Multiferroic properties of ErMnO3

Measurements of magnetic and dielectric properties of single crystalline ErMnO3 establish the Neel and ferroelectric transition temperatures to be 77 K and 588 K respectively. The dielectric constant of ErMnO3 shows an anomalous jump at T-N. At higher temperatures, the dielectric constant undergoes a significant decrease on application of magnetic fields. The study clearly exhibits multiferroic and magnetoelectric nature of ErMnO3.

Charge-order-driven multiferroic properties of Y1-xCaxMnO3

Dielectric measurements on the charge-ordered insulators, Y1-xCaxMnO3 (x = 0.4. 0.45 and 0.5), show maxima in the dielectric constant around the charge ordering transition temperature while magnetic measurements show the presence of weak ferromagnetic interactions at low temperatures. Besides the magnetic field dependence of the dielectric constant, these manganites also exhibit second harmonic generation. Thus, the charge-ordered Y1-xCaxMnO3 compositions are multiferroic and magnetoelectric, in accordance with theoretical predictions. Magnetoelectric properties are retained in small particles of Y0.5Ca0.5MnO3. (C) 2008 Elsevier Ltd. All rights reserved.

Multiferroic properties of microwave sintered BaTiO3-SrFe12O19 composites

The composites of xSrFe(12)O(19)-(1-x) BaTiO3 where x=0, 0.1, 0.3, 0.5, 0.7, 0.9 and 1were prepared by Sol gel method and consequently densified at 1100 degrees C/90 min using microwave sintering method. The phase formation and diphase microstructure of the composite samples was examined by X-ray diffraction and field emission electron microscope (FESEM), respectively. The effects of constituent phase variation on the ferroelecrric, dielectric and magnetic properties were examined. It was observed that with a decrease of x, the Curie temperature shifted towards low temperature side. (C) 2014 Elsevier B.V. All rights reserved.

Co-existence of tetragonal and monoclinic phases and multiferroic properties for x <= 0.30 in the (1-x)Pb(Zr0.52Ti0.48)O-3-(x)BiFeO3 system

Compositions with x <= 0.30 in the system (1- x)Pb(Zro(0.52)Ti(0.48))O-3-(x)BiFeO3 were synthesized by sol-gel method. Rietveld analysis of X-ray diffraction data reveals tetragonal structure (P4mm) for x <= 0.05 and monoclinic (Cm) phase along with the existence of tetragonal phase for 0.10 <= x <= 0.25 and monoclinic phase for x = 0.30. Transformation of E(2TO) and E + B1 vibrational modes in the range 210-250 cm(-1) (present for x <= 0.25) into A' + A `' modes at similar to 236 cm(-1) for x = 0.30, and occurrence of new vibrational modes A' and A `' in Raman spectra for x >= 0.10 unambiguously support the presence of monoclinic phase. Occurrence of remnant polarisation and enhanced magnetization with concentration of BiFeO3 indicates superior multiferroic properties. Variation of magneto-capacitance with applied magnetic field is a strong evidence of magneto-electric multiferroic coupling in these materials. (C) 2014 Elsevier B.V. All rights reserved.

Electric and magnetic polarizabilities of hexagonal Ln(2)CuTiO(6)(Ln = Y, Dy, Ho, Er, and Yb)

We investigated the rare-earth transition-metal oxide series, Ln(2)CuTiO(6) (Ln = Y, Dy, Ho, Er, and Yb), crystallizing in the hexagonal structure with noncentrosymmetric P6(3)cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln = Y, exhibit a low-temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the expected ferroelectric transition is frustrated by the large size difference between Cu and Ti at the B site. Interestingly, this leads these compounds to attain a rare and unique combination of desirable paraelectric properties with high dielectric constants, low losses, and weak temperature and frequency dependencies. First-principles calculations establish these exceptional properties result from a combination of two effects. A significant difference in the MO5 polyhedral sizes for M = Cu and M = Ti suppress the expected cooperative tilt pattern of these polyhedra, required for the ferroelectric transition, leading to relatively large values of the dielectric constant for every compound investigated in this series. Additionally, it is shown that the majority contribution to the dielectric constant arises from intermediate-frequency polar vibrational modes, making it relatively stable against any temperature variation. Changes in the temperature stability of the dielectric constant among different members of this series are shown to arise from changes in relative contributions from soft polar modes.

Charge-order driven multiferroic and magneto-dielectric properties of rare earth manganates

Charge-order driven magnetic ferroelectricity is shown to occur in several rare earth manganates of the general formula, Ln(1-x)A(x)MnO(3) (In = rare earth, A = alkaline earth). Charge-ordered manganates exhibit dielectric constant anomalies around the charge-ordering or the antiferromagnetic transition temperature. Magnetic fields have a marked effect on the dielectric properties of these compounds, indicating the presence of coupling between the magnetic and electrical order parameters. Magneto-dielectric properties are retained in small particles of the manganates. The observation of magneto-ferroelectricity in these manganates is in accordance with theoretical predictions.

Charge-order driven multiferroic and magneto-dielectric properties of rare earth manganates

Charge-order driven magnetic ferroelectricity is shown to occur in several rare earth manganates of the general formula, Ln(1-x)A(x)MnO(3) (In = rare earth, A = alkaline earth). Charge-ordered manganates exhibit dielectric constant anomalies around the charge-ordering or the antiferromagnetic transition temperature. Magnetic fields have a marked effect on the dielectric properties of these compounds, indicating the presence of coupling between the magnetic and electrical order parameters. Magneto-dielectric properties are retained in small particles of the manganates. The observation of magneto-ferroelectricity in these manganates is in accordance with theoretical predictions.

Multiferroic and magnetoelectric properties of core-shell CoFe2O4@BaTiO3 nanocomposites

Core-shell CoFe2O4@BaTiO3 nanoparticles and nanotubes have been prepared using a combination of solution processing and high temperature calcination. Both the core-shell nanostructures exhibit magnetic and dielectric hysteresis at room temperature and magnetoelectric effect. The dielectric constant of both the nanocomposites decreases upon application of magnetic field. The core-shell nanoparticles exhibit 1.7% change in magnetocapacitance around 134 K at 1 T, while the core-shell nanotubes show a remarkable 4.5% change in magnetocapacitance around 310 K at 2 T.(C) 2010 American Institute of Physics. [doi:10.1063/1.3478231].

Influence of growth ambience and doping on the structural properties of multiferroic DyMnO3

We report on the single crystal growth of 50% Sr and Y doped multiferroic DyMnO3 using optical floating zone technique. A comparison of the effect of growth ambience and of chemical substitution on the crystal structure of DyMnO3 is attempted. It is observed that DyMnO3 adopts Pm3m cubic structure with 50% Sr doping whereas with 50% Y doping, the crystal structure is hexagonal P6(3)cm. Orthorhombic Pnma structure is adopted by DyMnO3 when grown in air, whereas hexagonal P6(3)cm structure is obtained when grown under the ambience of argon. The structural polymorphism is discussed in terms of difference in ionic sizes of Sr, Y and Dy, comparable Gibbs free energies and coordination schemes of surrounding oxygens for hexagonal and orthorhombic structures of DyMnO3. (C) 2012 Elsevier B.V. All rights reserved.

Enhanced electric field tunable magnetic properties of lead-free Na0.5Bi0.5TiO3-MnFe2O4 multiferroic composites

Strong magnetoelectric (ME) interaction was exhibited at both dc and microwave frequencies in a lead-free multiferroic particulate composites of Na0.5Bi0.5TiO3 (NBT) and MnFe2O4 (MFO) multiferroic, which were prepared by sol-gel route. The room temperature permeability measurements were carried out in the frequency range of 1 MHz-1 GHz. A systematic study of structural, magnetic and ME properties were undertaken. The room temperature ferromagnetic resonance (FMR) was studied. Strong ME coupling is demonstrated in 70NBT-30MFO composite by an electrostatically tunable FMR field shift up to 428 Oe (at E = 4 kV/cm), which increases to a large value of 640 Oe at E = 8 kV/cm. Furthermore, these lead-free multiferroic composites exhibiting electrostatically induced magnetic resonance field at microwave frequencies provide great opportunities for electric field tunable microwave devices.

Effect of substitution of Y on the structural, magnetic, and thermal properties of hexagonal DyMnO3 single crystals

We investigate the structural, magnetic, and specific heat behavior of the hexagonal manganite Dy0.5Y0.5MnO3 in order to understand the effect of dilution of Dy magnetism with nonmagnetic yttrium. In this compound, the triangular Mn lattice orders antiferromagnetic at T-N(Mn) approximate to 68 K observed experimentally in the derivative of magnetic susceptibility as well as in specific heat. In addition, a low-temperature peak at T-N(Dy) similar to 3 K is observed in specific heat which is attributed to rare earth order. The T-N(Mn) increases by 9 K compared to that of hexagonal (h) DyMnO3 while T-N(Dy) is unchanged. A change in slope of thermal evolution of lattice parameters is observed to occur at temperature close to T-N(Mn). This hints at strong magnetoelastic coupling in this geometric multiferroic. In magnetization measurements, steplike features are observed when the magnetic field is applied along the c axis which shift to higher fields with temperature and vanish completely above 40 K. The presence of different magnetic phases at low temperature and strong magnetoelastic effects can lead to such field-induced transitions which resemble metamagnetic transitions. This indicates the possibility of strong field-induced effects in dielectric properties of this material, which is unexplored to date.

Interplay of structural distortions, dielectric effects and magnetic order in multiferroic GdMnO3

Multiferroic materials are characterized by simultaneous magnetic and ferroelectric ordering making them good candidates for magneto-electrical applications. We conducted thermal expansion and magnetostriction measurements in magnetic fields up to 14 T on perovskitic GdMnO3 by highresolution capacitive dilatometry in an effort to determine all longitudinal and transversal components of the magnetostriction tensor. Below the ordering temperature T (N) = 42 K, i.e., within the different complex (incommensurate or complex) antiferromagnetic phases, lattice distortions of up to 100 ppm have been found. Although no change of the lattice symmetry occurs, the measurements reveal strong magneto-structural phenomena, especially in the incommensurate sinusoidal antiferromagnetic phase. A strong anisotropy of the magnetoelastic properties was found, in good agreement with the type and propagation vector of the magnetic structure. We demonstrate that our capacitive dilatometry can detect lattice expansion effects and changes of the dielectric permittivity simultaneously because the sample is housed inside the capacitor. A separation of both effects is possible by shielding the sample. Dielectric transitions could be detected by this method and compared to the critical values of H and T in the magnetic phase diagram. Dielectric changes measured at 1 kHz excitation frequency are detected in GdMnO3 at about 180 K, and between 10 K and 25 K in the canted antiferromagnetic structure which is characterized by a complex magnetic order on both the Gd- and Mn-sites.

Metastable morphotropic phase boundary state in the multiferroic BiFeO3-PbTiO3

Temperature-time study of the magnetoelectric multiferroic (1-x)BiFeO3-(x)PbTiO3 by x-ray and electron diffraction on the reported morphotropic phase boundary (MPB) compositions revealed that this MPB does not correspond to the equilibrium state. The MPB like state is rather of metastable nature and arise due to kinetic arrest of metastable rhombohedral (R3c) phase, along with the equilibrium tetragonal (P4mm) phase. The life time of the metastable R3c nuclei is very sensitive to composition and temperature, and nearly diverges at x -> 0.27. The MPB like state appears only if the system is cooled before the metastable R3c nuclei could vanish. These findings resolve the long standing controversy with regard to seemingly erratic phase formation behaviour reported by different groups and provides a rational basis for developing genuine equilibrium MPB compositions in this system for better piezoelectric properties. (C) 2013 AIP Publishing LLC.

Stabilization of metastable tetragonal phase in a rhombohedral magnetoelectric multiferroic BiFeO3-PbTiO3

The phase formation behaviour of the magnetoelectric multiferroic 0.8BiFeO(3)-0.2PbTiO(3) was studied as a function of heat treatment at different temperatures of a sol-gel derived powder. While under ordinary synthesis conditions this composition exhibits antiferromagnetic ordering and a rhombohedral structure; the sol-gel-enabled low-temperature synthesis could stabilize a tetragonal metastable phase along with the stable rhombohedral phase, mimicking a morphotropic phase boundary state. The phase coexistence state exhibits relatively enhanced ferromagnetic correlation. The same system with a relatively higher PbTiO3 concentration, 0.65BiFeO(3)-0.35PbTiO(3), on the other hand, exhibits a rhombohedral metastable phase. These results suggest that the occurrence of metastable phases is a very common feature in the BiFeO3-PbTiO3 magnetoelectric ferroelectric system and that it affects the ferroelectric and magnetic properties of system quite remarkably.

Equilibrium phases in the multiferroic BiFeO3-PbTiO3 system - a revisit

The(1-x) BiFeO3-(x) PbTiO3 solid solution exhibiting a Morphotropic Phase Boundary (MPB) has attracted considerable attention recently because of its unique features such as multiferroic, high Curie point (T-C similar to 700 degrees C) and giant tetragonality (c/a -1 similar to 0.19). Different research groups have reported different composition range of MPB for this system. In this work we have conclusively proved that the wide composition range of MPB reported in the literature is due to kinetic arrest of the metastable rhombohedral phase and that if sufficient temperature and time is allowed the metastable phase disappears. The genuine MPB was found to be x=0.27 for which the tetragonal and the rhombohedral phases are in thermodynamic equilibrium. In-situ high temperature structural study of x=0.27 revealed the sluggish kinetics associated with the temperature induced structural transformation. Neutron powder diffraction study revealed that themagnetic ordering at room temperature occurs in the rhombohedral phase. The magnetic structure was found to be commensurate G-type antiferromagnetic with magnetic moments parallel to the c-direction (of the hexagonal cell). The present study suggests that the equilibrium properties in this solid solution series should be sought for x=0.27.