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.     

Inhomogeneous magnetic states in the Nd(Mn<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Cr<Subscript>x</Subscript>)O<Subscript>3</Subscript> system

The crystal structure and magnetic properties of the Nd(Mn_?xCr_x)O₃ system (x≤0.85) have been studied. Substitution of chromium for manganese was shown to induce a transition from the antiferromagnetic to ferromagnetic state (x≈0.2) and a decrease in the critical temperature followed, conversely, by an increase in the Néel temperature and decay of spontaneous magnetization. At low temperatures, the magnetization was found to behave anomalously as a result of magnetic interaction between the ferromagnetic and antiferromagnetic phases. The formation of the ferromagnetic phase is attributed to destruction of cooperative static orbital ordering, while the coexistence of different magnetic phases is most probably due to internal chemical inhomogeneity of the solid solutions.     

Enhanced polarization and magnetoelectric response in Tb1−x Ho x MnO3

A series of manganites Tb_1−x Ho _x MnO₃ (0≤x≤0.6) with orthorhombic structure are synthesized and detailed investigations on their multiferroicity are performed. Successive magnetic transitions upon temperature variation are evidenced for all the samples, and both the Mn³⁺spiral spin ordering and rare-earth spin ordering are suppressed with increasing x. A significant enhancement of both the polarization and magnetoelectric response within 0.2<x<0.4 is observed, which may probably result from the shortening of the spiral-spin-ordering period, due to the competition between the spiral spin order and E-type antiferromagnetic order. This argument is supported by further theoretical calculations based on the two e _g -orbital double-exchange model.     

The magnetic behavior of La1−xTbxMn2Si2 (0≤x≤0.3) in weak magnetic fields

The structure and magnetic properties of La_1−xTb_xMn₂Si₂ (0≤x≤0.3) were studied by X-ray powder diffraction and DC magnetization measurements. All the compounds crystallize in ThCr₂Si₂-type structure. Substitution of Tb for La led to a linear decrease in the lattice constants and the unit-cell volume. A ferromagnetic phase for x≤0.15, and an antiferromagnetic phase for x=0.3 have been observed at about room temperature, whereas the compounds with x=0.2 and 0.25 exhibit a magnetic phase transition from ferromagnetism to antiferromagnetism.     

Jahn-Teller distortion and magnetoresistance in electron doped Sr1-xCexMnO3 (x = 0.1, 0.2, 0.3 and 0.4)

Neutron and electron diffraction, electrical transport and magnetic measurements have been carried out on a newly synthesized electron doped Sr_1-xCe _x MnO₃ (x = 0.1, 0.2, 0.3 and 0.4) system. For x=0.1, while cooling, it undergoes a first-order metal-insulator transition at 315 K which is associated with a structural transition from cubic (Pm3m) to tetragonal (I4/mcm) due to Jahn-Teller ordering () which stabilizes a chain like (C-type) antiferromagnetic ground state with . The antiferromagnetic insulator state is insensitive to an applied magnetic field of 7 T. With increase of x, while the nuclear structure at room temperature for x=0.2 and 0.3 remains tetragonal, for x=0.4 it becomes orthorhombic (Imma) where the doping electrons seem to occupy mainly the d _x2-y2 symmetry. Further, the JT distortion and the antiferromagnetic interactions decrease with doping and a small negative magnetoresistance appears for . Magnetic measurements show that the dilution of antiferromagnetic interaction results into a spin glass like behaviour at low temperature for the samples with x=0.3 and 0.4. This behaviour is in contrast with the CMR properties of calcium based electron doped systems and hole doped manganites. The stability of C-type antiferromagnetic ordering in the electron doped system with large A-site cationic size may be responsible for the absence of double exchange ferromagnetism and CMR effect. Received 10 September 1999     

Magnetic phase diagrams of Ho1−xDyxNi2B2C

We performed the magnetization measurement on Ho_1−xDy_xNi₂B₂C single crystals (x=0.1, 0.2, 0.3, 0.4, and 0.6) with magnetic field applied perpendicular and parallel to the c-axis. But only for the magnetic field perpendicular to the c-axis, the increase of Dy³⁺ concentration affects the magnetically ordered states of HoNi₂B₂C compound and makes the phase diagram more complicated. The antiferromagnetic ordering state attributed to Dy³⁺ sublattice starts to appear from a case of x=0.2 and finally the magnetic phase diagram becomes analogous to that of DyNi₂B₂C as x is increased which is consistent with the neutron scattering result.     

Magnetocaloric effect of Gd–Tb alloys: influence of the sample shape anisotropy

The magnetocaloric effect of Gd_1−x Tb _x alloys with x=0.00, 0.10, 0.20, 0.25, 0.30 and 0.40 was studied. The magnetic ordering temperatures were determined from the magnetization measurement. The data obtained from magnetization and specific-heat measurements as well as by the direct measurement are well comparable within their experimental errors. The values of ΔT _ad are in the proximity of 2.5 K for field change of 1 T and all studied concentrations. The dependence of magnetocaloric effect on the sample shape anisotropy was documented by the magnetization measurement as well as by the direct measurement.     

Magnetic properties of multiferroics Bi1 ? xAxFeO3 ? x/2 (A = Ca, Sr, Pb, Ba)

The magnetic properties of Bi_{1 − x} A _x FeO_{3 − x/2} (A is an alkaline-earth ion) solid solutions have been studied in magnetic fields of up to 140 kOe. The ferroelectric phase (space group R3c) transforms into the nonpolar pseudocubic phase at x ≈ 0.2. It is demonstrated that the substitution of alkaline-earth ions for bismuth ions (x ≥ 0.1) leads to a complete destruction of the modulated antiferromagnetic structure and the appearance of a weakly ferromagnetic state within the R3c state. In the pseudocubic phase, the spontaneous magnetization is absent; however, the field dependence of the magnetization is nonlinear and depends on the magnetic prehistory.     

Phase transitions and magnetic-transport phenomena in the system La2/3Ba1/3(Mn1−x Cox)O3

A study is performed of the crystalline structure, magnetization, and magnetotransport properties of the system La_2/3Ba_1/3(Mn_1−x Co_x)O₃ with perovskite structure. It is shown that cubic solid solutions exist over the entire range of cobalt concentrations 0⩽x⩽1. Compositions with x⩽0.2 are ferromagnets with maximum resistance near T _C . Compositions with 0.2<x<0.4 manifest properties of inhomogeneous ferromagnets. Measurements of magnetic properties indicate the absence of long-range magnetic order in compositions with 0.5⩽x⩽0.9, which are probably spin glasses. The spontaneous magnetization of cobaltate (2μ _B per formula unit) corresponds to ferromagnetic ordering of the moments of the Co³⁺ and Co⁴⁺ ions found in the intermediate spin state. It is conjectured that the magnetoresistance consists of an extrinsic and an intrinsic contribution. The first arises as a result of intergrain transport of spin-polarized charge carriers, and the second, as a result of magnetic ordering near T _C . The magnetoresistance is essentially independent of the spontaneous magnetization and decreases abruptly as the cobalt concentration is increased with a corresponding transition from long-range to short-range magnetic order. Zh. éksp. Teor. Fiz. 116, 604–610 (August 1999)     

Charge-Ordered Antiferromagnetic to Ferromagnetic Phase Transition in Cr-Doped Nd0.5Ca0.5Mn1−x Cr x O3: EMR and Magnetization Study

The Cr-doped rare-earth manganites Nd_0.5Ca_0.5Mn_1−x Cr _x O₃ (x = 0.03, 0.05, 0.10) are studied by electron magnetic resonance (EMR) and magnetization measurements in the paramagnetic as well as in the ferromagnetic phase. The magnetization measurements show that the charge-ordered antiferromagnetic phase decreases at the expense of ferromagnetic metallic phase and for Cr doping of x = 0.1, the charge-ordered phase melts completely. The EMR shows multiple signals for all three compositions in the ferromagnetic phase indicative of an anisotropic ferromagnetic phase. The difference between the shift of the high-field and low-field signals decreases with Cr doping, indicating that the magnetic anisotropy decreases with the Cr doping. In the paramagnetic phase the EMR line width follows Causa's model as observed in other colossal magnetoresistant manganites. Authors' address: Ajay Sharma, Department of Physics, Indian Institute of Science, Bangalore, India     

The antiferromagnetic-ferromagnetic transition in the system Zn1−x CuxCr2S4

The magnetization and paramagnetic susceptibility of the system of compounds Zn_1−x Cu_xCr₂S₄ (0<x⩽1) are investigated at low temperatures. It is shown that as the content of Cu increases the system exhibits a transition from an antiferromagnetic to a ferromagnetic state. Fiz. Tverd. Tela (St. Petersburg) 40, 278–279 (February 1998)     

Magnetic ordering in the perovskites Eu1−x CaxMnO3 (0⩻x⩻0.5)

The magnetic properties of Eu_1−x Ca_xMnO₃ have been investigated. As the calcium content increased up to x=0.2, the magnetization and the blocking temperature of the magnetic moments of clusters increased and the magnetic anisotropy decreased. As the calcium content increased further, the magnetization decreased, while the “freezing” temperature of the magnetic moments increased. Anomalies of the magnetic properties were observed in compositions with x=0.4 and 0.5 at T=40 K; these anomalies are attributed to a transition to the antiferromagnetic state in the charge-ordered phase. Fiz. Tverd. Tela (St. Petersburg) 39, 117–120 (January 1997)     

Magnetic properties of ferromagnetic diluted Zn x Cd1–x Cr2Se4 spinels are studied by Green's functions,mean field theory and high temperature series expansions theories

The field induced reorientation of the magnetization of ferromagnetic (or antiferromagnetic) structure is treated within the framework of many-body Green's function theory by considering all components of the magnetization. The mean field theory is used to calculate the nearest neighbour and the next-neighbour super-exchange J₁(Cr–Cr) and J₂(Cr–(Zn(Cd)–Se)–Cr), respectively, for the Zn_1–x Cd _x Cr₂Se₄ in the range 0 < x < 1. The intraplanar and the interplanar interactions are deduced. The high temperature series expansions (HTSEs) are derived for the magnetic susceptibility and the two-spin correlation functions for a Heisenberg ferromagnetic model on the B-spinel lattice. The calculations are developed in the framework of the random phase approximation (RPA). The magnetic phase diagram is deduced. A spin glass phase is predicted for intermediate range of concentration. The obtained results are comparable with those obtained by magnetic measurements. The critical exponents associated with the magnetic susceptibility (γ) and the correlation lengths (ν) have been deduced. The obtained values are comparable to those of 3D Heisenberg model.     

Selected properties of EuCo2(Si1−xGex)2 alloys

EuCo₂(Si_1−xGe_x)₂, x=0, 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1 samples were synthesised by induction melting followed by annealing at 900 °C and rapid quenching. X-ray powder diffraction and Auger electron spectroscopy studies revealed that solid solutions are formed only for x?0.2 and x?0.7. Magnetic susceptibility investigations for the solid solutions revealed a dominant divalent europium valence state in the germanium-rich samples and a dominant trivalent europium component in the silicon-rich samples. In the germanium-rich samples, a long-range antiferromagnetic ordering was observed. In all samples studied, additional magnetic transitions at various temperatures were detected, which could be attributed to small clusters containing different europium chemical surrounding from that in the predominant phase.     

Structure, transport and magnetic properties in La2xSr2−2xCo2xRu2−2xO6

The perovskite solid solutions of the type La_2xSr_2−2xCo_2xRu_2−2xO₆ with 0.25≤x≤0.75 have been investigated for their structural, magnetic and transport properties. All the compounds crystallize in double perovskite structure. The magnetization measurements indicate a complex magnetic ground state with strong competition between ferromagnetic and antiferromagnetic interactions. Resistivity of the compounds is in confirmation with hopping conduction behaviour though differences are noted especially for x=0.4 and 0.6. Most importantly, low field (50 Oe) magnetization measurements display negative magnetization during the zero field cooled cycle. X-ray photoelectron spectroscopy measurements indicate the presence of Co²⁺/Co³⁺ and Ru⁴⁺/Ru⁵⁺ redox couples in all compositions except x=0.5. Presence of magnetic ions like Ru⁴⁺ and Co³⁺ gives rise to additional ferromagnetic (Ru-rich) and antiferromagnetic sublattices and also explains the observed negative magnetization.     

Influence of a nonmagnetic impurity on the properties of the quasi-one-dimensional antiferromagnet CsNiCl3

Various magnetic properties of the diluted quasi-one-dimensional antiferromagnet CsNi_1−x MgxCl₃ are investigated experimentally for several impurity concentrations. The antiferromagnetic resonance spectrum and the phase diagrams are found to depend significantly on the amount of added Mg. The field and temperature dependences of the static magnetization is measured for crystals with two different contents x. A substantial increase in the magnetization is observed at low temperature, where the additional susceptibility is approximately proportional to the concentration. The physical mechanisms underlying the observed strong influence of magnetic defects formed at breaks in the spin chains in a quasi-one-dimensional antiferromagnet on its magnetic properties in the ordered state and for T<T _N are discussed. Zh. éksp. Teor. Fiz. 112, 209–220 (July 1997)     

Magnetic-Field-Controlled Quantum Critical Points in the Triangular Antiferromagnetic Cs2CuCl4-xBrx Mixed System

The triangular antiferromagnetic Cs₂CuCl_4-xBr_x mixed system is studied by neutron single-crystal diffraction in magnetic field. It shows a rich magnetic phase diagram consisting of four regimes depending on the Br concentration and is characterized by different exchange coupling mechanisms. For the investigated compositions from regime I (0 < x ≤ 1.5), a critical magnetic field B_c is found for a Br concentration x = 0.8 at B_c = 8.10(1) T and for x = 1.1 at B_c = 7.73(1) T and from regime IV (3.2 < x < 4) for x = 3.3 at B_c = 0.99(3) T. For magnetic fields larger than the respective B_c, magnetic superlattice reflections of these compounds are not found. The incommensurate magnetic wave vector q = (0, 0.470, 0) appears below the ordering temperature T_N = 0.51(1) K for Cs₂CuCl_3.2Br_0.8, and q = (0, 0.418, 0) below T_N = 1.00(6) K for Cs₂CuCl_0.3Br_3.7. Neutron diffraction experiments at around 60 mK for x = 3.7 in a magnetic field show the critical magnetic field at B_c = 7.94(16) T and the formation of the second magnetic phase at around 8.5 T depending on the temperature. Inelastic neutron scattering experiments for the compound from regime III (2 < x ≤ 3.2) with x = 2.2 show dynamical correlations at a temperature around 50 mK giving evidence for a spin liquid phase.     

Electron transport in NbxTi1−xO2 with 0.04 < x < 1

Electrical conductivity and thermopower have been determined in the Nb_xTi_1?xO₂ solid solutions for 0.04 < x < 1 and between 300 and 1300 K. Experimental results are fitted with a small polaron model of electron transport. Thermopower results are consistent with localized particle motion with a binding energy increasing with Nb content up to 0.1 eV. Nevertheless, it seems that this localized particle is a single small polaron only at low temperatures because of the high calculated energy at high temperatures for the associated phonon according to the single small polaron theory. A tentative interpretation for the high-temperature range is proposed: the existence of a bipolaron for 0.04 < x < 0.2 (as in Ti₄O₇) and a tripolaron for 0.2 < x < 0.5. This assumption accounts correctly for the hightemperature thermopower and the variation of the activation energy of mobility with temperature. Nevertheless, new experiments such as magnetic susceptibility determination are required to prove this idea.     

Phase states in the Y<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>Ca<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> solid solution system

The room-temperature stability region of the tetragonal phase in the Y_{1 − x} Ca _x MnO₃ solid solution system has been found for the first time. The concentration boundaries between this phase and the orthorhombic (x > 0.5) and hexagonal (x < 0.25) phases are sensitive to the sample preparation conditions. The coexistence of the hexagonal and tetragonal phases in the range 0.15 < x < 0.25 indicates that these phases undergo a first-order reconstructive phase transition. Preliminary measurements of magnetic ordering effects for compositions with x = 0.3, 0.5, and 0.7 have been performed.