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Lead-free piezoelectric ceramics of (1 − x)K0.5Na0.5NbO3-xCaTiO3 were fabricated, and their crystal structure, microstructure, and electrical properties were systematically studied. Rietveld refinement of the x-ray diffraction data and Raman spectroscopic analyses revealed a composition-dependent structural phase transition: three phase transitions, namely, from a pure orthorhombic phase for x ≤ 0.02 to a mixed phase of orthorhombic and tetragonal phases (0.03 ≤ x ≤ 0.08) and finally another mixed phase of tetragonal + cubic for x = 0.10 and 0.15 at room temperature (RT). The morphological study reveals a decrease in grain size along with a more uniform distribution of grains as the concentration of CaTiO3 (CT) increases; notably, a homogeneous distribution of grains is observed for x = 0.05. The temperature-dependent dielectric properties show two phase transitions, from orthorhombic to tetragonal (TO-T) and tetragonal to cubic (TC), for unmodified K0.5Na0.5NbO3 (KNN). However, both the phase transition temperatures (TO-T and TC) decrease, and the transition peaks broaden with an increase in CT substitution, and for x > 0.06, the TO-T shifted below RT. The broadening of the transition peak at TO-T may be due to the relaxation behavior. Among the prepared samples, the 5 mol. % CT-modified KNN shows the optimum electrical properties (d33 = 114 pC/N, ɛr = 412, and 2Pr = 15.25 μC/cm2) at RT. The enhanced electrical properties for x = 0.05 are due to the coexistence of orthorhombic and tetragonal phases, facilitating easy polarization rotation and flattening of the free energy profile. A phase diagram has been constructed based on the information gathered from the temperature-dependent dielectric measurements, RT x-ray diffraction, and Raman spectroscopy data and is discussed in detail. [ABSTRACT FROM AUTHOR]

Multiferroic composites consisting of a single-phase multiferroic [0.6(PbZr0.53Ti0.47O3)-0.4(PbFe0.5Ta0.5)O3] as a matrix and a magnetostrictive phase (Co0.6Zn0.4Fe1.7Mn0.3O4) dispersed in the matrix are fabricated via hybrid synthesis technique. The structure and surface morphology studies using x-ray diffraction and field emission scanning electron microscopy techniques indicate the formation of 3-0 type particulate composites. Coexistence of soft-magnetic behavior and ferroelectric characteristics are confirmed for composites from magnetization vs magnetic field (M–H) and polarization vs electric field (P–E) measurements, respectively. Magneto-dielectric (MD) measurement shows significant changes in the dielectric properties with the application of a magnetic field, indicating the existence of strong MD behavior. The biquadratic nature of magneto-electric (ME) coupling is described by the Landau free energy equation arising from the strain transfer at the interfaces between the constituent phases. The direct magneto-electric voltage coefficient measurement also confirms very strong coupling between ferroelectricity and magnetism and supports the strain-mediated magneto-electric effect in composites. The Φ = 0.3 composite exhibits the maximum ME coefficient of 20.72 mV/cm Oe with MS = 24.62 emu/g, HC = 59.66 Oe, and piezoelectric coefficient value d33 = 19 pC/N. The strong magneto-electric effect along with low dielectric loss at room temperature in these composites suggests their suitability for multifunctional magneto-electric device applications such as magnetic sensors, etc. [ABSTRACT FROM AUTHOR]

Doping of suitable metal ions in ferroelectric oxides modifies the physical properties and can induce additional functionalities. Here, we present a detailed study on the effects of Sm concentration on the structural, dielectric, ferroelectric, and piezoelectric properties of ((K0.5Na0.5)1−3xSmx)NbO3 (KNSN) (0.00 ≤ x ≤ 0.02) ceramics. X‐ray diffraction and Raman spectroscopic analysis indicate that KNSN ceramics exhibit the single‐phase orthorhombic (Amm2) structure for x = 0.00 and the coexistence of orthorhombic and tetragonal (Amm2 + P4mm) structure for the composition range 0.005 ≤ x ≤ 0.02. The tetragonal phase fraction increases with an increase in Sm concentration. We observed dielectric relaxation behavior in KNSN at orthorhombic to tetragonal (TO–T) phase transition temperature, and its origin can be attributed to the structural heterogeneity at the inter‐ferroelectric phase boundary. Increasing Sm concentration leads to the broadening of the ferroelectric phase transition peaks. Further, the structural heterogeneity of the ceramics was seen from the slope of the dielectric constant versus log frequency and central peak behavior of Raman spectra at room temperature (RT). The study reveals that x = 0.005 shows maximum dielectric constant (Ɛr = 583), remanent polarization (2Pr = 57.02 μC/cm2), and piezoelectric coefficient (d33 = 94 pC/N) at RT and is associated with increased local structural heterogeneity due to Sm doping. [ABSTRACT FROM AUTHOR]

In this article, we present the results of low-temperature dielectric, magnetic and magnetodielectric properties of BiFeO3 nanoceramics prepared by auto-combustion method. Rietveld refinement results of X-ray diffraction data show that sample crystallizes in single-phase rhombohedral perovskite structure with R3c (No. 161) space group. The average crystallite size was found to be ≈ 600 Å from Williamson–Hall analysis. The temperature-dependent dielectric data have been presented in permittivity and modulus formalism to understand the relaxation dynamics. Three non-Debye-type relaxation processes were observed in the experimental window (173 to 423 K), which are explained using Kohlrausch–Williams–Watts (KWW) decay function. The temperature variation of relaxation times obeys Arrhenius's behaviour. The anomaly observed in the temperature dependence of relaxation times data near 240 K corresponds to the magnetic transition of BiFeO3. We found that single ionized oxygen vacancies with activation energy ranging from 0.4 to 0.8 eV are involved in the relaxation process. A crossover from AFM/PM to weak ferromagnetic ordering is observed at low temperature. The variation of capacitance with an applied magnetic field shows a hysteresis effect. The magnetocapacitance (MC%) changes by 3% at a magnetic field of 2 T for 200 kHz, indicating an intrinsic bulk magnetocapacitance effect in the ceramics. Hence, the above findings highlight the significance of the material as a potential candidate for device applications. [ABSTRACT FROM AUTHOR]

Ferroelectric materials exhibiting switchable and spontaneous polarization have strong potential to be utilized in various novel electronic devices. Solid solutions of different perovskite structures induce the coexistence of various phases and enhance the physical functionalities around the phase coexistence region. The construction of phase diagrams is important as they describe the material properties, which are linked to the underpinning physics determining the system. Here we present the phase diagram of (K0.5Na0.5NbO3)–(Ba0.5Sr0.5TiO3) (KNN-BST) system as a function of composition and their associated physical properties. Lead-free (1 − x)KNN–xBST (0 ≤ x ≤ 0.3) solid solution ceramics were synthesized by conventional solid-state reaction technique. The X-ray diffraction and Raman spectroscopic studies indicate composition-dependent structural phase transitions from an orthorhombic phase for x = 0 to orthorhombic + tetragonal dual-phase (for 0.025 ≤ x ≤ 0.15), then a tetragonal + cubic dual-phase (x = 0.2) and finally a cubic single phase for x ≥ 0.25 at room temperature (RT). Among these, the orthorhombic + tetragonal dual-phase system shows an enhanced value of the dielectric constant at room temperature. The phase transition temperatures, orthorhombic to tetragonal (TO-T) and tetragonal to cubic (TC), decrease with the increase in BST concentrations. The ferroelectric studies show a decrease of both 2Pr and EC values with a rise in BST concentration and x = 0.025 showed a maximum piezoelectric coefficient. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Magnetoelectric (ME) composite thin films are promising candidates for novel applications in future nanoelectronics, spintronics, memory, and other multifunctional devices as they exhibit much higher ME coupling and transition temperatures (Tc) than well-known single phase multiferroics discovered to date. Among the three types of multiferroic composite nanostructures, (2–2) layered and (1–3) vertically aligned composite nanostructures exhibit comparatively smaller ME coupling due to different shortcomings that restrict their use in many applications. Here, we study the morphological, piezoresponse force microscopic (PFM), ferroelectric, magnetic, and magnetodielectric properties of 0–3 [magnetic nanoparticles (0) homogeneously distributed in ferroelectric matrices (3)] multiferroic composite thin films. The Pb(Fe0.5Nb0.5)O3 (PFN)–Ni0.65Zn0.35Fe2O4 (NZFO) particulate composite films were synthesized by pulsed laser deposition. These particulate composite thin films are completely c-axis oriented with very low surface roughness. We observed magnetic and ferroelectric Tc above room temperature (RT) for all composite thin films. The PFN–NZFO 0–3 composites exhibit large polarization, high saturated magnetization with low coercive field, and low dielectric loss along with magnetodielectric coupling at RT. These nanocomposites might be utilized in next generation nano/microelectronics and spintronic devices. [ABSTRACT FROM AUTHOR]

In this study, the impact of Nd doping on the structural, microstructural, dielectric, ferroelectric, and transport properties of Pb (1 - x) Nd x (Fe 0.5 Nb 0.5) 1 - x / 4 O 3 (PNFN) solid solutions ( x = 0 , 0.02 , 0.04 , 0.08 , and 0.1 ) is reported. For all the solid solutions, room temperature Rietveld refined X-ray diffraction (XRD) analysis reveals the monoclinic crystal structure with Cm space group. From Field emission scanning electron microscope (FESEM) studies, the polyhedral-shaped grains are found to be homogeneously distributed. Variation of dielectric properties with temperature displays the decrease of phase transition temperature (TC) with increasing Nd content. The temperature-dependent AC conductivity follows the Arrhenius behavior and the activation energies are calculated for high temperature regions. The frequency dependent AC conductivity behavior obeys the Johnscher's power law. Impedance spectroscopy results show the impact of conductivity from the bulk (grain) and displays non-Debye type of behaviour. Electric modulus demonstrates thermally activated relaxation phenomenon in the materials. Polarization vs. electric field (P-E) loops analysis confirms the ferroelectric nature of the materials. With increase in Nd concentrations, the value of remanent polarization (2Pr) increases, on the other hand, the coercive field (2Ec) value decreases. Both of these properties are suitable for enhancement of the physical properties of the multiferroic materials. [ABSTRACT FROM AUTHOR]

The single-phase (HfxZr0.8−x) (Ta0.1Dy0.1) O2 with 0.2 ≤ x ≤ 0.6 ceramics were synthesized by conventional solid-state reaction. The structural and morphological/microstructural characteristics were studied using x-ray diffraction and scanning electron microscopy, respectively. The dielectric properties and electrical conductivity of the bulk material were investigated as a function of temperature and frequency in the metal–insulator–metal configuration. The room-temperature dielectric constant at 100 kHz was found to be in the range of 17–35, along with low dielectric loss < 0.02. The leakage current densities at 3 kV/cm were 3.085 × 10−5, 1.67 × 10−5, and 3.93 × 10−6 A/cm2 for (Hf0.2Zr0.6)(Ta0.1, Dy0.1) O2, (Hf0.4Zr0.4)(Ta0.1, Dy0.1)O2, and (Hf0.6Zr0.2)(Ta0.1Dy0.1)O2, respectively. The frequency dependence of ac conductivity obeyed the Jonscher power law, suggesting hopping-based conduction. [ABSTRACT FROM AUTHOR]

In this report, we have investigated the effect of BaTiO3 on the preliminary structural analysis, ferroelectric phase transition and electrical properties of (1 − x) P b (F e 0.5 N b 0.5 ) O 3 − x B a T i O 3 (P F N − B T) (x = 0 , 0.025 , 0.05, and 0.1) solid solutions. Conventional solid-state reaction technique is adopted to synthesize P F N − B T solid solution. X-ray diffraction (XRD) analysis is used to study the preliminary structural analysis, which suggests the formation of the single-phase materials. The surface morphology is studied using field emission scanning electron microscope (FESEM). The temperature-dependent dielectric properties display a broad diffuse phase transition from ferroelectric to paraelectric state and the phase transition temperature was found to be decreased with an increase in BT concentrations. Ferroelectric property of the solid solutions is confirmed by the polarization vs. electric field (P–E) loops study at room temperature. Variation of AC conductivity with frequency and temperature is also studied. The addition of BT leads to a decrease in the dielectric loss and phase transition temperature. [ABSTRACT FROM AUTHOR]

With the rapid development of new device miniaturization technology, there is invigorated interest in magnetic nanostructures for potential application in novel multifunctional devices. In continuation to our search for a suitable magnetic material having Curie temperature (Tc) well above room temperature for multifunctional applications, we have studied the dielectric, optical, magnetic, and resistance switching characteristics of Ni0.65Zn0.35Fe2O4 (NZFO) thin films. The observation of only (004) reflection in the X-ray diffraction patterns confirms the c-axis orientation and high quality growth of NZFO thin films. The presence of mixed valences of Fe2+/Fe3+ cations is probed by X-ray photon spectroscopy, which supports the cationic ordering-mediated large dielectric response. Our investigations reveal NZFO to be an indirect band gap material (~1.8eV) with a direct gap at ~2.55eV. These nanostructures exhibit high saturation magnetization and a low coercive field with a ferrimagnetic-paramagnetic phase transition of ~713K. Magnetic force microscopy studies revealed the stripe-like domain structure of the investigated thin films. In addition, these thin films exhibit reliable and repeatable unipolar resistive switching characteristics. The observed high dielectric permittivity with low loss tangent, large magnetization with soft magnetic behavior, striped magnetic domain structure and reliable resistance switching in NZFO thin films above room temperature suggest potential application in memory, spintronics, and multifunctional devices. [ABSTRACT FROM AUTHOR]

This manuscript presents a systematic study of conductivity and dielectric relaxations in the solid solution of (BiFeO3)1-x -(YMnO3)x for compositional range (0.0 ≤ x ≤ 0.2) as function of frequency, temperature, and magnetic field. The samples have been synthesized by combustion method. The thermal activations of dc-conductivity and relaxation time obey Arrhenius behavior for, x = 0.0, 0.025, 0.05 but follow variable range hopping of small polarons above, x ≥ 0.075 with activation energy 0.45 eV. The compositional time-temperature superposition of dielectric modulus data suggests that conduction mechanism changes with composition. The bulk capacitance decreases with increase in magnetic field. [ABSTRACT FROM AUTHOR]

Spinel ferrites have been widely studied due to their remarkable properties such as high saturation magnetisation, large magnetic permeability, and high electrical resistivity. Among the oxides-based magneto strictive spinel ferrite, CoFe2O4 (CFO) possess the highest value of absolute magnetostriction coefficient (–110 ppm). But CFO has the disadvantage of large magnetic anisotropy and high coercivity. Therefore, doping of zinc (Zn) at Co-site of CFO is reported to reduce the magnetic coercivity and increases the resistivity (108Ω) keeping the magnetostriction coefficient with a sizable value. Also, substitution of Zn for Co in CFO reduces magnetic anisotropy. So, in view of this we have prepared Zn modified CFO compound: Co0.9Zn0.1Fe2O4 using sol-gel combustion technique. The room temperature (RT) XRD patterns indicate the formation of single-phase material without appearance of any impurity phases within the detection limit of X-ray diffractometer. The Rietveld refinement on the RT XRD pattern of CZFO sample was carried out using cubic crystal structure with space group Fd-3m. A good agreement between the experimental and the fitted data has been observed. The average crystallite size for the composition was calculated from the XRD patterns using Williamson–Hall method. Scanning electron micrographs displays homogeneous distribution of grains throughout the sample microstructure with the presence of minute amount of pores. The dielectric and electrical properties were studied as function of frequencies at different temperatures. Complex impedance spectroscopic technique study on this sample suggests existence of non-Debye type dielectric relaxation behaviour. [ABSTRACT FROM AUTHOR]