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Magnetoelectric (ME) materials exhibit interesting physics with cross coupling between ferroelectric and magnetic order parameters and thus strong potential to be utilized in memory, spintronics and other multifunctional electronic/magnetic devices. Doping of suitable transition metals in ferroelectrics can induce magnetism and ME coupling and modify the physical properties. Here, we report the structural, electronic, magnetic and ME coupling of 3.5, 5 and 7.5 mol% cobalt doped BaTiO3 (BTO) ceramics. X-ray diffraction and Raman spectroscopy indicate that the samples are single phase having a tetragonal crystal structure with P4mm symmetry. The tetragonality ratio is found to decrease with increasing cobalt content. We observed a Fano-like asymmetric peak in the [A1(LO1)] Raman mode at ∼173 cm−1 in all the cobalt doped BTO samples. The cobalt dopants are shown to be uniformly distributed throughout the surface of the samples. We observed a lowering of the ferroelectric transition temperature and increasing diffusivity parameter with increasing cobalt concentration. The electrical properties of all the samples have been investigated in detail by impedance spectroscopy and ac conductivity studies before and after the ferroelectric phase transitions. All the samples show hysteretic ferroelectric behavior with a clear saturation state that decreases with increasing cobalt content. The observed ferroelectricity in these samples is intrinsic in nature. The 3.5% cobalt doped BTO sample exhibits paramagnetic behavior whereas the 5 and 7.5% cobalt doped BTO samples show ferromagnetic ordering below 43 K. The 7.5% cobalt doped BTO samples show significant ME coupling.

There is increasing interest in novel magnetoelectric (ME) materials that exhibit robust ME coupling at room temperature (RT) for advanced memory, energy, spintronics, and other multifunctional device applications, by making use of the ability to control polarization with a magnetic field and/or magnetization via an electric field. Obtaining ME materials with strong ME coupling, understanding the origin, and manipulating its processing along with composition to realize large ME coefficients at RT constitute an important step in multiferroic research. To address this, we have investigated the multiferroic and ME properties of Ni-doped $\mathrm{Pb}({\mathrm{Zr}}_{0.20}{\mathrm{Ti}}_{0.80}){\mathrm{O}}_{3}$ (PZT). We find that the ferroelectric $({T}_{\mathrm{C}}\ensuremath{\sim}700\phantom{\rule{0.16em}{0ex}}\mathrm{K})$ and weak ferromagnetic (\ensuremath{\sim}602 K) phase transitions of Ni-doped PZT are well above room temperature (RT), leading to a strong ME coupling coefficient (${\ensuremath{\alpha}}_{E,31}$) of $11.7\phantom{\rule{0.16em}{0ex}}\mathrm{mV}\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{--1}\phantom{\rule{0.16em}{0ex}}{\mathrm{Oe}}^{--1}$ (${H}_{\mathrm{ac}}=1\phantom{\rule{0.16em}{0ex}}\mathrm{Oe}$ and $f=1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}$). While x-ray diffraction suggests a single-phase material, high-resolution transmission electron microscopy reveals regions with and without Ni present; thus magnetoelectric coupling between two phases is possible. First-principles calculations suggest the $(\mathrm{N}{\mathrm{i}}_{\mathrm{Pb}}{)}^{\ifmmode\times\else\texttimes\fi{}}$ defect is likely to be responsible for the experimental observed magnetism and ME coupling in Ni-doped PZT. We further demonstrate that Ni-doped PZT exhibits low loss tangent, low leakage current, large saturation polarization, and weak ferromagnetism. Ultimately, our work demonstrates that Ni-doped PZT is a cost-effective RT multiferroic with strong ME coupling.

Development of lead-free BaTiO3/NiFe2O4/BaTiO3 (BTO/NFO/BTO) trilayer structure thin films is significant for the realization of eco-friendly and implantable microelectromechanical systems (MEMS)-based devices. In the present work, we report BTO/NFO/BTO trilayer structure as a representative ferroelectric/ferromagnetic/ferroelectric (FE/FM/FE) system deposited on Pt(111)/TiO2/SiO2/Si using Pulsed Laser Deposition (PLD) technique. We report the ferroelectric, magnetic, and ME properties of BTO/NFO/BTO trilayer nanoscale heterostructure having dimensions 140/80/140 nm, at room temperature. High room temperature dielectric constant ~2145 at 100 Hz with low dielectric loss ~0.05 at 1 MHz is observed. Further, the deposited (BTO/NFO/BTO) tri-layered thin films showed magnetoelectric, multiferroic behavior with remanent polarization of 8.63 μCcm−2 at about 0.25 MV/cm and a reasonably high saturation magnetization of ~16 emu/cm3 at ~10 kOe is witnessed at room temperature. Tri-layered films have shown interesting magnetoelectric (ME) coupling coefficient (αE) ~54.5 mV/cm Oe at room temperature. Published version

Magnetoelectric (ME) heterostructures can exhibit higher magnetic and ferroelectric ordering temperatures along with large ME coupling compared to single-phase multiferroic materials. We synthesized Pb(Fe0.5Nb0.5)O3 (PFN)/Ni0.65Zn0.35Fe2O4 (NZFO)/Pb(Fe0.5Nb0.5)O3 (PFN)/Ni0.65Zn0.35Fe2O4 (NZFO)/Pb(Fe0.5Nb0.5)O3 (PFN) multilayer heterostructures having dimensions of 40/10/40/10/40 nm. High quality epitaxial growth of these heterostructures was confirmed via X-ray diffraction (XRD) and selected area electron diffraction (SAED) patterns. These nanostructures show well saturated polarization (∼52 μC cm−2) and magnetization (∼62 emu cm−3) at room temperature (RT). The magnetic and ferroelectric transitions occur well above RT. These heterostructures exhibit relaxor behavior and undergo 2nd order ferroelectric phase transition. Magnetodielectric measurements show significant coupling between the magnetic and electrical order parameters at RT. These characteristics of the heterostructures make them suitable as potential candidates for ultra-low power memory, spintronics, and different multifunctional (micro)nanoscale device applications.

This study reports the magnetocaloric effect (MCE) and piezoresponse of integrated ferroelectric-ferromagnetic heterostructures of PbZr 0.52Ti 0.48O 3 (PZT) (5 nm)/Bi-Sr-Ca-Cu 2-O X (BSCCO) (5 nm)/La 0.67Sr 0.33MnO 3 (LSMO) (40 nm)/MgO (0 0 1). Magnetic and pizoresponse behavior of the heterostructures are found to be governed by magneto-electric coupling and induced lattice strains. In addition, a maximum MCE is studied using Maxwell equations from both Field Cooled (FC) and Zero Field Cooled (ZFC) magnetization data. Maximum MCE entropy change (|ΔS|) of 42.6 mJkg −1K −1 (at 258 K) and 41.7 mJkg −1K −1 (at 269 K) are found corresponding to FC and ZFC data, respectively. The variation in maximum entropy change and corresponding temperatures for FC and ZFC data revealed that the application of a magnetic field can significantly contribute towards tuning of the MCE. Interestingly, these multilayered structures are found to sustain MCE over a broad temperature range, which makes them attractive for improved solid-state energy conversion devices.

Here, we have studied the phase transition and magneto-electric properties of a 70 wt. % Pb(Fe0.5Nb0.5)O3–30 wt. % Co0.6Zn0.4Fe1.7Mn0.3O4 (70 wt. % PFN–30 wt. % CZFMO) multiferroic composite that exhibits a maximum magneto-electric (ME) coefficient of 26.78 mV/cm Oe at room temperature. Raman analysis confirms the formation of composite and development of strain with the shifting of Raman modes. The local symmetry breaking of end members of the composite is observed by the splitting of Raman modes. The first-order derivative of magnetization with temperature (dM/dT vs T) shows anomalies across 140 K due to the PFN phase, whereas the anomaly around 250 K is due to the spin glass transition of the CZFMO phase. The magnetization vs magnetic field (M–H) study at different temperatures reveals the existence of superparamagnetic behavior above 300 K. The temperature-dependent dielectric behavior of the composite shows an anomaly around ferroelectric phase transition (Tm) for the PFN phase along with the broad relaxation peak arising due to the CZFMO phase. The linear behavior of magnetocapacitance (MD%) with the square of magnetization (M2) suggests the existence of biquadratic ME coupling. The ME study on the composite suggests the existence of both direct and converse ME effects.

Ba0.70Sr0.30TiO3-(BST) ceramics were fabricated by conventional mixed oxide route. The structural phase transition, ferroelectric, dielectric and energy storage properties of BST ceramics capacitor...

Bimetallic alloys with large discrepancies in atomic radii and crystal structure typically yield systems that are highly immiscible, even at high temperatures. The AgxFe1−x binary system has limited solid and liquid solubility and thus phase separated Ag + Fe alloys should result. Furthermore, Ag has interesting plasmonic properties and Fe is a strong ferromagnet, thus magneto-plasmonic nanoparticles/films should result due to their phase separation. We have leveraged a combinatorial sputter deposition to synthesize thin films with a large AgxFe1−x (0.19

We report a detailed investigation on magnetic and electrical properties of the multiferroic GaFeO3 (GFO) thin films grown on SrRuO3 (SRO) buffered SrTiO3 (1 1 1) substrates. The magnetic transition temperature (Tc) of GFO thin films is observed ∼240 K, which is higher by 20 K than in GFO ceramic. The clear and reversible out-of-plane phase-contrast seen in the Piezoresponse Force Microscopy (PFM) phase and amplitude images measured within positive and negative poling confirms the polarization reorientation and hence piezoelectric nature of the compound. The temperature and frequency dependence of permittivity studies demonstrates the relaxor behavior of these thin films. The observed near room temperature (RT) magnetic phase transition with RT piezoelectric nature of these thin films elucidates the possible potential candidates for a multiferroic world with spintronics device applications.

Modifying Fe and Mn contents in GaFeO3 (GFO) enhances the magnetic properties, increases the magnetic transition temperature (TC) and reduces the leakage current. Here, we report structural, magnetic, and leakage current characteristics of manganese-doped gallium ferrite with different Fe-content, i.e. Ga2−xFexO3 (1 ≤ x ≤ 1.4) system. Structural characterization reveals that all the samples retain the orthorhombic phase with space group Pc21n for above amounts of doping. Magnetization of the samples with respect to temperature shows the lower magnetic transition temperature (TC) for pure GFO, i.e. 220 K, which increases to 345 K above room temperature (RT) for 2% Mn-doped Ga0.6Fe1.4O3 (GFMO3). Higher remanent magnetization (~16 emu g−1) with a lower coercive field (~4 kOe) is obtained for Mn-doped Ga0.6Fe1.4O3. We found the decrease of leakage current with doping of Mn. The observation of multiferroicity in these single-phase materials (i.e. GFO3 and GFMO3) at RT make them potential candidates for memory, multifunctional, and spintronics device applications.

Multiferroic materials have attracted considerable attention as possible candidates for a wide variety of future microelectronic and memory devices, although robust magnetoelectric (ME) coupling between electric and magnetic orders at room temperature still remains difficult to achieve. In order to obtain robust ME coupling at room temperature, we studied the Pb(Fe0.5Nb0.5)O3/Ni0.65Zn0.35Fe2O4/Pb(Fe0.5Nb0.5)O3 (PFN/NZFO/PFN) trilayer structure as a representative FE/FM/FE system. We report the ferroelectric, magnetic and ME properties of PFN/NZFO/PFN trilayer nanoscale heterostructure having dimensions 70/20/70 nm, at room temperature. The presence of only (00l) reflection of PFN and NZFO in the X-ray diffraction (XRD) patterns and electron diffraction patterns in Transmission Electron Microscopy (TEM) confirm the epitaxial growth of multilayer heterostructure. The distribution of the ferroelectric loop area in a wide area has been studied, suggesting that spatial variability of ferroelectric switching behavior is low, and film growth is of high quality. The ferroelectric and magnetic phase transitions of these heterostructures have been found at ~575 K and ~650 K, respectively which are well above room temperature. These nanostructures exhibit low loss tangent, large saturation polarization (Ps ~ 38 µC/cm2) and magnetization (Ms ~ 48 emu/cm3) with strong ME coupling at room temperature revealing them as potential candidates for nanoscale multifunctional and spintronics device applications.

We report studies of the ferroelectric and magnetic phase transitions of (1 – x)Pb(Fe0.5Nb0.5)O3 – xCo0.65Zn0.35Fe2O4 (x = 0.2) composite with emphasis upon the nature of magnetoelectric coupling at room temperature. The presence of all cationic elements with their required stoichiometry have been confirmed by SEM and XPS studies. The composite shows well-saturated ferroelectric and ferromagnetic (multiferroic) behavior at room temperature. A ferroelectric-paraelectric phase transition has been confirmed from the temperature dependent dielectric spectra along with DSC and Raman spectroscopic studies. Antiferromagnetic, ferromagnetic, and relaxor paramagnetic states have been observed in this composite. This composite shows strong bulk biquadratic magnetoelectric coupling at room temperature, which can be useful for potential multifunctional device applications.

The bismuth layer structured ferroelectric (BLSF) ceramics consisting of four-layers (BaLa0.75Bi3.25Ti4O15) and five-layers (Ba2La0.75Bi3.25Ti5O18) were prepared by the conventional solid-state reaction method. Summerfield ac-conductivity scaling analysis was used to evaluate the electrical behavior and the ac-conductivity isotherm curves. The relaxation results were corroborated with the Raman Peak positions and full width at half maximum was obtained by using Lorentzian peak fit method. Finally, the results were compared with the two-layered relaxor-compound (Bi2.45 La0.55TiNbO9) and technologically standard three-layered compounds (La0.75Bi3.25Ti3O12; BLT). The dielectric relaxation of Bi2.45La0.55TiNbO9 was verified using modified Curie-Weiss law and Vogel-Fulcher relationship. An attempt is made to realize the typical collective nature of the ionic conductivity of the samples.

Rare-earth (Sm) and transition metal (Co) modified polycrystalline BiFeO3 (BFO) thin films have been deposited on Pt/TiO2/SiO2/Si substrate successfully through pulsed laser deposition (PLD) technique. Piezoelectric, leakage current and temperature dependent dielectric and magnetic behaviour were investigated for the films. Typical \"butterfly-shaped\" loop were observed in BSFCO films with an effective piezoelectric constant (d(33)) similar to 94 pm/V at 0.6 MV/cm. High dielectric constant similar to 900 and low dielectric loss similar to 0.25 were observed at room temperature. M-H loops have shown relatively high saturation magnetization similar to 35 emu/cm(3) at a maximum field of H similar to 20 kOe. Enhanced magnetoelectric coupling response is observed under applied magnetic field. The multiferroic, piezoelectric, leakage current behaviours were explored. Such studies should be helpful in designing multiferroic materials based on BSFCO films. (C) 2014 Elsevier B.V. All rights reserved.

Ba0.70Ca0.30TiO3-(BCT),Ba(Zr0.2Ti0.8)O3-(BZT) ceramics were fabricated by conventional mixed oxide route to develop inorganic dielectric materials suitable for use as an insulator with high dielectric constant and low energy loss for capacitor applications. The structural phase transition, ferroelectric, dielectric and energy storage properties of BCT, BZT ceramic capacitors were investigated. Room temperature X-ray diffraction (XRD) patterns revealed prominent peaks corresponding to tetragonal perovskite crystal structure for both BCT, BZT solid solutions. Slim ferroelectric hysteresis (P-E) loops were observed for BCT, BZT solid solutions. Temperature dependent dielectric property measurements of BCT, BZT solid solutions have shown a high dielectric constant and low dielectric loss. Room temperature (300K) breakdown field strength and energy densities were obtained from the integral area of P-E loops. For the BCT ceramics, the largest recoverable energy (unreleased energy) density is 1.41 J/cm3 with die...

Magnetoelectric (ME) materials with ferroelectric and magnetic transition temperatures near room temperature are of current interest in research due to their technological importance and potential applications. Herein, we report the coupled magnetic ordering and phonons in gallium ferrite (GaFeO3), a near room temperature ME perovskite, using magnetization and inelastic light scattering measurements as a function of temperature. Temperature-dependent magnetization behavior studied in a wide temperature range of 5–395 K at both field-cooled (FC) and zero-field-cooled (ZFC) conditions using different static magnetic fields confirms the magnetic transition temperature Tc at 220 K. On temperature dependent Raman spectroscopy, no significant changes in Raman spectra were observed at an elevated temperature that can be attributed to the absence of structural phase transition. Instead of expected anharmonic behavior, several librational (rigid rotation) and stretching modes of rigid BO6 units were found to be hardening below Tc, suggesting the significant magnetoelastic coupling contributions to phonon frequencies. The asymmetric stretching mode at 753 cm−1 is found to have larger spin-phonon coupling contribution (λ∼2.93), while the lattice mode at 153 cm−1 and external librational mode at 240 cm−1 had the lowest effect (λ∼0.88).

This paper reports the development of a lead free {Ba(Zr 0.2 Ti 0.8 )O 3 } (1− x ) {(Ba 0.7 Ca 0.3 )TiO 3 } x – x =0.10, 0.15 and 0.20 – BZT–BCT ceramic solid solution system prepared using a solid-state reaction technique. The evolution of the Raman spectra with temperature was used to study the variation of the basic phase transition of BaTiO 3 in these compositions. The phase transition temperature on heating was found to decrease to 310 K, 300 K, and 300 K, respectively, with increasing Ca content on BCT end and decreasing Zr content on BZT end of lead free pseudobinary ferroelectric BZT–BCT system. Tetragonal and rhombohedral phase coexistence is observed at room temperature from X-ray diffraction (XRD) spectra. Rhombohedral phase is identified between the 83 K and 273 K from temperature dependent Raman studies. Raman results are in excellent agreement with those obtained from temperature dependent dielectric measurements. Bulk ceramic BZT–BCT materials have shown interesting temperature dependent dielectric properties and as well as higher values of room temperature dielectric constant ∼7800, 8400, 5200, dielectric tunability ∼82%, figure of merit (FOM) ∼93.71 % with low dielectric loss (tan δ ) ∼0.015 to 0.024 and good thermal stability at high sintering temperature (1600 °C); they might be one of the strong candidates for dielectric tunable capacitor applications in an environmentally protective atmosphere.

Multiferroic composite structures, i.e., composites of magnetostrictive and piezoelectric materials, can be envisioned to achieve the goal of strong room-temperature ME coupling for real practical device applications. Magnetic materials with high magnetostriction, high Neel temperature (TN), high resistivity and large magnetization are required to observe high ME coupling in composite structures. In continuation of our investigations on suitable magnetic candidates for multiferroic composite structures, we have studied the crystal structure, dielectric, transport, and magnetic properties of Co0.65Zn0.35Fe2O4 (CZFO). Rietveld refinement of X-ray diffraction patterns confirms the phase purity with a cubic crystal structure with the (Fdm) space group; however, we have found a surprisingly large magneto-dielectric anomaly at the Neel temperature, unexpected for a cubic structure. The presence of mixed valences of Fe2+/Fe3+ cations is probed by X-ray photoelectron spectroscopy (XPS), which supports the catonic ordering-mediated large dielectric response. Large dielectric permittivity dispersion with a broad anomaly is observed in the vicinity of the magnetic phase transition temperature (TN) of CZFO suggesting a strong correlation between dielectric and magnetic properties. The evidence of strong spin-polaron coupling has been established from temperature dependent dielectric, ac conductivity and magnetization studies. The ferrimagnetic–paramagnetic phase transition of CZFO has been found at ∼640 K, which is well above room temperature. CZFO exhibits low loss tangent, a high dielectric constant, large magnetization with soft magnetic behavior and magnetodielectric coupling above room temperature, elucidating the possible potential candidates for multiferroic composite structures as well as for multifunctional and spintronics device applications.

The polycrystalline sample of (K0.5Bi0.5)(Fe0.5Nb0.5)O3 was synthesized by a high- temperature solid-state reaction technique. The material crystallizes in cubic structure at room temperature. The dielectric properties of the material were investigated in a temperature range from 30-200 oC in the frequency range (10 2 -10 7 Hz). Impedance data is well fitted using proper equivalent circuit composed of a parallel resistance and capacitance in series with a parallel resistance, constant phase element and a capacitance. The compound shows a typical negative temperature coefficient of resistance type (NTCR) behavior like that of semiconductors. Modulus spectroscopy and dielectric conductivity formalism were employed to study dielectric relaxation phenomena in the material. The frequency dependence of conductivity is well fitted to Jonscher's single power law. Copyright © 2012 VBRI Press.

Bismuth ferrite- (BiFeO3) ceramic is the most studied and attractive multiferroic material with low magnetization, moderate leakage current, and low polarization. Samarium substituted bulk BiFeO3 prepared at low synthesis temperature ∼600 °C by the sol–gel process. Room temperature X-ray diffraction (XRD) patterns confirmed the formation of perovskite structure Bi0.9Sm0.10FeO3 (BSFO) phases. Present compositions possess high dielectric constant (e≈199) and low dielectric loss (tanδ≈0.009) at room temperature for 100 Hz frequency. Room temperature dielectric permittivity and dielectric loss decreased with increasing frequency from 100 Hz to 10 MHz. As the temperature increased, an enormous increase in both dielectric permittivity and dielectric loss is observed at all frequency regions. Temperature dependent M–H hysteresis loops were saturated. Spin glass-like ferromagnetic behavior is retained in M–H hysteresis loops measured from the low temperature region and normal ferromagnetic behavior is observed in the high temperature region, both at room temperature and above ∼350 K, 400 K, respectively. The origin of the ferromagnetic property in BSFO may be due to the presence of rare earth metal ions at the lattice sites of BFO.

Piezoelectric and other physical properties are significantly enhanced at (or near) a morphotropic phase boundary (MPB) in ferroelectrics. MPB materials have attracted significant attention owing to both fundamental physics as well as the possibility of well-regulated energy and information storage devices which are dominated by lead (Pb)-based materials. Here, we report the crystal structure, Raman spectra, dielectric constant and polarization near the MPB of lead free (1 - x) Na0.5Bi0.5TiO3 - x BaTiO3 (0.00 ⩽ x ⩽ 0.10) solid-solution, prepared by sol-gel auto combustion technique and sintered by microwave sintering technique. With the addition of BaTiO3 into Na0.5Bi0.5TiO3, it induces a structural phase transition from R3c (a single phase) to R3c + P4mm (a dual phase) close to x = 0.06 and 0.07 and transform to a high symmetry tetragonal phase P4mm at higher compositions (x = 0.08 to 0.10) as evident from our x-ray Rietveld refinement and Raman spectroscopic results. We perform first-principles calculations based on density functional theory that confirm a structural transition from a rhombohedral to a tetragonal phase under increasing x. In the prepared solid solution, an anomalous enhancement of remnant polarization ([Formula: see text]) was observed for x = 0.06 and 0.07, which has been explained based on the existence of the MPB. On the other hand, the value of coercive field [Formula: see text] was found to be decreased linearly from x = 0.00 to 0.06; it is constant for higher compositions. Further details of the ferroelectric properties on the electric field poled samples have been studied and compared with the as-grown (unpoled) samples.

The search for a room temperature single phase multiferroic material displaying strong magnetoelectric coupling and low leakage current for practical device applications has been underway and a long-standing challenge. In continuation to our investigations for achieving robust ME coupling and enhanced electrical insulation at room temperature, we report magnetic, electrical insulation, and magneto-dielectric properties of Nd and Mn co-doped BiFeO3 (Bi0.95Nd0.05)(Fe0.97Mn0.03)O3 (BNFM) polycrystalline electro-ceramics. Magnetic studies have been carried out in two different temperature regions, i.e., 15–300 K and 300–800 K. The doping of Nd and Mn in the BiFeO3 (BFO) lattice slightly reduces the Neel temperature (TN) with broad weak ferromagnetic (FM) to paramagnetic (PM) phase transition by increasing ferromagnetic domain fractions. A small amount of magnetic frustration is also found in the low temperature regions, below 300 K at fields of 100 and 200 Oe, and below 200 K at higher field cooled and zero f...

We report photovoltaic (PV) effect in multiferroic Bi0.9Sm0.1Fe0.95Co0.05O3 (BSFCO) thin films. Transition metal modified polycrystalline BiFeO3 (BFO) thin films have been deposited on Pt/TiO2/SiO2/Si substrate successfully through pulsed laser deposition (PLD). PV response is observed under illumination both in sandwich and lateral electrode configurations. The open-circuit voltage (V-oc) and the short-circuit current density (J(sc)) of the films in sandwich electrode configuration under illumination are measured to be 0.9 V and -0.051 mu A cm(-2). Additionally, we report piezoresponse for BSFCO films, which confirms ferroelectric piezoelectric behaviour.

This paper investigates the crystal structure, ferroelectric, temperature-dependent leakage current conduction mechanism and the piezoresponse force microscopy (PFM) behaviours of (Ba0.955Ca0.045) (Zr0.17Ti0.83)O3–BZT–BCT () films at the vicinity of the morphotropic phase boundary (MPB) of the [(1 − x) BaZr0.20Ti0.80O3–xBa0.70Ca0.30TiO3] () composition. Epitaxial BZT–BCT thin films were grown on conductive La0.5Sr0.5CoO3 (LSCO) layers coated onto MgO (1 0 0) single-crystal substrates by pulsed laser deposition (PLD). High resolution x-ray diffraction (HR-XRD) reciprocal space maps (RSMs) confirmed the epitaxy with in-plane tetragonal symmetry (c < a), and Raman spectra also revealed a tetragonal perovskite crystalline lattice structure. Polarisation studies demonstrate that BZT–BCT films exhibit a high saturation polarisation of 148 µC cm−2 and a high recoverable (discharged) energy-storage density of 39.11 J cm−3 at 2.08 MV cm−1. Temperature-dependent P–E hysteresis loops resulted in a decrease in polarisation. Temperature-dependent leakage current behaviour was obtained and possible conduction mechanism is discussed. PPFM images revealed switchable ferroelectric piezoelectric contrasts after the application of a ±9 V dc voltage on the conductive tip of the piezoresponse force microscope.

This work is partially supported by DST fast track Project No. SR/FTP/PS-16/2009. Dhiren K. Pradhan acknowledges IFN (NSF Grant No. EPS—01002410) for fellowship. The work at UPR was supported by National Science Foundation (NSF DMR 1410869) and Institute for Functional Nanomaterials (IFN). We report systematic studies on crystal structure and magneto-dielectric properties of (1 − x) BiFeO3-x DyMnO3 (0.0 ≤ x ≤ 0.2) nanoceramics synthesized by auto-combustion method. Rietveld refinement of X-ray diffraction data indicates a structural transition from R3c to R3c + Pn21a at x = 0.1. Field emission scanning electron micrographs display a decrease in grain size with increase in x. The presence of dielectric anomalies around antiferromagnetic transition temperature implies the magnetoelectric coupling. Dielectric measurements showed decrease in magnetic ordering temperature with increasing x in agreement with differential scanning calorimetry results. A significant increase in magnetization has been found with increasing DyMnO3 substitution. Magneto-impedance spectroscopy reveals a significant change (∼18%) in dielectricpermittivity at H = 2 T for x = 0.2. Publisher PDF

We report the crystal structure, dielectric, transport, and magnetic properties of Ni0.65Zn0.35Fe2O4. Rietveld refinement results of X-ray diffraction patterns confirm the phase formation of the material with cubic crystal structure ( Fd3¯m). The frequency dependent ac conductivity behavior obeys the Jonscher's power law and is explained using the jump relaxation model. The observed behavior of temperature dependent bulk conductivity is attributed to the variable-range hopping of localized polarons. The correlation of polaron conduction and high permittivity behavior of NZFO is established on the basis of long range and short range conduction mechanisms. The complex impedance spectra clearly show the contribution of both grain and grain boundary effect on the electrical properties.

We report magnetoelectric coupling and Raman spectroscopic studies on [(1 − x)Pb(Fe0.5Nb0.5)O3-xNi0.65Zn0.35Fe2O4] (x = 0.20) PFN-NZFO composite. Apart from the presence of zone centre Raman active modes of the parent compound, some new peaks are observed in the low frequency region. The electric field controlled peak position (∼48 cm−1) suggests that this mode is of magnetic origin. From temperature dependent Raman scattering studies, temperature coefficients for phonons of different symmetries were estimated. Our measurements on electrical control of magnetic order and magnetic control of electrical order confirmed the existence of converse and direct magnetoelectric coupling in this composite at room temperature.

Polycrystalline sample of lead-free 1/3( Ba 0.70 Sr 0.30 TiO 3) + 1/3( Ba 0.70 Ca 0.30 TiO 3) + 1/3( BaZr 0.20 Ti 0.80 O 3)( BST - BCT - BZT ) ceramic was synthesized by solid state reaction method. Phase purity and crystal structure of as-synthesized materials was confirmed by X-ray diffraction (XRD). Temperature-dependent dielectric permittivity studies demonstrated frequency-independent behavior, indicating that the studied sample has typical diffuse phase transition behavior with partial thermal hysteresis. A ferroelectric phase transition between cubic and tetragonal phase was noticed near room temperature (~ 330 K). Bulk P–E hysteresis loop showed a saturation polarization of 20.4 μC/cm2 and a coercive field of ~ 12.78 kV/cm at a maximum electric field of ~ 115 kV/cm. High dielectric constant (ε ~ 5773), low dielectric loss (tan δ ~ 0.03) were recorded at room temperature. Discharge energy density of 0.44 J/cm3 and charge energy density of 1.40 J/cm3 were calculated from nonlinear ferroelectric hysteresis loop at maximum electric field. Dielectric constant at variable temperatures and electric fields, ferroelectric to paraelectric phase transition and energy storage properties were thoroughly discussed.

We report the crystal structure, dielectric, magnetic, and magneto-electric properties of (1−x) BiFeO3-xYMnO3 (0.00 ≤ x ≤ 0.2) multiferroic nanoceramics prepared by auto-combustion technique. YMnO3 substitution is found to induce a structural phase transition from R3c to R3c+Pbnm after x ≈ 0.1 using Rietveld refinement technique. Field emission scanning electron micrographs show decrease in grain size with increase in YMnO3 content. The dielectric permittivity and loss tangent are found to be increased with composition x. The anomalies noticed from the temperature dependent dielectric analysis reveal the signature of magneto-electric coupling in the system. A decrease in magnetic ordering temperature as a function of composition is found from dielectric study. At room temperature, the dielectric permittivity of all the YMnO3 modified samples decrease with increasing magnetic field. The maximum value of magneto-electric coupling coefficient (e(H)-e(0))/e(0) is found to be ∼ −5.5% at H = 2 T for x = 0.2. The behaviour of the magnetic hysteresis loop observed at room temperature suggests the suppression of space modulated spin structure.

Alkali-free [0.10 BaO + 0.4 B2O3 + 0.5 ZnO], [0.3 BaO + 0.6 B2O3 + 0.1 ZnO] glass powder materials were mixed with [(BaZr0.2Ti0.80)O3]0.85 − [(Ba0.70Ca0.30)TiO3]0.1—BZT–BCT ceramic materials for energy density storage capacitor applications. Calcined (1,250 °C/10 h) BZT–BCT ceramic powder materials were mixed with (15 wt. %) two different glass compositions of [0.10 BaO + 0.4 B2O3 + 0.5 ZnO], [0.3 BaO + 0.6 B2O3 + 0.1 ZnO] separately and were ground using low energy ball milling for 2 h at 400 rpm. The ball milled powders were made into discs having 13 mm diameter and 0.5 mm thickness using hydraulic press (2 ton) and sintered at 900 °C for 2 h. Both the compositions have shown dielectric breakdown field strength ~260, 280 kV/cm and energy density values ~1.118 and 0.50 J/cm3.