Chemical synthesis and characterization of hydrous tin oxide (SnO<Subscript><Emphasis Type="Bold">2</Emphasis></Subscript>:H<Subscript><Emphasis Type="Bold">2</Emphasis></Subscript>O) thin films

In the present investigation, we report chemical synthesis of hydrous tin oxide (SnO ₂ :H ₂ O) thin films by successive ionic layer adsorption and reaction (SILAR) method at room temperature ( \thicksim \thicksim 300 K). The films are characterized for their structural and surface morphological properties. The formation of nanocrystalline SnO ₂ with porous and agglomerated particle morphology is revealed from X-ray diffraction (XRD) and scanning electron microscopy (SEM) studies, respectively. The Fourier transform infrared spectroscopy (FTIR) study confirmed the formation of Sn–O phase and hydrous nature of the deposited film. Static water contact angle studies showed the hydrophilic nature of SnO ₂ :H ₂ O thin film. Electrical resistivity showed the semiconducting behaviour with room temperature electrical resistivity of 10 ⁵  W\boldsymbol\Omega cm. The electrochemical properties studied in 0·5 M Na ₂ SO ₄ electrolyte showed a specific capacitance of 25 F g ^− 1 at 5 mVs ^− 1 scan rate.     

Phase developments and dielectric responses of barium substituted four-layer CaBi<Subscript>4</Subscript>Ti<Subscript>4</Subscript>O<Subscript>15</Subscript> Aurivillius

In this paper, mixed Ca–Ba oxide Ca_1 − x Ba _x Bi₄Ti₄O₁₅ (CBBT) ceramics, fabricated by the improved traditional ceramics process were investigated by doping concentrations of Ba ion up to x =\emph{x} {=} 0·9 (in steps of 0·1). At room temperature, an orthorhombic crystal system was confirmed using XRD, and their parameter was obtained using the Rietveld method. Dielectric properties and phase transitions were studied and are explained in terms of lattice response of these ceramics. A shift in ferroelectric–paraelectric phase transition (T_C\emph{T}_{C}) to lower temperatures and a corresponding decrease in permittivity peak with increasing concentration of Ba^2 + are also observed. The ferroelectric–paraelectric phase transition of CBBT compounds is of normal type in nature, differing from the relaxor characteristic of BBT. The decrease of orthorhombicity in the lattice structure by the larger Ba^2 + ion incorporation, indicating an approach of a and b, results in lower Curie temperature. Appearance of anomalous loss peaks of Ba-rich compounds at 530°C reveals a phase transition development trend from ferroelectric orthorhombic structure to the paraelectric orthorhombic structure. Relationship of polarization with lattice response is discussed.     

Synthesis and characterization of polythiophene-modified TiO<Subscript>2</Subscript> nanotube arrays

The highly ordered and uniform TiO₂ nanotube arrays were fabricated by anodic oxidation method and PTh(polythiophene)/TiO₂ nanotube arrays electrode were obtained by electrochemical polymerization. X-ray powder diffraction (XRD) analysis confirmed the formation of TiO₂ phase. The morphologies and optical characteristics of the TiO₂ nanotube arrays were studied by scanning electron microscope (SEM), UV-Vis absorption spectra and Raman spectra. The results demonstrate that the PTh/TiO₂ electrode could enlarge the visible light absorption region and increase the photocurrent in visible region. The modified TiO₂ electrode with light-to-electric energy conversion efficiency of 1·46%, the short-circuit current density of 4·52 mAcm^− 2, open-circuit voltage of 0·74 V and fill factor of 0·44, were obtained.     

Low-firing Li<Subscript>2</Subscript>ZnTi<Subscript>3</Subscript>O<Subscript>8</Subscript> microwave dielectric ceramics with BaCu(B<Subscript>2</Subscript>O<Subscript>5</Subscript>) additive

Phase purity, microstructure, sinterability and microwave dielectric properties of BaCu(B₂O₅)-added Li₂ZnTi₃O₈ ceramics and their cofireability with Ag electrode were investigated. A small amount of BaCu (B₂O₅) can effectively reduce the sintering temperature from 1075°C to 925°C, and it does not induce much degradation of the microwave dielectric properties. Microwave dielectric properties of ε _r = 23·1, Q × f = 22,732 GHz and τ _f = − 17·6 ppm/°C were obtained for Li₂ZnTi₃O₈ ceramic with 1·5 wt% BaCu(B₂O₅) sintered at 925°C for 4 h. The Li₂ZnTi₃O₈ +BCB ceramics can be compatible with Ag electrode, which makes it a promising microwave dielectric material for low-temperature co-fired ceramic technology application.     

Effect of low level substitution of Sr–Ba on transport and magnetic behaviour of La<Subscript>0·67</Subscript>Ca<Subscript>0·33</Subscript>MnO<Subscript>3</Subscript>

In this paper we report the investigation of transition metal oxide compound, La_0·67Ca_0·25Sr_0·04Ba_0·04MnO₃ (LCSBMO), along with La_0·67Ca_0·33MnO₃ (LCMO), synthesized by sol–gel route under identical conditions. The effect of simultaneous low level substitution of large size ions such as Sr²⁺ and Ba^2 + for Ca^2 + ions on the electronic transport and magnetic susceptibility properties are analysed and compared apart from microstructure and lattice parameters. The temperature dependent electrical transport of the polycrystalline pellets of LCSBMO and LCMO when obeying the well studied law, r = r₀ + r₂   T²\rho = \rho_{0} + \rho_{2} \;T^{2} for T < T _MI , is observed to differ by more than 50% from the values of ρ ₀ and ρ ₂, with the former compound showing enhanced electrical conductivity than the latter. Similarly in fitting the adiabatic small polaron model for resistivity data of both the samples for T > T _MI , the polaron activation energy is found to differ by about 11%. In addition, the temperature dependent a.c. magnetic susceptibility study of the compounds shows a shift of about 6% in the paramagnetic to ferromagnetic transition temperature (285 K for LCSBMO and 270 K for LCMO).     

High-<Emphasis Type="Italic">T</Emphasis><Subscript>C</Subscript> phase transition in K<Subscript>2</Subscript>Ti<Subscript>6</Subscript>O<Subscript>13</Subscript> lead-free ceramic synthesised using solid-state reaction

Solid-state reaction synthesised K₂Ti₆O₁₃ lead-free ceramic was characterized using XRD, SEM, and X-band EPR, at room temperature. EPR-spectra showed the presence of ( \textFe_\textTi^￠ - V_\textO ^·· ) \left( {{\text{Fe}}_{\text{Ti}}^{\prime } - V_{\text{O}}^{ \bullet \bullet } } \right) defect associate dipoles, in orthorhombic phase, responsible for the broadening of the dielectric anomaly identified in the ε _r (T) plots at T _C  ~ 300 °C. This anomaly resembled a ferroelectric–paraelectric type phase transition following Curie–Weiss type trend. Besides, dielectric loss mechanism jointly represented electrical conduction, dipole orientation, and space charge polarization.     

Synthesis and applications of fluorescent-magnetic-bifunctional dansylated Fe<Subscript>3</Subscript>O<Subscript>4</Subscript>@SiO<Subscript>2</Subscript> nanoparticles

Bifunctional magnetic-luminescent dansylated Fe₃O₄@SiO₂ (Fe₃O₄@SiO₂-DNS) nanoparticles were fabricated by the nucleophilic substitution of dansyl chloride with primary amines of aminosilane-modified Fe₃O₄@SiO₂ core–shell nanostructures. The morphology and properties of the resultant Fe₃O₄@SiO₂-DNS nanoparticles were investigated by transmission electron microscopy, FT–IR spectra, UV–vis spectra, photoluminescence spectra, and vibrating sample magnetometry. The Fe₃O₄@SiO₂-DNS nanocomposites exhibit superparamagnetic behavior at room temperature, and can emit strong green light under the excitation of UV light. They show very low cytotoxicity against HeLa cells and negligible hemolysis activity. The T ₂ relaxivity of Fe₃O₄@SiO₂-DNS in water was determined to be 114.6 Fe mM⁻¹ s⁻¹. Magnetic resonance (MR) imaging analysis coupled with confocal microscopy shows that Fe₃O₄@SiO₂-DNS can be uptaken by the cancer cells effectively. All these positive attributes make Fe₃O₄@SiO₂-DNS a promising candidate for both MR and fluorescent imaging applications.     

Effect of heating rate on the microstructural and magnetic properties of nanocrystalline Fe<Subscript>81</Subscript>Si<Subscript>4</Subscript>B<Subscript>12</Subscript>P<Subscript>2</Subscript>Cu<Subscript>1</Subscript> alloys

The effect of heating rate on the structural and magnetic properties of the nanocrystalline Fe₈₁Si₄B₁₂P₂Cu₁ alloy has been investigated. Amorphous Fe₈₁Si₄B₁₂P₂Cu₁ alloy was annealed at 753 K for 180 s at different heating rates ranging from 0.05 to 5 K/s in protective argon atmosphere. The structural and magnetic properties of the as-quenched and annealed alloys were studied using X-ray diffractometer (XRD), differential scanning calorimeter (DSC), vibrating sample magnetometer (VSM), and B–H loop tracer, respectively. Amorphous precursor prepared by industry-grade raw materials is obtained. The increase of heating rate is found to be significantly effective in decreasing the grain size of α-Fe(Si) phase, but the grain size increases at higher heating rate. The volume fraction of α-Fe(Si) phase shows a monotonic decrease with the increase of the heating rate. The coercivity H _c markedly decreases with increasing heating rate and exhibits a minimum at the heating rate of 0.5 K/s, while the saturation magnetization, M _s, shows a slight decrease. These results suggest that the effect of heating rate on H _c and M _s is originated from the changes of grain size and the volume fraction of α-Fe(Si) phase.     

Enhanced thermal stability in K<Subscript>2</Subscript>O-metakaolin-based geopolymer concretes by Al<Subscript>2</Subscript>O<Subscript>3</Subscript> and SiO<Subscript>2</Subscript> fillers addition

Based on the principle of stability of geopolymer gel as refractory binder, a geopolymeric paste in the K₂O–Al₂O₃–SiO₂ system was developed and used to produce refractory concretes by adding various amount of α-quartz sand (grain size in the range 0.1 μm to 1 mm) and fine powder alumina (grain size in the range 0.1–100 μm). The consolidated samples were characterized before and after sintering using optical dilatometer, DSC, XRD and SEM. The total shrinkage in the range of 25–900 °C was less than 3%, reduced with respect to the most diffused potassium or sodium based geopolymer systems, which generally records a >5% shrinkage. The maximum shrinkage of the basic geopolymer composition was recorded at 1000 °C with a 17% shrinkage which is reduced to 12% by alumina addition. The temperature of maximum densification was shifted from 1000 °C to 1150 or 1200 °C by adding 75 wt% α-quartz sand or fine powder alumina respectively. The sequences of sintering of geopolymer concretes could be resumed as dehydration, dehydroxylation, densification and finally plastic deformation due to the importance of liquid phase. The geopolymer formulations developed in this study appeared as promising candidates for high-temperature applications: refractory, fire resistant or insulating materials.     

Temperature-stable and low loss Fe-containing dielectrics in BaO-Ln<Subscript>2</Subscript>O<Subscript>3</Subscript>-Fe<Subscript>2</Subscript>O<Subscript>3</Subscript>-Ta<Subscript>2</Subscript>O<Subscript>5</Subscript> system

Polycrystalline samples of Ba₄Ln₂Fe₂Ta₈O₃₀ (Ln = La and Nd) were prepared by a high temperature solid-state reaction technique. The formation, structure, dielectric and ferroelectric properties of the compounds were studied. Both compounds are found to be paraelectrics with filled tetragonal tungsten bronze (TB) structure at room temperature. Dielectric measurements revealed that the present ceramics have exceptional temperature stability, a relatively small temperature coefficient of dielectric constant (τ _ε ) of −25 and −58 ppm/°C, with a high dielectric constant of 118 and 96 together with a low dielectric loss of 1.2 × 10⁻³ and 2.8 × 10⁻³ (at 1 MHz) for Ba₄La₂Fe₂Ta₈O₃₀ and Ba₄Nd₂Fe₂Ta₈O₃₀, respectively. The measured dielectric properties indicate that both materials are possible candidates for the fabrication of discrete multilayer capacitors in microelectronic technology.     

Combustion synthesis and structural characterization of Li–Ti mixed nanoferrites

Polycrystalline samples of the mixed nanoferrites, Li_{0·5 + 0·5x} Ti _x Fe_{2·5 − 1·5x} O₄ (0·02 ≤ x ≤ 0·1), were prepared by combustion method at lower temperatures compared to the conventional high temperature sintering for the first time at low temperatures, using PEG which acts as a new fuel and oxidant. XRD patterns reveal a single-phase cubic spinel structure. The as synthesized Li–Ti ferrites are in nanocrystalline phase. The crystallite size was found to be in the range 16–27 nm. SEM images reveal rod-like morphology in all the samples with a discontinuous grain growth. The B–H loops have been traced using VSM technique, for all the compositions, at room temperature and the hysteresis parameters are calculated. Saturation magnetization decreases with increase in Ti content due to the fact that the Ti^4 + ion, which is a non-magnetic ion, replaces a magnetic Fe^3 + ion. The hysteresis loops show clear saturation at an applied field of ±10 kOe and the loops are highly symmetric in nature. The cation distribution is known indirectly by using saturation magnetization values.     

Effect of Dy<Subscript>2</Subscript>O<Subscript>3</Subscript> addition on microstructure,electrical properties,and aging behavior of ZnO–V<Subscript>2</Subscript>O<Subscript>5</Subscript>–MnO<Subscript>2</Subscript>–CoO varistor ceramics

The microstructure, electrical properties, and aging behavior of ZnO–V₂O₅–MnO₂–CoO–Dy₂O₃ varistor ceramics were investigated for different contents of Dy₂O₃. The microstructure consisted of ZnO grain as a main phase and secondary phases such as Zn₃(VO₄)₂, ZnV₂O₄, and DyVO₄. The average grain size increased from 7.6 to 10.1 μm and the sintered density slightly increased from 5.53 to 5.57 g/cm³ with the increase of Dy₂O₃ content. The varistor ceramics added with 0.05 mol% Dy₂O₃ exhibited the most nonlinear properties, with nonlinear coefficient of 30, and the highest stability against DC-accelerated aging stress. The Dy₂O₃ acted as an acceptor due to the decrease of donor density in the range of 2.73 × 10¹⁸/cm³ to 1.28 × 10¹⁸/cm³.     

Synthesis of Mn-doped CeO<Subscript>2</Subscript> nanorods and their application as humidity sensors

Mn-doped CeO₂ nanorods have been prepared from CeO₂ particles through a facile composite-hydroxide-mediated (CHM) approach. The products were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The analysis from the X-ray photoelectron spectroscopy indicates that the manganese doped in CeO₂ exists as Mn^4 +. The responses to humidity for static and dynamic testing proved doping Mn into CeO₂ can improve the humidity sensitivity. For the sample with Mn% about 1·22, the resistance changes from 375·3 to 2·7MΩ as the relative humidity (RH) increases from 25 to 90%, indicating promising applications of the Mn-doped CeO₂ nanorods in environmental monitoring.     

Synthesis and characterization of LiNi<Subscript>0.9</Subscript>Co<Subscript>0.1</Subscript>O<Subscript>2</Subscript> for lithium batteries

LiNi_0.9Co_0.1O₂ cathode material is prepared from LiOH·H₂O and Ni_0.9Co_0.1(OH)₂ by co-precipitation and subsequent two-stage heat treatment in flowing oxygen based on the results of thermogravimetric. The structural and electrochemical properties of the samples are characterized by means of inductively coupled plasma-atomic emission spectrometer (ICP-AES), X-ray diffraction (XRD), scanning electron microscope (SEM), cyclic voltammogram (CV) and charge–discharge studies. All the samples sintered at different temperatures have a typical layered structure with space group R3-m and good electrochemical performances. The sintering temperature has a remarkable effect on the electrochemical performance of the samples. The sample sintered at 730 °C shows the largest initial discharge capacity 191.1 mAh g⁻¹ (50 mA g⁻¹, 3.0–4.3 V) and the best cycling performance. The initial discharge capacity rises to above 200 mAh g⁻¹ with the voltage range 3.0–4.5 V.     

Structural changes induced by Fe<Subscript>2</Subscript>O<Subscript>3</Subscript> addition in strontium-borate glass matrix

Glasses of the xFe₂O₃·(100−x)[B₂O₃·SrO] system, with 0 ≤ x ≤ 30 mol% were studied by X-ray diffraction, density, optical microscopy and FT-IR spectroscopy measurements. The X-ray patterns for the prepared system show that vitreous phase is present only in the sample with x < 40 mol%. For x ≥ 40 mol% in the studied samples is evidenced crystalline phase of Fe₂O₃. SEM measurements for the sample with x = 40 mol% shows that there are formed Fe₂O₃ microcrystallites with 10–20 μm dimension. FT-IR spectroscopy measurements shown that BO₃ and BO₄ are the main structural units of the glass system and the iron ions are located in the glass network.     

Dielectric and ferromagnetic properties of BaTiO<Subscript>3</Subscript>/Ni<Subscript>0.93</Subscript>Co<Subscript>0.02</Subscript>Cu<Subscript>0.05</Subscript>Fe<Subscript>2</Subscript>O<Subscript>4</Subscript> composites

xBaTiO₃ + (1 − x)Ni_0.93Co_0.02Cu_0.05Fe₂O₄ (x = 0.5, 0.6, 0.7, 0.8) composites with ferroelectric–ferromagnetic characteristics were synthesized by the ceramic sintering technique. The presence of constituent phases in the composites was confirmed by X-ray diffraction studies. The average grain size was calculated by using a scanning electron micrograph. The dielectric characteristics were studied in the 100 kHz to 15 MHz. The dielectric constant changed higher with ferroelectric content increasing; and it was constant in this frequency range. The relation of dielectric constant with temperature was researched at 1, 10, 100 kHz. The Curie temperature would be higher with frequency increasing. The hysteresis behavior was studied to understand the magnetic properties such as saturation magnetization (M _s). The composites were a typical soft magnetic character with low coercive force. Both the ferroelectric and ferromagnetic phases preserve their basic properties in the bulk composite, thus these composites are good candidates as magnetoelectric materials.     

Inducing multiferroic behaviour in the diamagnetic Y<Subscript>2</Subscript>O<Subscript>3</Subscript> system

The synthesis and characterization of Y_2−xFe_xO₃ (where x = 0–0.3) compounds has been carried out for their importance in the field of multiferroic materials. The powder X-ray diffraction reveal that the compounds Y_1.95Fe_0.05O₃, Y_1.9Fe_0.1O₃, Y_1.85Fe_0.15O₃ and Y_1.8Fe_0.2O₃ crystallize in tetragonal structure whereas Y_1.75Fe_0.25O₃ and Y_1.7Fe_0.3O₃ compounds crystallize in orthorhombic structure. The change in crystal system with respect to the concentration of Fe may be attributed to the variation in occupancy position of Fe³⁺ into the Y³⁺ site of Y₂O₃ system. Variation in crystal structure, surface morphology and composition was studied by micro-Raman analysis, SEM and EDX analysis. The shift in intense Raman signals from 426 to 385 cm⁻¹ confirms the change in the crystal structure of the prepared compounds. Further it is also identified that the E_g mode of vibration is the dominant in the Fe substituted compounds. The substitution of Fe in the Y₂O₃ system leads to the increase in the intensity of resonance band, which indicates a large polarisability variation in the Y_2−xFe_xO₃ compounds. Diffused reflectance studies show a red shift in energy gap values while increasing the concentration of Fe. The room temperature magnetization and electron paramagnetic resonance studies reveal that the incorporation of Fe in the Y₂O₃ system leads to magnetic phase change from diamagnetic to ferromagnetic. The electric polarization studies imply that the substitution of lower ionic radii element Fe³⁺ in the Y³⁺ site leads to distortion in the lattice and show the way to spontaneous dipole moment and it was found that the Y_1.8Fe_0.2O₃ compound exhibits the possibility of multiferroic behaviour. Therefore this paper explores the possibility of inducing ferromagnetic and ferroelectric behaviour in the Fe substituted yttrium oxide system.     

Giant dielectric and electrical properties of sodium yttrium copper titanate: Na<Subscript>1/2</Subscript>Y<Subscript>1/2</Subscript>Cu<Subscript>3</Subscript>Ti<Subscript>4</Subscript>O<Subscript>12</Subscript>

The electrical properties and dielectric response in Na_1/2Y_1/2Cu₃Ti₄O₁₂ ceramic prepared by conventional solid-state reaction method and sintered at 1,090 °C for 5 h were investigated as functions of frequency and temperature. Main phase of Na_1/2Y_1/2Cu₃Ti₄O₁₂ with CaCu₃Ti₄O₁₂-like crystallographic structure and CuO secondary phase were observed in the X-ray diffraction pattern. Abnormal grain growth was observed just as observed in CaCu₃Ti₄O₁₂ ceramics. The Na_1/2Y_1/2Cu₃Ti₄O₁₂ ceramic exhibits a high ε′ of ~2.04 × 10⁴ at 20 °C and 1 kHz and low tan δ (with the minimum 0.080 at 5 kHz). Impedance spectroscopy analysis reveals that Na_1/2Y_1/2Cu₃Ti₄O₁₂ ceramic is electrically heterogeneous, consisting of semiconducting grains and insulating grain boundaries. Giant ε′ response in Na_1/2Y_1/2Cu₃Ti₄O₁₂ ceramic is therefore attributed to an internal barrier layer capacitor effect.     

Magnetic and Superconducting Properties of Doped and Undoped Double Perovskite Sr<Subscript>2</Subscript>YRuO<Subscript>6</Subscript>

We report here SQUID (magnetization) measurements, along with supporting specific heat, Raman, SEM (scanning electron microscope), EDX (energy dispersive X-ray) and XRD (X-ray diffraction) measurements, on Cu-doped and undoped double perovskite Sr₂²⁺Y³⁺Ru⁵⁺O₆^2-\mathrm{Sr}_{2}^{2+}\mathrm{Y}^{3+}\mathrm{Ru}^{5+}\mathrm{O}_{6}^{2-} (abbreviated as SrY2116) system grown as single crystal using high-temperature solution growth technique. These measurements show the undoped system to be a nonmetallic (insulating) spin glass (SG) and the ∼5–30% Cu-doped (i.e. Cu-concentration/(Cu + Ru-concentration) ∼5–30%) system to be a spin glass superconductor (SGSC) with T _c (critical temperature) ∼28–31 K and superconducting volume fraction, f _sc∼2.2–9%. To mention, similar measurements done on undoped and Cu-doped BaY2116 and BaPr2116 systems show for them the same (SG, SGSC) behaviors. However they show a decrease in T _c and f _sc when diamagnetic Y³⁺ ions are replaced by Pr³⁺ spins, presumably due to enhanced internal pair breaking, and also decreased Cu–O–Cu overlap, owing to Pr³⁺ presence; these phenomena are known to exist in the Pr123 compound, PrBa₂Cu₃O_7−δ (δ∼0), due to ∼10% of Pr³⁺ ions having tendency to occupy Ba²⁺ sites. Measurements done on undoped and Cu-doped SrHo2116 show similar SG and SGSC properties. Further, the undoped and Cu-doped SrY2116 crystals grown by hydrothermal growth technique (i.e., grown using lower temperature and high pressure) show same behaviors. From these investigations it can be said that the undoped Ru-double perovskites (A₂BB′O₆, B′=Ru) are SG systems and that Cu-doped Ru-double perovskites (A₂BB′O _δ , δ∼6, B′=Ru_1−x Cu _x , 0<x≲0.3) are SG superconductors (SGSCs). Results are discussed.     

Dielectric relaxation behaviour of Sr<Subscript><Emphasis Type="Bold">2</Emphasis></Subscript>SbMnO<Subscript><Emphasis Type="Bold">6</Emphasis></Subscript> ceramics fabricated from nanocrystalline powders prepared by molten salt synthesis

Double perovskite polycrystalline single phase and dense Sr ₂ SbMnO ₆ (SSM) ceramics, fabricated using the nanocrystalline powders synthesized by molten salt method, exhibited high dielectric constant with low dielectric loss as compared to that of SSM ceramics obtained from the powders prepared by solid-state synthesis method. The dielectric data obtained over a wide frequency (100 Hz–1 MHz) and temperature (190 K–300 K) ranges exhibited distinct relaxations owing to both the grain and grain boundary. The dielectric dispersion was modeled using the Cole–Cole equation consisting of two separate relaxation terms corresponding to the grain and grain boundary. The grain and grain boundary relaxations observed in the Nyquist plots (Z ^′ and Z ^″) were modeled by an equivalent circuit consisting of two parallel RC circuits connected in series with each other. A careful analysis of both the impedance (Z ^″ vs ω) and modulus (M ^″ vs ω) behaviour corroborated the conclusions drawn from the dielectric data.