Post-sintering annealing effect on the diffuse phase transition in (Pb1−xBax)(Yb0.5Ta0.5)O3 ceramics

The effect of post sintering annealing on the dielectric response of (Pb_1−xBa_x)(Yb_0.5Ta_0.5)O₃ ceramics in the diffuse phase transition range (x=0.2) has been investigated. The samples are prepared by conventional solid-state reaction method. The samples are sintered at 1300 °C for 2 h and annealed at different temperatures (800, 900 and 1000 °C) for 8 h and at 800 °C for different time durations (8, 12 and 24 h). A significant change in the dielectric response has been observed in all the samples. The dielectric constant increases remarkably and the dielectric loss tangent decreases. The dielectric peaks of the annealed samples are observed to be more diffused with noticeable frequency dispersion compared to the as sintered sample.     

Study of (Bi2O3)(BaxMo1−xO3) polycrystalline ceramic as relaxor ferroelectric

Solid solutions of bismuth layered (Bi₂O₃)(Ba_xMo_1−xO₃) (0.2≤x≤0.8, x is in step of 0.2) ceramics were prepared by conventional solid-state reaction of the constitutive oxides at optimized temperatures with a view to study its electrical properties. Powder X-ray diffraction has been employed for physical characterization and an average grain size of ∼16 to 22 nm was obtained. XRD study reveals the single phase structure of the samples. Dielectric properties such as dielectric constant (ε′), dielectric loss (tanδ) and ac electrical conductivity (σ_ac) of the prepared ceramics sintered at various temperatures in the frequency range 10¹–10⁷ Hz have been studied. A strong dispersion observed in the dielectric properties shows the relaxor type behavior of the ceramic. The presence of maxima in the dielectric permittivity spectra indicates the ferroelectric behavior of the samples. Impedance plots (Cole–Cole plots) at different frequencies and temperatures were used to analyze the electric behavior. The value of grain resistance increases with the increase in Ba ion concentration. The conductivity mechanism shows a frequency dependence, which can be ascribed to the space charge mainly due to the oxygen vacancies. The relaxation observed for the M″ (ω) or Z″ (ω) curves is correlated to both localized and long range conduction. A single ‘master curve’ for the normalized plots of all the modulus isotherms observed for a given composition indicates that the conductivity relaxation is temperature independent.     

Structure and dielectric properties of (Na0.50Bi0.50)1−xBaxTiO3: 0≤x≤0.10

Solid solution of (1−x)Na_0.5Bi_0.5TiO₃-xBaTiO₃ is investigated in the composition range 0.00≤x≤0.10. It is shown that the system exhibits rhombohedral structure up to x=0.055 and then becomes ‘nearly cubic’ for x≥0.06. Temperature dependent dielectric measurements reveals three peaks in the imaginary part of the dielectric constant for compositions exhibiting rhombohedral as well as ‘nearly cubic’ structures. The first of these three peaks exhibits Vogel-Fulcher type relaxation behaviour.     

Na1−xLixNbO3 ceramics studied by X-ray diffraction, dielectric, pyroelectric, piezoelectric and Raman spectroscopy

Na_1−xLi_xNbO₃ ceramics with composition 0.05≤x≤0.30 were prepared by solid-state reaction method and sintered in the temperature range 1100-1150 °C. These ceramics were characterised by X-ray diffraction as well as dielectric permittivity measurements and Raman spectroscopy. Dielectric properties of ceramics belonging to the whole composition domain were investigated in a broad range of temperatures from 300 to 750 K and frequencies from 0.1 to 200 kHz. The Rietveld refinement powder X-ray diffraction analysis showed that these ceramics have a single phase of perovskite structure with orthorhombic symmetry for x≤0.15 and two phases coexistence of rhombohedral and orthorhombic above x=0.20. The evolution of the permittivity as a function of temperature and frequency showed that these ceramics Na_1−xLi_xNbO₃ with composition 0.05≤x≤0.15 present the classical ferroelectric character and the phase transition temperature T_C increases as x content increases. The polarisation state was checked by pyroelectric and piezoelectric measurements. For x=0.05, the piezoelectric coefficient d₃₁ is of 2pC/N. The evolution of the Raman spectra was studied as a function of temperatures and compositions. The results of the Raman spectroscopy study confirm our dielectric measurements, and they indicate clearly the transition from the polar ferroelectric phase to the non-polar paraelectric one.     

Improved multiferroic properties and a novel magnetic behavior of Bi0.8La0.2Fe1−xCoxO3 nanoparticles

Bi_0.8La_0.2Fe_1−xCo_xO₃ nanoparticles of single phase (BLFCO_x, x=0, 0.005, 0.01, 0.02) were prepared by a sol-gel method using polyvinyl alcohol as a surfactant. Co substitution at Fe site improved further dielectric properties of Bi_0.8La_0.2FeO₃ nanoparticles in the frequency range below 25 MHz at room temperature. Magnetization at 10 kOe, coercivities, and remanence of BLFCO_x nanoparticles increased with increasing Co content. It is interesting that the hysteresis loop of all the BLFCO_x nanoparticles presented a wasp-waisted shape. The property can open an important way to design new multiferroic applications of low hysteresis loss in low magnetic fields.     

Structural and magnetic properties of sol-gel Co2xNi0.5−x Zn0.5−xFe2O4 thin films

Nanocrystalline Co_2xNi_0.5−xZn_0.5−xFe₂O₄ (x=0−0.5) thin films have been synthesized with various grain sizes by a sol-gel method on polycrystalline silicon substrates. The morphology as well as magnetic and microwave absorption properties of the films calcined at 1073 K were studied using X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and vibrating sample magnetometry. All films were uniform without microcracks. The Co content in the Co-Ni-Zn films resulted in a grain size ranging from 15 to 32 nm while it ranged from 33 to 49 nm in the corresponding powders. Saturation and remnant magnetization increased with increase in grain size, while coercivity demonstrated a drop due to multidomain behavior of crystallites for a given value of x. Saturation magnetization increased and remnant magnetization had a maximum as a function of grain size independent of x. In turn, coercivity increased with x independent of grain size. Complex permittivity of the Co-Ni-Zn ferrite films was measured in the frequency range 2-15 GHz. The highest hysteretic heating rate in the temperature range 315-355 K was observed in CoFe₂O₄. The maximum absorption band shifted from 13 to 11 GHz as cobalt content increased from x=0.1 to 0.2.     

Microstructure and nanohardness of the diluted magnetic semiconducting Cd1−xMnxS nano-crystalline films

Cd_1−xMn_xS nano-crystalline films (0 ≤ x ≤ 0.5) were formed on glass substrates by thermal evaporation technique at room temperature (300 K). AFM studies showed that all the films were in nano-crystalline form with the grain size varying in the range between 36 and 58 nm and exhibited hexagonal structure of the host material. The lattice parameters varied linearly with composition, following Vegard's law in the entire composition range. The nanohardness and Young's modulus decreased sharply with ‘Mn’ content upto x = 0.3 and increased with high Mn content.     

Conduction mechanism and the dielectric relaxation process of a-Se75Te25−xGax (x=0, 5, 10 and 15 at wt%) chalcogenide glasses

Se₇₅Te_25−xGa_x (x=0, 5, 10 and 15 at wt%) chalcogenide compositions were prepared by the well known melt quenching technique. Thin films with different thicknesses in the range (185–630 nm) of the obtained compositions were deposited by thermal evaporation technique. X-ray diffraction patterns indicate that the amorphous nature of the obtained films. The ac conductivity and the dielectric properties of the studied films have been investigated in the frequency range (10²–10⁵ Hz) and in the temperature range (293–333 K). The ac conductivity was found to obey the power low ω^s where s≤1 independent of film thickness. The temperature dependence of both ac conductivity and the exponent s can be well interpreted by the correlated barrier hopping (CBH) model. The experimental results of the dielectric constant ε₁ and dielectric loss ε₂ are frequency and temperature dependent. The maximum barrier height W_m calculated from the results of the dielectric loss according to the Guintini equation, and agrees with that proposed by the theory of hopping of charge carriers over a potential barrier as suggested by Elliott for chalcogenide glasses. The density of localized state was estimated for the studied film compositions. The variation of the studied properties with Ga content was also investigated. The correlation between the ac conduction and the dielectric properties were verified.     

Enhancing upconversion emissions of NaTm0.02YbxY0.98−xF4 nanocrystals through increasing Yb doping

By increasing the content of Yb³⁺ ions from 20% to 98% in NaTm_0.02Yb_xY_0.98−xF₄ (x=0.2−0.98) nanocrystals with size about 10 nm, the intensities of near infrared (800 nm) and blue (470 nm) upconversion (UC) luminescence can be enhanced by orders of 45 and 49 times, respectively, under 970 nm diode laser excitation. Pump power dependence illustrated that the 800 and 470 nm radiations are still two- and three-photon processes, respectively. TEM imaging showed that the enhancement is not from the change of the crystal size. Steady-state equation and the measured lifetimes indicated that the enhanced 800 nm radiations can induce the enhancement of the 470 nm emissions, which is in good agreement with the experimental data.     

Synthesis and characterization of MnFe2O4-BiFeO3 multiferroic composites

The mixed spinel-perovskite composites of xMnFe₂O₄-(1-x)BiFeO₃ with x=0, 0.1, 0.2, 0.3 and 0.4 were prepared by solid state reaction method. The structure and grain size were examined by means of X-ray diffraction (XRD) and field emission scanning electron microscopy (FESEM), respectively. The XRD results showed that the composites consisted of spinel MnFe₂O₄ and perovskite BiFeO₃ phases after being calcined at the temperature 950 °C for 2 h. The grain size ranged from 0.8 to 1 μm. Magnetization was found to increase with increasing concentration of ferrite content. The variation of dielectric constant and dielectric loss with frequency showed dispersion in the low frequency range. Magnetocapacitance was also observed in the prepared composites, which may be the sign of magnetoelectric coupling in the synthesized composites at room temperature.     

Evolution from relaxor-like dielectric to ferroelectric in Ba[(Fe0.5Nb0.5)1−xTix]O3 solid solutions

Ba[(Fe_0.5Nb_0.5)_1−xTi_x]O₃ (x=0.2,0.4,0.6,0.8,0.85,0.9 and 0.95) solid solutions were synthesized by a standard solid-state reaction technique. X-ray diffraction at room temperature and dielectric characteristics over a broad temperature and frequency range were evaluated systematically. The structure of Ba[(Fe_0.5Nb_0.5)_1−xTi_x]O₃ solid solutions changed from cubic to tetragonal with increasing x. A Debye-like dielectric relaxation following the Arrhenius law similar to that in Ba(Fe_0.5Nb_0.5)O₃ was observed at lower temperature in the composition range 0.2≤x≤0.8, while the relaxor ferroelectric, diffused ferroelectric and normal ferroelectric behavior were observed for x=0.85,0.9 and 0.95, respectively. The process of the evolution of relaxor-like dielectric to ferroelectric suggested the changing from dilute polar micro-domains to polar micro-domains, polar micro/macro-domains and then polar macro-domains in the present ceramics.     

Structural and optical properties of a-Si1−xCx:H films synthesized by dc magnetron sputtering technique

Hydrogenated amorphous SiC films (a-Si_1−xC_x:H) were prepared by dc magnetron sputtering technique on p-type Si(1 0 0) and corning 9075 substrates at low temperature, by using 32 sprigs of silicon carbide (6H-SiC). The deposited a-Si_1−xC_x:H film was realized under a mixture of argon and hydrogen gases. The a-Si_1−xC_x:H films have been investigated by scanning electronic microscopy equipped with an EDS system (SEM-EDS), X-ray diffraction (XRD), secondary ions mass spectrometry (SIMS), Fourier transform infrared spectroscopy (FTIR), UV-vis-IR spectrophotometry, and photoluminescence (PL). XRD results showed that the deposited film was amorphous with a structure as a-Si_0.80C_0.20:H corresponding to 20 at.% carbon. The photoluminescence response of the samples was observed in the visible range at room temperature with two peaks centred at 463 nm (2.68 eV) and 542 nm (2.29 eV). In addition, the dependence of photoluminescence behaviour on film thickness for a certain carbon composition in hydrogenated amorphous SiC films (a-Si_1−xC_x:H) has been investigated.     

Open atmosphere synthesis and wide range colossal magnetoresistance in La0.7Sr0.3−xHgxMnO3 (0≤x≤0.2) system

We have synthesized several polycrystalline samples with nominal compositions La_0.7Sr_0.3−xHg_xMnO_3+δ (0≤x≤0.2) by the standard solid-state reaction method. Instead of the sealed quartz tube method widely employed for the Hg-based systems, we adopted open atmosphere synthesis route. All the samples exhibited monophasic nature with rhombohedral structure as revealed by the X-ray diffraction data. A variation in the unit cell volume is observed with x, which is interpreted as a result of extra oxygen in-diffusion and subsequent cation vacancy creation. A broad metallic behavior is seen in the entire temperature range from 300 to 4 K. The samples showed varying amount of colossal magnetoresistance depending upon the temperature and applied magnetic field. The MR value as high as 30% was observed in x=0.2 sample and the MR is persistent over a wide temperature range with a little change in magnitude.     

Structural and magnetic properties of MnxCo1−xFe2O4 ferrite nanoparticles

We report on the structural and magnetic properties of nanoparticles of Mn_xCo_1−xFe₂O₄ (x=0.1, 0.5) ferrites produced by the glycothermal reaction. From the analysis of XRD spectra and TEM micrographs, particle sizes of the samples have been found to be about 8 nm (for x=0.1) and 13 nm (for x=0.5). The samples were characterized by DC magnetization in the temperature range 5-380 K and in magnetic fields of up to 40 kOe using a SQUID magnetometer. Mössbauer spectroscopy results show that the sample with higher Mn content has enhanced hyperfine fields after thermal annealing at 700 °C. There is a corresponding small reduction in hyperfine fields for the sample with lower Mn content. The variations of saturation magnetization, remnant magnetization and coercive fields as functions of temperature are also presented. Our results show evidence of superparamagnetic behaviour associated with the nanosized particles. Particle sizes appear to be critical in explaining the observed properties.     

Electric quadrupole interaction of Cd in (Ce1−xLax)Ru2 and (Ce1−yCay)Ru2 synthesized at high pressure

Quasibinary Laves systems (Ce_1−xLa_x)Ru₂ and (Ce_1−yCa_y)Ru₂ doped with ¹¹¹In were synthesized at a pressure of 8 GPa, and variations of the electric quadrupole interaction of ¹¹¹Cd at the Ru sites have been studied by the method of time-differential perturbed angular correlation in a wide range of Ce-La and Ce-Ca relative concentrations. In the first case two sites with quadrupole frequencies ν_Q≅220 and 150 MHz persist at x≤0.2, while at x≥0.3 only the higher frequency component remains in the spectra, which are similar to that of pure LaRu₂. In the series (Ce_1−yCa_y)Ru₂, at y≥0.03 the lower frequency component was washed out except in samples with y=0.1 and 0.2, where it was restored.     

Complex permittivity, permeability and microwave absorbing properties of (Mn2−xZnx)U-type hexaferrite

Complex permittivity, permeability and microwave absorbing properties of a U-type hexaferrite series Ba₄Mn_(2−x)Zn_xFe₃₆O₆₀ (with 0≤x≤2 in step of 0.5) have been examined in the X-band (8.2-12.4 GHz) frequency range. The series have been prepared using conventional solid state reaction route. Microstructural variations with composition have been found with X-ray diffraction (XRD) and scanning electron microgram (SEM). The complex permittivity (ε^?=ε′−jε″) and permeability (μ^?=μ′−jμ″) were measured using vector network analyzer (Agilient Make model PNA E8364B). These parameters were then used for calculating the reflection loss for determination of microwave absorbing properties. Addition of Zn resulted in an increase in reflection loss from −4 dB (or 60 % absorption) in sample with x= 0 to −32 dB (99.92% absorption) in sample with x=1 when the sample thickness was 1.7 mm. Multiple peaks of resonance were obtained in the dielectric and magnetic loss spectra for all samples with x>0. The result indicates that the sample with composition Ba₄MnZnFe₃₆O₆₀, i.e., x=1, can be used effectively for microwave absorption and suppression of electromagnetic interference.     

Low-voltage cathodoluminescence property of Li-doped Gd2−xYxO3:Eu

Cathodoluminescent (CL) spectra of Li-doped Gd_2−xY_xO₃:Eu³⁺ solid-solution (0.0?x?0.8) were investigated at low voltages (300 V-1 kV). The CL intensity is maximum for the composition of x=0.2 and gradually reduces with increasing the amount of substituted Y content. In particular, small (∼100 nm) particles of Li-doped Gd_1.8Y_0.2O₃:Eu³⁺ are obtained by firing the citrate precursors at only 650°C for 18 h. Relative red-emission intensity at 300 V of this phosphor is close to 180% in comparison with that of commercial red phosphor Y₂O₃:Eu³⁺. An increase of firing temperature to 900°C results in 400-600 nm sized spherical particles. At low voltages (300-800 V), the CL emission of 100 nm sized particles is much stronger than that of 400-600 nm sized ones. In contrast, the larger particles exhibit the higher CL emission intensity at high voltages (1-10 kV). Taking into consideration small spherical morphology and effective CL emission, Li-doped Gd_1.8Y_0.2O₃:Eu³⁺ appears to be an efficient phosphor material for low voltage field emission display.     

Optical characterization of InxGa1−xN alloys

InGaN layers were grown by molecular beam epitaxy (MBE) either directly on (0 0 0 1) sapphire substrates or on GaN-template layers deposited by metal-organic vapor-phase epitaxy (MOVPE). We combined spectroscopic ellipsometry (SE), Raman spectroscopy (RS), photoluminescence (PL) and atomic force microscopy (AFM) measurements to investigate optical properties, microstructure, vibrational and mechanical properties of the InGaN/GaN/sapphire layers.The analysis of SE data was done using a parametric dielectric function model, established by in situ and ex situ measurements. A dielectric function database, optical band gap, the microstructure and the alloy composition of the layers were derived. The variation of the InGaN band gap with the In content (x) in the 0 < x ≤ 0.14 range was found to follow the linear law E_g = 3.44-4.5x.The purity and the stability of the GaN and InGaN crystalline phase were investigated by RS.     

Ordered fluorite phases in the Bi2O3-Ta2O5 system: A structural and electrical investigation

Structure and electrical behaviour are reported for the system Bi_1-xTa_xO_1.5 + x (0.167 ≤ x ≤ 0.250). In the compositional range 0.200 < x ≤ 0.250 an incommensurately modulated pseudo-cubic phase (type II) is observed, with the appearance of a larger pseudo-cubic phase in the region 0.167 ≤ x ≤ 0.200. Structural analysis of the type II phases by neutron diffraction reveals subtle changes in the oxide ion distribution with temperature, associated with changes in the incommensurate modulation parameter. Analysis of the defect structure of the type II phase reveals chains of tantalate octahedra as a likely structural motif. It is proposed that these chains facilitate an electronic contribution to total conductivity at low temperatures through electron hopping along the chains. Changes in oxide ion vacancy ordering may explain the observed non-linear behaviour in the thermal expansion of lattice parameter and Arrhenius plots of total conductivity.     

Influence of substitution on dielectric and impedance spectroscopy of Sr1 − xBi2 + yNb2O9 ferroelectric ceramics synthesized by chemical route

Nanocrystalline powders of Sr_1 − xBi_2 + yNb₂O₉ (SBN, x = 0.0, 0.1, 0.2, 0.3, and 0.4; y = 0, 0.066, 0.133, 0.200, and 0.266) were prepared by aqueous solution method using water-soluble Sr-EDTA, Bi-EDTA and Nb-tartarate as the starting materials. XRD showed that the samples were free from fluorite or pyrochlore phase within heat-treatment temperature from 550 to 600 °C. Average crystallite size and particle diameter were observed to be between 10 and 25 nm, which were analyzed through XRD and TEM, respectively. Bi-substitution has substantially improved the sinterability of SBN and enabled to achieve high density (96%), which was otherwise difficult in the case of pure SBN. The dielectric properties of SBN ceramics were significantly enhanced by the partial replacement of Sr²⁺ ions by the trivalent bismuth ions. The complex impedance diagrams of Bi-substituted SBN, x = 0.4 ceramics exhibited only one semicircle indicating a significant contribution from the grains. In contrast, the impedance plots for pure and other substituted SBN ceramics show an additional low-frequency semicircle, which was attributed to the blocker size effects. The dielectric behavior of pure and Bi-substituted SBN ceramics was rationalized using the impedance and modulus data.