased of about 50 K by introducing 0.034 hole per Mn mole.     

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.     

Magnetic dilution and electronic nature in La0.7Pb0.3Mn1−xZnxO3

We have studied the magnetic dilution and electronic nature of Zn doping on the Mn site in the colossal magnetoresistant material La_0.7Pb_0.3MnO₃ (x≤0.3). Small non-magnetic Zn²⁺ doping tends to separate the system into ferromagnetic clusters to weaken the long-range ferromagnetic order and to reduce the Curie temperature. The spin polarizability of the x=0–0.3 samples is estimated to be 0.97–1.00, indicating that the x=0–0.3 samples are the spin polarized materials in which the conductivity is dominated by single-spin charge carriers. Small doping (x≥0.1) induces the metal–insulator transition and destroys the metallic state with long-range ferromagnetic order.     

Effect of oxygen deficiency on the electrical and magnetic properties of the manganites La1 ? x Ca x MnO3 ? α ( x = 0.5, 0.6, and 0.7)

The electrical conductivity of La_{1 − x} Ca _x MnO_{3 − α} (x = 0.5) alloys in a magnetic field of 0.6 T is investigated in the temperature range 78–300 K. According to the phase diagram, this compound at α = 0 corresponds to an intermediate region between the ferromagnetic conducting (x < 0.5) and antiferromagnetic semiconducting (x s> 0.5) phases and contains islands of the metallic phase. Under oxygen-deficient conditions, the fraction of the metallic phase increases and the semiconductor-metal transition takes place. The formation of bound islands of the metallic phase is observed under oxygen-deficient conditions in the La_0.4Ca_0.6MnO_{3 − α} compounds. Original Russian Text ? Yu.M. Baĭkov, E.I. Nikulin, Yu.P. Stepanov, 2008, published in Fizika Tverdogo Tela, 2008, Vol. 50, No. 8, pp. 1448–1451.     

Orbital correlations in doped manganites

We review our recent X-ray scattering studies of charge and orbital order in doped manganites, with specific emphasis on the role of orbital correlations in Pr_1-xCa_xMnO₃. For x=0.25, we find an orbital structure indistinguishable from the undoped structure and long-range orbital order at low temperatures. For dopings 0.3≤x≤0.5, we find scattering consistent with a charge and orbitally ordered CE-type structure. While in each case the charge order peaks are resolution limited, the orbital order exhibits only short-range correlations. We report the doping dependence of the correlation length and discuss the connection between the orbital correlations and the finite magnetic correlation length observed on the Mn³⁺ sublattice with neutron-scattering techniques. The physical origin of these domains, which appear to be isotropic, remains unclear. We find that weak orbital correlations persist well above the phase transition, with a correlation length of 1–2 lattice constants at high temperatures. Significantly, we observe similar correlations at high temperatures in La_0.7Ca_0.3MnO₃, which does not have an orbitally ordered ground state, and we conclude that such correlations are robust to variations in the relative strength of the electron–phonon coupling. Received: 22 May 2001 / Accepted: 4 July 2001 / Published online: 5 October 2001     

Conductivity jumps and low-temperature magnetoresistance in the new semiconducting perovskites La1− x BixMnO3+δ

Abrupt jumps are observed on the temperature dependences of the electrical conductivity of La_{1− x} Bi_xMnO_3+δ (0.1<x<0.7) and La_0.3Bi_0.7Na_0.1MnO_3+δ ceramics. The temperatures at which the jumps take place can be reduced by several degrees by applying an external magnetic field of 15 kOe. It can be seen from the magnetization data that the poorly conducting low-temperature phase is not antiferromagnetic (it is likely ferromagnetic) and hence the real-space charge ordering mechanism is not sufficient for explaining the experimental results. An interpretation in terms of magnetic phase nonuniformity is proposed. All the samples studied exhibit high low-temperature magnetoresistance. Pis’ma Zh. éksp. Teor. Fiz. 64, No. 4, 250–253 (25 August 1996) Published in English in the original Russian journal. Edited by Steve Torstveit.     

Electrical and magnetic behavior of La0.7Ca0.3MnO3/La0.7Sr0.2Ca0.1MnO3 composites

The electrical transport properties and the magnetoresistance of La_0.7Ca_0.3MnO₃/La_0.7Sr_0.2Ca_0.1MnO₃ composites are investigated as a function of sintering temperature. On the basis of an analysis by X-ray powder diffraction and scanning electron microscopy we suggest that raising the sintering temperature enhanced the interfacial reaction and creates interfacial phases at the boundaries of the La_0.7Ca_0.3MnO₃ and La_0.7Sr_0.2Ca_0.1MnO₃. Results also show that in 3 kOe, and at the Curie temperature, the magnetoresistance value of 14% was observed for the composite sintered at 1300 °C. Based on the phenomenological equation for conductivity under a percolation approach, which depends on the phase segregation of ferromagnetic metallic clusters and paramagnetic insulating regions, we fitted the experimental resistivity—temperature data from 50-300 K and find that the activation barrier decreases as temperature is increased.     

Study of crystal and magnetic structures of manganite Pr<Subscript>0.7</Subscript>Ba<Subscript>0.3</Subscript>MnO<Subscript>3</Subscript> at high pressure

The crystal and magnetic structures of manganite Pr_0.7Ba_0.3MnO₃ have been studied at high pressures of up to 5.1 GPa and temperatures from 10 to 300 K by means of the neutron diffraction. At normal pressure and a temperature T _C = 200 K, a ferromagnetic state forms in Pr_0.7Ba_0.3MnO₃. At high pressures P ≥ 1.9 GPa and T < T _N ≈ 153 K, a new antiferromagnetic state of A-type have been observed. Under high pressure, the Curie temperature T _C increases with the characteristic quantity dT _C/dP ≈ 2.4 K/GPa. A possible reason for the appearance of an A-type antiferromagnetic phase in Pr_0.7Ba_0.3MnO₃ at high pressures may be anisotropic uniaxial compression of oxygen octahedra along the b axis of the orthorhombic structure.     

Isotope effect in (La-Pr-Ca)MnO3 manganites

An explanation of the “giant” oxygen isotope effect is suggested for the Curie temperature T _C of the (La_0.75Pr_0.25)_0.7Ca_0.3MnO₃ compound. The model takes into account the proximity of the ferromagnetic transition to the dielectric antiferromagnetic phase. To explain the experimental data, it is sufficient to include a weak electron-phonon interaction for free charge carriers.     

Sub-picosecond photo-induced melting of a charge-ordered state in a perovskite manganite

Ultrafast melting of a charge-ordered state has been observed in the photo-irradiated colossal magnetoresistive compound Pr_0.7Ca_0.3MnO₃. Pump-and-probe spectroscopy experiments reveal the formation of a conducting phase with typical features of an insulator–metal transition (IMT) after less than 1 ps. This phase is metastable and can be maintained for about 1 μs unless it is stabilized persistently into a pathlike metallic region by an electric field. Although laser-induced lattice heating may play a role in the initial excitation, electronic correlations are the dominant effect which leads to the formation of the metallic state upon the breakdown of the charge-ordered state. Received: 26 January 2000 / Published online: 16 June 2000