Phase separation with charge self-organization in the Tb0.95Bi0.05MnO3, Gd0.75Ce0.25Mn2O5, and Eu0.8Ce0.2Mn2O5 manganite multiferroics

New doped manganite multiferroics Tb_0.95Bi_0.05MnO₃, Gd_0.75Ce_0.25Mn₂O₅, and Eu_0.8Ce_0.2Mn₂O₅, which are semiconductors, have been grown and studied. The starting dielectric multiferroics TbMnO₃ and RMn₂O₅ (R = Gd and Eu) have close magnetic and ferroelectric ordering temperatures of 30–40 K. The crystals studied are multiferroics in which states with giant permittivity and ferromagnetism coexist at room temperature. An analysis of the dielectric properties suggests that, at temperatures T ≥ 180 K, these crystals undergo a phase separation involving dynamic periodic alternation of quasi-2D layers of mixed-valence manganese ions, a process accounting for the onset of charge-induced ferroelectricity. At low temperatures (T < 100 K), a small phase volume in the crystals is occupied by as-grown quasi-2D layers containing dopants and carriers. Most of the crystal volume is occupied by the carrier-free dielectric phase. Thermally activated hopping conduction involving carrier self-organization in the crystal matrix with ferroelectric frustrations drives a phase transition to the state of charge-induced ferroelectricity at T ∼ 180 K. Original Russian Text ? V.A. Sanina, E.I. Golovenchits, V.G. Zalesskiĭ, 2008, published in Fizika Tverdogo Tela, 2008, Vol. 50, No. 5, pp. 874–882.     

Antiferromagnetic resonance and dielectric properties of rare-earth ferroborates in the submillimeter frequency range

The magnetoresonance and dielectric properties of a number of crystals of a new family of multiferroics, namely, rare-earth ferroborates RFe₃(BO₃)₄ (R = Y, Eu, Pr, Tb, Tb_0.25Er_0.75), are studied in the sub-millimeter frequency range (ν = 3–20 cm⁻¹). Ferroborates with R = Y, Tb, and Eu exhibit permittivity jumps at temperatures of 375, 198, and 58 K, respectively, which are caused by the R32 → P3₁21 phase transition. Antiferromagnetic resonance (AFMR) modes in the subsystem of Fe³⁺ ions are detected in the range of anti-ferromagnetic ordering (T < T _N = 30–40 K) in all ferroborates that have either an easy-plane (Y, Eu) or easy-axis (Pr, Tb, Tb_0.25Er_0.75) magnetic structure. The AFMR frequencies are found to depend strongly on the magnetic anisotropy of a rare-earth ion and its exchange interaction with the Fe subsystem, which determine the type of magnetic structure and the sign and magnitude of an effective anisotropy constant. The basic parameters of the magnetic interactions in these ferroborates are found, and the magnetoelectric contribution to AFMR is analyzed.     

Dielectric relaxation in Bi12SiO20 crystals

Anomalies of the dielectric properties of undoped and aluminum-and gallium-doped crystals of Bi₁₂SiO₂₀ are investigated in the frequency and temperature range ν=10²–10⁸ Hz and T=300–800 K. They are shown to be due to Debye relaxation processes and determined by the relaxor parameters. The mechanism of electron thermal polarization is discussed. Fiz. Tverd. Tela (St. Petersburg) 39, 1223–1229 (July 1997)     

Synthesis and magnetic properties of Cu3B2O6 single crystals

The temperature dependence of the magnetic susceptibility of Cu₃B₂O₆ single crystals grown by spontaneous crystallization from a melt consisting of a mixture of CuO and B₂O₃ and the behavior of their magnetization are investigated in magnetic fields up to 55 kOe. A broad susceptibility maximum is observed near 39 K, and a sharp drop in susceptibility is observed at T<10 K. The paramagnetic Néel temperatures for all orientations of the magnetic field in the crystal investigated are negative, attesting to the predominantly antiferromagnetic character of the exchange interactions. The effective magnetic moment of the Cu²⁺ ion is anisotropic and lies in the range from 1.054μ _B to 1.545μ _B. The magnetization depends linearly on magnetic field at T>10 K, whereas at temperatures below 10 K a discontinuity is observed at fields of the order of 40 kOe. At room temperature, electron magnetic resonance characterized by an almost isotropic g factor (g=2.165) is detected at 36.22 GHz. The exchange interactions in Cu₃B₂O₆ are analyzed on the basis of the Goodenough-Kanamori rules. The possibility of the establishment of a singlet magnetic state in the crystal is analyzed. Fiz. Tverd. Tela (St. Petersburg) 41, 677–679 (April 1999)     

Magnetic and dielectric properties of orthorhombic and hexagonal multiferroics Tb<Subscript>1 − <Emphasis Type="Italic">x</Emphasis></Subscript>Y<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript>

The transition from a stable orthorhombic structure to a hexagonal structure has been revealed in Tb_1−x Y _x MnO₃ multiferroics at x = 0.2–0.4. It has been shown that almost single-phase crystals with an orthorhombic or hexagonal structure can be obtained by choosing the growth conditions. It has been found that the magnetic and dielectric properties of orthorhombic single crystals with x = 0.2–0.3 are similar to the properties of pure TbMnO₃ and are characterized by a strong anisotropy of the magnetic susceptibility at low temperatures and by the presence of a number of magnetic phase transitions, including those to the ferroelectric state. New spontaneous (T ≤ 15 K) and magnetic-field induced (H | C ₆) phase transitions accompanied by the appearance of an uncompensated rare-earth magnetic moment ∼1 μ_B/mole have been observed in hexagonal single crystals with x = 0.3–0.5.     

Paramagnetic and spin-glass properties of pyrochlore-like oxides Ln2Mn2/3Mo4/3O7 (Ln=Sm, Gd, Tb, or Y)

The magnetic properties of complex oxides Ln ₂Mn_2/3Mo_4/3O₇ (Ln=Sm, Gd, Tb, or Y) with a pyrochlore-type structure are studied in the temperature range 2–300 K. For all compounds in the paramagnetic state, the temperature dependence of the magnetic susceptibility is described by a generalized Curie-Weiss law with a temperature-independent component of ∼10⁻⁶ cm³/g and with a Weiss constant Θ<0 and |Θ|<16 K. At low temperatures (T<10–12 K), the compounds have spin-glass properties; they exhibit magnetic and temperature hysteresis and the typical dependences of the imaginary and real parts of the dynamic magnetic susceptibility on temperature and the frequency of an ac magnetic field in a wide range of magnetization relaxation times. The data obtained suggest that d electrons are responsible for the formation of frustrated exchange interactions in the compounds and that 4f electrons in the compounds with Sm or Tb provide strong magnetic-anisotropy effects. __________ Translated from Fizika Tverdogo Tela, Vol. 46, No. 2, 2004, pp. 287–295. Original Russian Text Copyright ? 2004 by Korolev, Bazuev.     

Crystal structure and magnetic anisotropy of ludwigite Co<Subscript>2</Subscript>FeO<Subscript>2</Subscript>BO<Subscript>3</Subscript>

Co₃O₂BO₃ and Co₂FeO₂BO₃ single crystals with a ludwigite structure are fabricated, and their crystal structure and magnetic properties are studied in detail. Substituted ludwigite Co₂FeO₂BO₃ undergoes two-stage magnetic ordering at the temperatures characteristic of Fe₃O₂BO₃ (T _N1 ≈ 110 K, T _N2 ≈ 70 K) rather than Co₃O₂BO₃ (T _N = 42 K). This effect is explained in terms of preferred occupation of nonequivalent crystallographic positions by iron, which was detected by X-ray diffraction. Both materials exhibit a pronounced uniaxial magnetic anisotropy. Crystallographic direction b is an easy magnetization axis. Upon iron substitution, the cobalt ludwigite acquires a very high magnetic hardness.     

Muon-spin-relaxation investigation of EuMn<Subscript>2</Subscript>O<Subscript>5</Subscript>

The magnetic properties of the EuMn₂O₅ multiferroic (samples consisting of single crystals and ceramic samples) have been investigated by the muon-spin-relaxation (μSR) method in the temperature range of 10–300 K. Below the magnetic ordering temperature T _N = 40 K, the loss of the polarization of muons and the effect of the external magnetic field have been observed. Both phenomena can be explained by an additional channel of the depolarization of muons owing to the appearance of muons in a medium with a low electron density due to the charge separation process (the redistribution of the electron density in the phase transition process). The “memory” phenomenon has been revealed in a sample in the external magnetic field; the memory relaxation time depends on the size of the structure units of the samples (single crystals or ceramic grains).     

Characteristic features of the magnetic ordering of Dy3+ ions in a monoclinic RbDy(WO4)2 single crystal

The investigation of the specific heat of a RbDy(WO₄)₂ single crystal at temperatures 0.2–2.5 K and in magnetic fields up to 2 T are reported. The temperature dependence of the specific heat near T _N=0.818 K is compared with the predictions for different models. The 2D Ising model describes satisfactorily C(T) below T _N, while for T>T _N none of the theoretical models agree with the behavior of C(T) of RbDy(WO₄)₂. The H-T phase diagram for H∥c is complicated and possesses a triple point, where regions of existence of three magnetic phases converge. The magnetic ordering is analyzed from the standpoint of the Jahn-Teller nature of the structural phase transitions occurring in RbDy(WO₄)₂ at higher temperatures. It is shown that the form of the phase diagram depends on the direction of the vector H, for the general case of an arbitrary direction of H, two phase transitions can occur with increasing field. Fiz. Tverd. Tela (St. Petersburg) 41, 491–496 (March 1999)     

Low-temperature behavior of specific heat curves in ruthenocuprate RuSr<Subscript>2</Subscript>Gd<Subscript>1.5</Subscript>Ge<Subscript>0.5</Subscript>Cu<Subscript>2</Subscript>O<Subscript>10 − δ</Subscript>: Superconducting,magnetic and crossing-point effects

Magnetic and superconducting properties of polycrystalline samples of RuSr₂Gd_1.5Ce_0.5Cu₂O_{(10 − δ)}, asprepared (by solid-state reaction) and annealed in pure oxygen at different pressure are presented. Specific heat and magnetization were investigated in the temperature range 1.8–300 K with a magnetic field up to 8 T. Specific heat, C (T), shows a jump at the superconducting transition (with onset at T ≈ 37.5 K) and a Schottky-type anomaly below 20 K. It is found that curves C(T) taken for different values of magnetic field have the same crossing point (at T _* ≈ 2.7 K) for all samples studied. At the same time, C(H) curves taken for different temperatures have a crossing point at a characteristic field H _* ≈ 3.7 T. These effects are manifestations of the crossing-point phenomenon, which is supposed to be inherent for strongly correlated electron systems.     

Thermal conductivity of crystalline fullerite C60 in the simple cubic phase

The behavior of the thermal conductivity k(T) of bulk faceted fullerite C₆₀ crystals is investigated at temperatures T=8–220 K. The samples are prepared by the gas-transport method from pure C₆₀, containing less than 0.01% impurities. It is found that as the temperature decreases, the thermal conductivity of the crystal increases, reaches a maximum at T=15–20 K, and drops by a factor of ∼2, proportional to the change in the specific heat, on cooling to 8 K. The effective phonon mean free path λ _p, estimated from the thermal conductivity and known from the published values of the specific heat of fullerite, is comparable to the lattice constant of the crystal λ _p∼d=1.4 nm at temperatures T>200 K and reaches values λ_p∼50d at T<15 K, i.e., the maximum phonon ranges are limited by scattering on defects in the volume of the sample in the simple cubic phase. In the range T=25−75 K the observed temperature dependence k(T) can be described by the expression k(T)∼exp(Θ/bT), characteristic for the behavior of the thermal conductivity of perfect nonconducting crystals at temperatures below the Debye temperature Θ (Θ=80 K in fullerite), where umklapp phonon-phonon scattering processes predominate in the volume of the sample. Pis’ma Zh. éksp. Teor. Fiz. 65, No. 8, 651–656 (25 April 1997)     

Magnetoelectric effect and toroidal ordering in Ga2−x FexO3

The field dependence of the magnetoelectric effect and longitudinal magnetostriction of Ga_2−x Fe_xO₃ single crystals is studied in magnetic fields up to 200 kOe in the temperature range from 4.2 to 300 K. It is shown that the magnetoelectric effect in these materials is determined mainly by the toroidal moment T and is not related to magnetostriction, as was previously theorized. A new method for determining the toroidal moment by measuring the electric polarization in a strong magnetic field is proposed. The value of the toroidal moment of the unit cell in Ga_1.15Fe_0.85O₃ is calculated: T=(T _a ,0,0), where T _a =24.155μ _B Å per unit cell. Experimental data are analyzed using a theory of toroidal spin ordering, which gives good agreement with experiment. Zh. éksp. Teor. Fiz. 114, 263–272 (July 1998) Deceased.     

The spin-glass state in Y2Co2/3Mo4/3O7 and Y2Fe2/3Mo4/3O7 complex oxides

The magnetic properties of Y₂ B _2/3Mo_4/3O₇ complex oxides (B = Co, Fe) were studied in the temperature range 2–300 K. At low temperatures, these compounds exhibit spin-glass properties with freezing temperatures T _f=26 and 33 K, respectively, and typical features in the magnetic hysteresis and in the dependences of the real part of the dynamic magnetic susceptibility on temperature and ac magnetic field frequency. Above T _f, the static magnetic susceptibility of the samples studied depends on the applied magnetic field, which is tentatively assigned to the presence of metallic cobalt and/or yttrium orthoferrite YFeO₃ introduced in the course of sample preparation. __________ Translated from Fizika Tverdogo Tela, Vol. 47, No. 12, 2005, pp. 2182–2188. Original Russian Text Copyright ? 2005 by Bazuev, Korolev.     

Dielectric relaxation in the weak ferroelectric Li2Ge7O15 near the ferroelectric phase transition

The dielectric permittivity of Ni-doped Li₂Ge₇O₁₅ crystals was studied in the vicinity of the ferroelectric phase transition. Introduction of Ni has been shown to suppress the dielectric anomaly and to reduce substantially the transition temperature. A temperature hysteresis in ɛ (T) has been observed in nominally pure and Ni-doped Li₂Ge₇O₁₅ crystals near the transition point. Measurements performed under cooling from the paraphase reveal dispersion of dielectric permittivity at Debye relaxation frequencies of the order of 10⁴–10⁵ Hz at T _c . It is proposed that the hysteresis phenomena and the low-frequency dispersion are caused by residual defects (of the type of random local fields), which become polarized in the ferroelectric phase and become disordered above T _c . Fiz. Tverd. Tela (St. Petersburg) 40, 2198–2201 (December 1998)     

Low-field magnetization of ludwigites Co3O2BO3 and Co3 ? xFexO2BO3 (x ≈ 0.14)

Ludwigite single crystals of compositions Co₃O₂BO₃ and Co_{3 − x} Fe _x O₂BO₃ (x ≈ 0.14) have been synthesized. The crystal structure is investigated at room temperature, and the magnetization is studied in the temperature range T = 4.2–100 K in magnetic fields of up to 600 Oe. The orthorhombic symmetry is revealed, and the unit cell parameters are determined. A number of features are established for the temperature dependence of the magnetization. In unsubstituted Co₃O₂BO₃, two magnetic transitions are found at T _C1 = 43 K and T _C2 = 15 K. At temperatures below 40 K, spin-glass state is revealed. Substitution of iron ions for cobalt ions leads to a noticeable shift in the magnetic transitions toward the high-temperature range: T _C1 = 83 K and T _C2 = 74 K. A ferromagnetic ordering of the P type is found in the Co_{3 − x} Fe _x O₂BO₃ (x ≈ 0.14) compound. Original Russian Text ? N.V. Kazak, N.B. Ivanova, V.V. Rudenko, A.D. Vasil’ev, D.A. Velikanov, S.G. Ovchinnikov, 2009, published in Fizika Tverdogo Tela, 2009, Vol. 51, No. 5, pp. 916–919.     

Quasi-one-dimensional antiferromagnet LiCuVO4

An antiferromagnetic transition is observed in the quasi-one-dimensional metal-oxide compound LiCuVO₄. A wide peak is observed in the temperature dependence of the magnetic susceptibility at T _M =28 K, and the magnetic susceptibility exhibits a sharp drop at T _N ≈4 K. As the magnetic field increases, the antiferromagnetic-ordering temperature T _N =2.3 K at first increases somewhat and then decreases rapidly. The exchange interaction in the chains of copper-oxygen octahedra is estimated to be J ₁=22.5 K. The interchain interaction is estimated to be J ₂∼1 K. Pis’ma Zh. éksp. Teor. Fiz. 69, No. 11, 828–831 (10 June 1999)     

Thermal expansion of ScxTi1−x Fe2 itinerant magnets

A study of the thermal expansion coefficient (TEC) of the Sc_xTi_1−x Fe₂ itinerant magnets has been made within the 5–1200 K range at the transition from the TiFe₂ antiferromagnet (T _N=270 K) to the ScFe₂ ferromagnet (T _C=540 K). A negative TEC magnetic contribution α _m(T) has been found, which is associated with the formation of spin-fluctuation-induced local magnetic moments in both the magnetically ordered and the paramagnetic state. The specific features in the α _m(T) dependence are shown to be due to the shape of the density-of-states function near the Fermi level. Fiz. Tverd. Tela (St. Petersburg) 41, 2174–2178 (December 1999)     

Resistive transition and upper critical field in underdoped YBa2Cu3O6+x single crystals

A superconducting transition in the temperature dependence of the ab-plane resistivity of underdoped YBa₂Cu₃O_6+x crystals in the range T _c≲30 K has been investigated. Unlike the case of samples with the optimal level of doping, the transition width increased insignificantly with magnetic field, and in the range T≲13 K it decreased with increasing magnetic field. The transition point T _c(B) was determined by analyzing the fluctuation conductivity. The curves of B _c2(T) measured in the region T/T _c≳0.1 did not show a tendency to saturation and had a positive second derivative everywhere, including the immediate neighborhood of T _c. The only difference among the curves of B _c2(T) for different crystal states is the scales of Tand B, so they can be described in terms of a universal function, which fairly closely follows Alexandrov’s model of boson superconductivity. Zh. éksp. Teor. Fiz. 115, 268–284 (January 1999)     

Reduction in the rate of phonon scattering by a spatially correlated system of iron ions and low-temperature “anomaly” of the thermoelectric phenomena in HgSe:Fe crystals

A new effect of the reduction in the rate of phonon scattering by the spatially correlated system of iron ions in HgSe:Fe crystals is detected experimentally and calculated theoretically. The thermoelectric power is measured using HgSe:Fe samples with different iron content in the temperature range 7.5–60 K. It is found that the dependence of the thermoelectric power on iron content exhibits remarkable features at T<10 K: the quantity |α(N _Fe )| increases as the iron concentration increases to N _Fe =5×10¹⁸ cm⁻³, reaches a maximum at N _Fe ≈(1–2)×10¹⁹ cm⁻³, but then monotonically decreases with further increases in N _Fe . It is shown that the obseved increase in the thermoelectric power is due to a reduction in the rate of phonon scattering by the spatially correlated system of Fe³⁺ ions. This new effect is analyzed theoretically, and the theoretical results are compared with the experimental data. Zh. éksp. Teor. Fiz. 114, 191–207 (July 1998)