Enhanced ferroelectric property of (Pb0.95Ca0.05)(Nb0.02Zr0.80Ti0.20)O3 thin films prepared by RF magnetron sputtering

(Pb_0.95Ca_0.05)(Nb_0.02Zr_0.80Ti_0.20)O₃ [PCNZT] thin films were deposited on the Pt(1 1 1)/Ti/SiO₂/Si(1 0 0) substrates by RF magnetron sputtering with and without a LaNiO₃ [LNO] buffer layer. Ca and Nb elements in PZT films enhance the ferroelectric property, LaNiO₃ buffer layer improves the crystal quality of the PCNZT thin films. PCNZT thin films possess better ferroelectric property than that of PZT films for Ca and Nb ion substitution, moreover, PCNZT thin films with a LNO buffer layer possess (1 0 0) orientation and good ferroelectric properties with high remnant polarization (P_r = 38.1 μC/cm²), and low coercive field (E_c = 65 kV/cm), which is also better than that of PCNZT thin films without a LNO buffer layer (P_r = 27.9 μC/cm², E_c = 74 kV/cm). The result shows that enhanced ferroelectric property of PZT films can be obtained by ion substitution and buffer layer.     

Enhanced ferroelectric properties of (Pb0.90La0.10)Ti0.975O3 multilayered thin films prepared by RF magnetron sputtering

The (Pb_0.90La_0.10)Ti_0.975O₃/PbTiO₃ (PLT/PT), PbTiO₃/(Pb_0.90La_0.10)Ti_0.975O₃/PbTiO₃ (PT/PLT/PT) multilayered thin films with a PbO_x buffer layer were in situ deposited by RF magnetron sputtering at the substrate temperature of 600 °C. With this method, highly (1 0 0)-oriented PLT/PT and PT/PLT/PT multilayered thin films were obtained. The PbO_x buffer layer leads to the (1 0 0) orientation of the films. The dielectric, ferroelectric and pyroelectric properties of the PLT multilayered thin films were investigated. It is found that highly (1 0 0)-oriented PT/PLT/PT multilayered thin films possess higher remnant polarization 2P_r (44.1 μC/cm²) and better pyroelectric coefficient at room temperature p (p = 2.425 × 10⁻⁸ C/cm² K) than these of PLT and PLT/PT thin films. These results indicate that the design of the PT/PLT/PT multilayered thin films with a PbO_x buffer layer should be an effective way to enhance the dielectric, ferroelectric and pyroelectric properties. The mechanism of the enhanced ferroelectric properties was also discussed.     

Dielectric properties of SrBi2−xPrxNb2O9 ceramics (x=0, 0.04 and 0.2)

SrBi_2−xPr_xNb₂O₉ (x=0, 0.04 and 0.2) ceramics were prepared by a solid state reaction method. X-ray diffraction analysis indicated that single-phase layered perovskite structure ferroelectrics were obtained. A relaxor behavior of frequency dispersion was observed among Pr-doped SrBi₂Nb₂O₉. The degree of frequency dispersion ΔT increased from 0 for x=0-7 °C for x=0.2, and the extent of relaxor behavior γ increased from 0.94 for x=0-1.45 for x=0.2. The substitution of Pr ions for Bi³⁺ ions in the Bi₂O₂ layers resulted in a shift of the Curie point to lower temperatures and a decrease in remanent polarization. In addition, the coercive field 2E_c reduced from 110 kV/cm for an undoped specimen to 90 kV/cm for x=0.2.     

Influence of mobile space charges on electrical properties of ferroelectric Bi3.5La0.5Ti3O12 thin films

Lanthanum-substituted bismuth titanate, Bi_3.5La_0.5Ti₃O₁₂ (i.e., x=0.5 in Bi_4−xLa_xTi₃O₁₂), thin films have been grown on Pt/Ti/SiO₂/Si substrates using pulsed laser deposition. The frequency dependence of the real part ε′(ω) and the imaginary part ε″(ω) of the dielectric constant has been studied. The ε′(ω) does not show any sudden change within the frequency range of 10²-10⁶ Hz. In contrast, the ε″(ω) shows a large dispersion as frequency decreases. The observed relaxation behavior in ε″(ω) can be explained in terms of a migration of oxygen vacancies in (Bi₂O₂)²⁺ layers, not in Bi₂Ti₃O₁₀ perovskite layers.     

Effects of substrates on the structure and dielectric properties of Ba(Sn0.15Ti0.85)O3 thin films

Ba(Sn_0.15Ti_0.85)O₃ (BTS) thin films were grown on Pt(1 1 1)/Ti/SiO₂/Si and LaNiO₃(LNO)/Pt(1 1 1)/Ti/SiO₂/Si substrates by a sol-gel processing technique, respectively. The BTS thin films deposited on annealed Pt(1 1 1)/Ti/SiO₂/Si and annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrates exhibited strong (1 1 1) and perfect (1 0 0) orientations, respectively. The BTS thin films grown on un-annealed Pt(1 1 1)/Ti/SiO₂/Si substrates showed random orientation with intense (1 1 0) peak, while the films deposited on un-annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrate exhibited random orientation with intense (1 0 0) peak, respectively. The dielectric constant of the BTS films deposited on annealed Pt(1 1 1)/Ti/SiO₂/Si, annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si, un-annealed Pt(1 1 1)/Ti/SiO₂/Si and un-annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrates was 512, 565, 386 and 437, respectively, measured at a frequency of 100 kHz. A high tunability of 49.7% was obtained for the films deposited on annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrate, measured at the frequency of 100 kHz with an applied electric field of 200 kV/cm. The high tunability has been attributed to the (1 0 0) texture of the films and larger grain sizes.     

Enhanced spontaneous polarization in Sr and Ca co-doped BaTiO3 ceramics

The dielectric and ferroelectric properties of (Ba_xSr_1−x)_0.77Ca_0.23TiO₃ ceramics with x=1 to 0.7 were studied and compared with those of Ba_xSr_1−xTiO₃ and Ba_0.77Ca_0.23TiO₃ ceramics. It has been found that Sr doping of the Ba_0.77Ca_0.23TiO₃ ceramics causes a drastic decrease of the Curie temperature, just like Sr doping of pure BaTiO₃ ceramics, demonstrating a cell volume effect. However, the (Ba_xSr_1−x)_0.77Ca_0.23TiO₃ ceramics with x=0.9 and 0.8 have larger spontaneous polarization than those of the corresponding Ba_xSr_1−xTiO₃ and Ba_0.77Ca_0.23TiO₃ ceramics, along with sufficient insulating properties. The enhancement of their polarization was explained by the increase of the lattice parameter c/a ratio due to the lattice distortion and strain developed in the ceramics.     

Relaxor behavior of (Ba,Sr)(Zr,Ti)O3 ferroelectric ceramics

We examine the ferroelectric-relaxor behavior of (Ba_0.65Sr_0.35)(Zr_0.35Ti_0.65)O₃ (BSZT) ceramics in the temperature range from 80 to 380 K. A broad dielectric maximum, which shifts to higher temperature with increasing frequency, signifies the relaxor-type behavior of these ceramics. The value of the relaxation parameter γ∼2 estimated from the linear fit of the modified Curie-Weiss law, indicates the relaxor nature of the BSZT ceramics. The dielectric relaxation rate follows the Vogel-Fulcher relation with T_VF=107 K, E_a=0.121 eV, and ν₀=6.83×10¹⁴ Hz, further supports such relaxor nature. The slim P-E hysteresis loop and ‘butterfly’ shape dc bias field dependence of permittivity at T>T_m (T_m, the temperature of permittivity maximum) clearly signifies the occurrence of nanopolar clusters, which is the typical characteristic of ferroelectric relaxor. At 300 K and 10 kHz, the dielectric constant and loss tan δ are ∼1100 and 0.0015, respectively. The high tunability (∼25%) and figure of merit (∼130) at room temperature show that the BSZT ceramics could be a promising candidate for tunable capacitor applications.     

Radio-frequency (RF) studies of the magneto-dielectric composites: Cr0.75Fe1.25O3 (CRFO)-Fe0.5Cu0.75Ti0.75O3 (FCTO)

This paper concerns a study about the electrical properties of Cr_0.75Fe_1.25O₃ (CRFO)/Fe_0.5Cu_0.75Ti_0.75O₃ (FCTO) magneto-dielectric composites. These compounds were prepared by the conventional solid-state reaction synthesis. The samples synthesized, as well their two-phase composites [Cr_0.75Fe_1.25O₃]_Z-[Fe_0.5Cu_0.75Ti_0.75O₃]_100−Z (Z=17, 34, 50, 66, 83), were characterized by X-ray powder diffraction technique (XRD). Rietveld's method was employed to verify the quantitative phase abundances in the composites’ and their theoretical densities, which were compared with the experimental densities (pycnometer method).To predict the effect of the phases in the composites effective dielectric function (κ), traditional dielectric mixing models such as parallel, series, and Lichtenecker's model were observed. An alternative approach, a sigmoidal fitting function based on the Boltzmann equation, was proposed to fit the experimental data.     

Ferroelectric properties of Pr and Nb co-substituted Sr0.8Bi2.2Ta2O9 thin films

Thin film of both A- and B-site co-substituted Sr_0.8Bi_2.2Ta₂O₉ (SBT) by Pr³⁺ and Nb⁵⁺, i.e. Sr_0.8Pr_0.1Bi_2.1Ta_1.5Nb_0.5O₉ (SPBTN) was fabricated on Pt/Ti/SiO₂/Si substrates by metalorganic decomposition method. The Nb⁵⁺ substitution at B-site and Pr³⁺ substitution at A-site enhanced the remanent polarization and reduced the coercive field of the films, respectively. The remanent polarization (2P_r) value of the SPBTN film was 22 μC/cm². The coercive field (2E_c) value of the SPBTN film was 102 kV/cm, which was much lower than that of SBTN (165 kV/cm). The effects of substitution on structural and ferroelectric properties of SBT were discussed in detail. As a result, the A- and B-sites co-substitution may be one of the promising ways to improve ferroelectric properties of SBT.     

Dielectric and optical behaviors in relaxor ferroelectric Pb(In1/2Nb1/2)1−xTixO3 crystal

Dielectric permittivities (ε′,ε″) have been measured as functions of temperature (140-535 K) and frequency (500 Hz-2.0 MHz) in a (001)-cut Pb(In_1/2Nb_1/2)_0.7Ti_0.3O₃ (PINT30%) single crystal grown by the modified Bridgman method with Pb(Mg_1/3Nb_2/3)_0.71Ti_0.29O₃ (PMNT29%) seed crystal. A diffused phase transition was observed in the temperature region of ∼430-460 K with strong frequency dispersion. Above the Burns temperature T_B≅510 K, the dielectric permittivity was found to follow the Curie-Weiss behavior, ε′=C/(T−T_C), with parameters C=3.9×10⁵ and T_C=472 K. Below T_B≅510 K, polar nanoclusters are considered to appear and are responsible for the diffused dielectric anomaly. Optical transmission, refractive indices, and the Cauchy equations were obtained as a function of wavelength at room temperature. The unpoled crystal shows almost no birefringence, indicating that the average structural symmetry is optically isotropic. The crystal exhibits a broad transparency in the wavelength range of ∼0.4-6.0 μm.     

Electrical properties of pulsed laser-deposited SrxBiyTa2O9 thin films on Bi/Sr ratios

The dependence of the electrical properties of Sr_xBi_yTa₂O₉ thin films on the (Bi/Sr ratio 1.6, 2.3, 2.8, 3.4) has been investigated. The Sr_xBi_yTa₂O₉ ferroelectric thin films were synthesized on Pt/Ti/SiO₂/Si substrates using the pulsed laser deposition method. Saturation polarization (P_st) and coercive field (2E_c) depend on the Bi/Sr ratio. P_st increases while E_c decreases with an increase in Bi/Sr ratio. Atomic Force Microscopy images show that the grain size grows with increasing Bi/Sr ratio. It is observed that the impedance behavior in Sr_xBi_yTa₂O₉ thin film, conforms to the Constant Phase Element (CPE) model. It is believed that the diffuse charges at the grain boundary build up a surface polarization because the impedance behavior close to pure capacitor with grain size increased.     

Maxwell-Wagner characterization of dielectric relaxation in Ni0.8Zn0.2Fe2O4/Sr0.5Ba0.5Nb2O6 composite

Dense composites were prepared through incorporating the dispersed Ni_0.8Zn_0.2Fe₂O₄ ferromagnetic particles into Sr_0.5Ba_0.5Nb₂O₆ ferroelectric matrix. Extrinsic dielectric relaxation and associated high permittivities of the materials are reported in the composites. We used an ideal equivalent circuit to explain electrical responses in impedance formalism. A Debye-like relaxation in the permittivity formalism was also found. Interestingly, real permittivity (ε′) of the sample containing 30% Ni_0.8Zn_0.2Fe₂O₄ shows obvious independence of the temperature at 100 kHz. Dielectric relaxation and high-ε′ properties of the composites are explained in terms of the Maxwell-Wagner (MW) polarization model.     

Investigations of structural, dielectric and ferroelectric behavior of europium substituted SrBi2Ta2O9 ferroelectric ceramics

Europium substituted samples of the compositions Sr_1−xEu_xBi₂Ta₂O₉ (x=0.0,0.025,0.050,0.10 and 0.20) were synthesized by solid state reaction method and studied for their structural, dielectric and ferroelectric properties. The X-ray diffractograms confirmed the formation of single phase layered perovskite structure in all the samples. The temperature variation of dielectric constant shows that the Curie temperature (T_c) decreases on increasing concentration of europium. The dielectric loss reduces significantly with europium addition. The P-E studies of the Eu-substituted SBT ceramics show that the remanent polarization increases with increasing concentration of europium.     

The effect of potential of impedance in the pulsed-laser-deposited SrBi2Ta2O9 thin film

Ferroelectrics SrBi₂Ta₂O₉ (SBTO) thin films were grown on a highly oriented Pt/Ti/SiO₂/Si substrates using the pulsed laser ablation. The ac impedance of SBTO thin films have been measured at room temperature both in the frequency range from 10⁻¹ to 10⁶ Hz and bias voltage range from −6 to 6 V. The ac impedance dispersion was observed at low frequency with increasing bias voltage, which was interpreted based on a blocked charge. We can explain that the blocking interface gives rise to constant phase element (CPE) response, and we give an impedance model function that can fit data along the low frequency range when such a CPE is found. The low frequency dispersion phenomena of SBTO thin film are related to a charge diffusion process at the surface of thin film.     

TiO2-nonstoichiometry dependence on piezoelectric properties and depolarization temperature of (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ceramics

(Bi_0.5Na_0.5)_0.94Ba_0.06Ti_xO_1+2x lead-free piezoceramics with x varying from 0.97 to 1.03 were fabricated and characterized in order to investigate the effects of TiO₂-nonstoichiometry on the piezoelectric properties and depolarization temperature of (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ composition. X-ray diffraction (XRD) analysis showed that all samples have a single phase of perovskite structure with rhombohedral symmetry. Piezoelectric and dielectric measurements revealed that deficiency of TiO₂ leads to an increase in the piezoelectric coefficient (d₃₃), free relative permittivity (), and loss tangent (tan δ) besides an increase in the electromechanical coupling coefficient (k_p) within a certain amount, while excess of TiO₂ results in a decrease in k_p, d₃₃, and , but an increase in tan δ. Depolarization temperature (T_d) measurement indicated a decrease and an increase in T_d as a result of increasing TiO₂ deficiency and TiO₂ excess, respectively. This TiO₂-nonstoichiometry also induced changes in the remanent polarization (P_r) and coercive field (E_c) of the ceramics.     

Controllable microstructures and multiferroic properties of Pb(Zr0.53Ti0.47)O3-CoFe2O4 composite films

1-3 and 2-2 types Pb(Zr_0.53Ti_0.47)O₃-CoFe₂O₄ (PZT-CFO) composite films with controllable microstructures, consisted by CFO nanopillar embedded in PZT matrix and PZT-CFO gratings respectively, have been fabricated on Pt/Ti/SiO₂/Si substrates by combining lithography technology and pulsed laser deposition. X-ray diffraction confirms that the films are well crystallized under optimized postannealing conditions. Scanning electron microscope reveals that the periodic microstructures can be well controlled. Especially, intrinsic room temperature ferroelectric and ferrimagnetic behaviors are observed simultaneously. The structure-properties relationship is discussed. Our results may provide an alternative method to design and prepare multiferroic composite films with controllable microstructures.     

Relaxor behavior of (Sr,Ba,Bi)TiO3 ferroelectric ceramic

The dielectric behavior of (Sr_0.4Ba_0.6)_0.925Bi_0.05TiO₃ (SBBT) ceramic was investigated in the temperature range from 100 K to 450 K. Broad dielectric maxima, which shift to higher temperature with increasing frequency, and the value of the relaxation parameter γ=1.6-2 estimated from the linear fit of the modified Curie-Weiss law, indicated the relaxor nature of the SBBT ceramic. The dielectric relaxation which follows the Vogel-Fulcher relationship with  K, E_a=0.0392 eV, and ν_o=2.98×10¹¹ Hz, further supports such a relaxor nature. The P-E hysteresis loop at different temperatures and ‘butterfly’ shape dc bias field dependence of permittivity at T>T_m (the temperature of permittivity maximum) signifies the occurrence of nanopolar clusters, which is the typical characteristic of relaxor ferroelectrics. At 300 K and 10 kHz, the dielectric constant and loss tgδ are ∼2210 and 0.00118, respectively. The tunability (28%) and figure of merit (237) at room temperature show that the SBBT ceramic could be a promising candidate for tunable capacitor applications.     

First-principles study of structural, optical and elastic properties of cubic HfO2

The structural, optical and elastic properties of cubic HfO₂ were studied using the plane-wave ultrasoft pseudopotential technique based on the first-principles density-functional theory (DFT). The ground-state properties such as lattice parameter and bulk modulus were calculated and these results are in favorable agreement with the previous work. The complex dielectric function, refractive index, extinction coefficient, complex conductivity function, energy-loss spectrum, absorption coefficient and optical reflectivity are calculated and the peak position distributions of imaginary parts of the complex dielectric function have been explained. The calculated elastic properties are consistent with other calculated results.     

Physical properties of double perovskite compounds ALaVMoO6 (A=Ca, Sr, Ba)—a possible half-metallic antiferromagnetic system

Double perovskite compounds ALaVMoO₆ (A=Ca, Sr, Ba) have been synthesized and their electrical and magnetic properties have been investigated. Magnetization measurements have indicated the possible antiferromagnetic transitions at 120 and 130 K for A=Ca and Sr samples, respectively. Electrical resistivity ρ for this system shows metallic temperature dependence from 300 to 20 K, though the sample with A=Ca shows weak semiconducting behavior in the low temperature region (<70 K). Considering the magnetic and electrical properties and assuming the V³⁺S=1 and Mo⁴⁺S=1 valence and spin states, the samples with A=Ca and Sr can be promising candidates for half-metallic antiferromagnets.     

Effects of composition on phase structure and electrical properties of (K0.5Na0.5)0.90Li0.06Sr0.02Nb(1−x)SbxO3 ceramics

Lead-free (K_0.5Na_0.5)_0.90Li_0.06Sr_0.02Nb_(1−x)Sb_xO₃ (KNLSN-Sb_x) ceramics were synthesized by ordinary sintering technique. The compositional dependence of phase structure and electrical properties of the ceramics was systematically investigated. All samples possessed pure perovskite structure, showing room temperature symmetries of orthorhombic at x<0.01, coexistence of orthorhombic and tetragonal phases at x=0.01, and tetragonal at 0.02≤x≤0.05. The temperature of the polymorphic phase transition (PPT) was shifted to lower temperature and dielectric relaxor behavior was induced by increasing Sb content. The samples near the coexistence region (x=0.01) exhibited enhanced electrical properties: d₃₃∼145 pC/N, k_p∼38% and P_r∼20.4 μC/cm².