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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]

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]

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]

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]

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]

Multiferroic composites with enhanced magneto-electric coefficient are suitable candidates for various multifunctional devices. Here, we chose a particulate composite, which is the combination of multiferroic (PbFe0.5Nb0.5O3, PFN) as matrix and magnetostrictive (Co0.6Zn0.4Fe1.7Mn0.3O4, CZFMO) material as the dispersive phase. The X-ray diffraction analysis confirmed the formation of the composite having both perovskite PFN and magnetostrictive CZFMO phases. The scanning electron micrograph (SEM) showed dispersion of the CZFMO phase in the matrix of the PFN phase. The temperature-dependent magnetization curves suggested the transition arising due to PFN and CZFMO phase. The temperature-dependent dielectric study revealed a second-order ferroelectric to the paraelectric phase transition of the PFN phase in the composite with a small change in the transition temperature as compared to pure PFN. The magnetocapacitance (MC%) and magnetoimpedance (MI%) values (obtained from the magneto-dielectric study at room temperature (RT)) at 10 kHz were found to be 0.18% and 0.17% respectively. The intrinsic magneto-electric coupling value for this composite was calculated to be 0.14 mVcm-1Oe-1, which is comparable to other typical multiferroic composites in bulk form. The composite PFN-CZFMO exhibited a converse magneto-electric effect with a change in remanent magnetization value of -58.34% after electrical poling of the material. The obtained outcomes from the present study may be utilized in the understanding and development of new technologies of this composite for spintronics applications. [ABSTRACT FROM AUTHOR]

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. Magnetoimpedance spectroscopy reveals a significant change (∼18%) in dielectric permittivity at H=2T for x=0.2. [ABSTRACT FROM AUTHOR]

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 ([variant_greek_epsilon](H)-[variant_greek_epsilon](0))/[variant_greek_epsilon](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. [ABSTRACT FROM AUTHOR]

A series of lead-free perovskite solid solutions of (1 − x) Na0.5 Bi0.5 TiO3( NBT)- x BaSnO3( BSN), for 0.0 ≤ x ≤ 0.15 have been synthesized using a high-temperature solid-state reaction route. The phase transition behaviors are studied using dielectric and Raman spectroscopic techniques. The ferroelectric to relaxor phase transition temperature ( TFR) and the temperature corresponding to maximum dielectric permittivity ( Tm) are estimated from the temperature-dependent dielectric data. Dielectric studies show diffuse phase transition around ~335°C in pure NBT and this transition temperature decreases with increase in x. The disappearance of x-dependence of A1 mode frequency at ~134 cm−1 for x ≥ 0.1 is consistent with rhombohedral-orthorhombic transition. In situ temperature dependence Raman spectroscopic studies show disappearance and discontinuous changes in the phonon mode frequencies across rhombohedral ( x < 0.1)/orthorhombic ( x ≥ 0.1) to tetragonal transition. [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]

Abstract: Structural, microstructural and electrical properties of lanthanum-modified sodium bismuth titanate (Na0.5Bi0.5TiO3) (NBT) ceramics were investigated. X-ray diffraction (XRD) analysis of the prepared materials confirmed the formation of the compounds with rhombohedral crystal system. The nature of scanning electron micrographs of the compounds showed (i) the uniform distribution of grains on the sample surface with high density and (ii) reduction of grain size on La substitution at the (Na of NBT. Detailed studies of dielectric and impedance properties of the materials, carried out in the frequency range of 102–106 Hz at different temperatures (room temperature to 500°C), have provided many interesting properties. The dielectric constant at transition temperature was found to be decreased with increase of broadening of the dielectric peak on increasing La content in the sample. The transition temperature (T m) shifted to higher temperature side on addition of La (up to 6%), whereas the reverse trend was observed for higher concentration of La (i.e. 8%). The depolarization temperature (T d) of La-modified NBT compounds was found to be smaller than that of pure NBT. The tangent loss was also found to be decreased on the incorporation of La into NBT. The ac conductivity of the La-modified NBT obeyed the double power law behavior. Complex impedance spectroscopy has been carried out for better understanding of relaxation process and correlations between the microstructure–electrical properties of the materials. [Copyright &y& Elsevier]

Highlights • Acrylamide polymer gel template method has been used to prepare single phase DyMnO 3. • Heat capacity measurement shows three transitions due to T N (Dy), T lock and T N (Mn). • Magnetic field strongly affect T N (Dy) and T lock as observed in heat capacity data. • The magnetic study reveals the presence of two transitions due to T N (Dy) and T lock. • Increase in weak ferromagnetic behaviour with decrease in temperature. Abstract Single phase polycrystalline DyMnO 3 (DMO) was synthesized using acrylamide polymer gel template method. We report the structural, magnetic, specific heat and dielectric properties of DMO over wide experimental conditions. Room temperature XRD pattern shows the formation of singe phase material without any impurity. The magnetic properties such as magnetization versus temperature (M vs. T) and magnetization versus magnetic field (M vs. H) were studied around the transition temperatures region. The temperature dependent magnetization data suggest two phase transitions corresponding to the lock-in temperature below which ferroelectric ordering exist (around 19 K; T lock) and antiferromagnetic (AFM) ordering of Dy spin (around 8 K; T N (Dy)). The magnetic hysteresis obtained were fitted to extract weak ferromagnetic (FM) and antiferromagnetic/paramagnetic (AFM/PM) contribution to the magnetic data. The order of magnetic transitions were analyzed from Arrott plot. The temperature dependent specific heat measurement shows all three phase transitions corresponding to (i) AFM ordering of Mn spin (around 38 K; T N (Mn)), (ii) T lock transition and (iii) T N (Dy) transition. The effect of magnetic field to the transitions were studied using specific heat capacity measurement. The peak intensity of T N (Dy) decreases on the application of magnetic field whereas peak intensity of T lock increases with increase in magnetic field in specific heat measurement. Further the third anomaly, T N (Mn) remains more or less unaffected by the application of magnetic field. The intrinsic dielectric behaviour of the material was observed up to 160 K, above this temperature there is large increase in dielectric value due to the contribution from Maxwell- Wagner polarization. [ABSTRACT FROM AUTHOR]