Development of nanocrystalline Mn-Zn ferrites for high frequency transformer applications

Microwave-Hydrothermal (M-H) method has been successfully used for the synthesis of nanocrystalline Mn-Zn ferrites which are used for high-frequency applications. As synthesized powders were characterized using X-ray diffraction (XRD) and transmission electron microscopy (TEM). The nanopowders were annealed at 600 °C/20 min using the microwave sintering method. The frequency dependence of dielectric constant (ε′) was measured in the range of 10 Hz-1.3 GHz and initial permeability (μ_i) was measured in the range of 10 Hz-1 MHz. The total power loss (P_t) was measured on the annealed samples at 100 kHz and 200 mT condition. Conductor-embedded-ferrite transformers were fabricated and output power (P_o), efficiency (η) and temperature rise (ΔT) were measured at sinusoidal voltage of 25 V at 1 MHz. The transformer efficiency (η) was found to be high and surface rise of temperature (ΔT) is very low.     

Fuel additives and heat treatment effects on nanocrystalline zinc ferrite phase composition

Nanocrystalline ZnFe₂O₄ powder was prepared by the auto-combustion method using citric acid, acetic acid, carbamide and acrylic acid as fuel additives. Pure spinel zinc ferrite with the crystallite size of about 15 nm can be obtained by using acrylic acid as fuel additive. Samples prepared using other fuel additives contain ZnO impurities. In order to eliminate ZnO impurities, the sample prepared with citric acid as fuel additive was annealed at different temperatures up to 1000 °C in air and in argon. Annealed powders have pure ZnFe₂O₄ phase when annealing temperature is higher than 650 °C in air. Sample annealed at 650 °C in air is paramagnetic. However, annealed powders become a mixture of Fe₃O₄ and FeO after annealing at 1000 °C in argon atmosphere due to Zn volatility and the reduction reaction.     

Dielectric behavior of spin-deposited nanocrystalline nickel-zinc ferrite thin films processed by citrate-route

Nanocrystalline nickel-zinc ferrite thin films with the general formula Ni_1−xZn_xFe₂O₄, where x=0.0, 0.2, 0.4 and 0.6 were fabricated via a chemical route known as the citrate precursor route. These films were spin-deposited on indium-tin oxide coated glass, fused quartz and amorphous Si-wafer substrates, and annealed at various temperatures up to 650 °C. The films annealed below 400 °C were found to be X-ray amorphous, while the films annealed at and above 400 °C were polycrystalline exhibiting a single-phase spinel structure. The average grain size of the films evaluated by transmission electron microscopy, is found to be in the range 4-8.5 nm. The room temperature DC resistivity of the films is in the range 10³-10⁷ Ω m. Dielectric constant and dielectric loss were measured in the frequency range 100 Hz-1 MHz. Dielectric constant of the films is found to lie between 25 and 44, while the loss factor is if the order of 10⁻². The higher values of the dielectric constant for films having higher zinc concentration are attributable to the enhanced hopping between Fe²⁺ and Fe³⁺ ions in these samples. The M-H hysteresis measurement of the nickel ferrite thin films annealed at 650 °C showed narrow hysteresis loop—a characteristic of soft ferromagnetic material.     

The influence of substrate temperature and annealing on the properties of pulsed laser-deposited YIG films on fused quartz substrate

Yttrium iron garnet (YIG) thin films were deposited on fused quartz substrate at different substrate temperatures (T_s) varying from room temperature (RT) to 850 °C using pulsed laser deposition (PLD) technique. All the films in the as-deposited state were X-ray amorphous and non-magnetic at RT. The film deposited at RT after annealing at temperatures T_a?700 °C showed both X-ray peaks and the magnetic order. The films deposited at higher T_s (500–850 °C) and then annealed at 700 °C resulted in better-quality films with higher 4πM_s value. The highest value of magnetization was for the sample deposited at 850 °C and annealed at 700 °C, which is 68% of the bulk 4πM_s value.     

Microwave electromagnetic property of SiO2-coated carbonyl iron particles with higher oxidation resistance

Flake carbonyl iron (CI) particles and amorphous silica were used to fabricate SiO₂-coated CI particles through the Stober process. The as-prepared SiO₂-coated CI particles were annealed at 500 °C for 1 h under argon and air atmosphere. The XRD results showed that only a little amount of oxides were formed when the SiO₂-coated CI particles were annealed under the air atmosphere. The magnetic properties of the SiO₂-coated CI particles before and after annealing treatment showed little change, indicating that amorphous silica appears to be very effective in reducing oxidation of the CI particles. The reflection loss exceeding −10 dB can be obtained in the frequency range of 9.9-14.6 GHz and a minimum value can be reached to −21.5 dB at 12.2 GHz for the annealed SiO₂-coated CI particles with the composite thickness being 1.5 mm. The mechanism of annealing treatment influence on the electromagnetic properties and microwave absorption of the SiO₂-coated CI particles was also discussed.     

Magnetic properties of xNi0.53Cu0.12Zn0.35Fe1.88O4+(1−x)BaTiO3 nanocomposites

The nanocrystalline Ni_0.53Cu_0.12Zn_0.35Fe_1.88O₄ and BaTiO₃ powders were prepared using Microwave-Hydrothermal (M-H) method at 160 °C/45 min. The as synthesized powders were characterized using the X-ray diffraction (XRD) and Transmission Electron Microscope (TEM). The size of the powders that were synthesized using M-H system was found to be ∼30 and ∼50 nm for ferrite phase and ferroelectric phases, respectively. The powders were densified using microwave sintering method at 900 °C/30 min. The ferrite and ferroelectric phases were observed from XRD and morphology of the composites was observed with the Scanning Electron Microscope (SEM).The magnetic hysteresis loops were recorded using the Vibrating Sample Magnetometer (VSM).The frequency dependence of real (μ′) and imaginary (μ″) parts of permeability was measured in the range of 1 MHz-1.8 GHz. The permeability decreases with an increase of BaTiO₃ content at 1 MHz. The transition temperature (T_C) of ferrite was found to be 245 °C. The T_C of composite materials decreases with an increase in BaTiO₃ content.     

Dynamical properties of Cr-Fe amorphous powders obtained from mechanical milling

Mössbauer measurements have been performed in situ in the temperature range of 25 to 550°C for three Cr-Fe samples: Cr₇₂Fe₂₈ crystalline alloy (I), as-milled amorphous Cr₆₅Fe₃₅ powders made by mechanical grinding (II) and the same powder annealed at 420°C for 2 h (III). The temperature dependence of isomer shifts for samples I and III follows the variation predicted by the second-order Doppler effect, while for the sample II a deviation has been observed. The Debye temperatures have been determined to be 420, 400 and 380 K for sample I, III and II, respectively. A linear dependence onT ^3/2 of quadrupole splitting of the annealed powder is observed.     

Spin-deposited nanocrystalline lithium ferrite thin films: Fabrication and characterization

Thin films of lithium ferrite (with general composition Li_0.5Fe_2.5O₄) were fabricated at low temperatures (up to 650 °C) by citrate-route using spin-deposition technique. Deposited films consisted of nanometer-sized grains as evidenced by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) and atomic force microscopy (AFM) techniques. XRD patterns for annealed films showed broad peaks exhibiting a spinel phase. Size of nanocrystallites is estimated to be 3-7 nm using Scherrer's equation. Average grain size ∼8.5 nm is observed from TEM images of films annealed at 650 °C. Scanning electron micrographs show the formation of spherical aggregates of around 130 nm in diameter. The AFM analysis clearly evidenced the development of nanograins even at low (∼500 °C) annealing temperatures. Significant decrease in complex dielectric permittivity (∈′ − j∈″) with frequency is observed in the low frequency (100 Hz-1 MHz) as well as in X-band microwave frequency (8-12 GHz) region. ∈′ is found to be in the range of 15.7-33.9 in low frequency region, whereas in X-band microwave frequency region, it is found to lie between 3.9 and 4.9. Similarly, ∈″ is found to be 0.16-5.9 in the low frequency region, and 0.002-0.024 in the X-band microwave frequency region. Room temperature dc resistivity of these films is estimated to lie in the range of 10⁶-10⁸ Ω cm. These results strongly suggest that citrate-route processed nanocrystalline lithium ferrite thin films are promising candidates for monolithic microwave integrated circuits (MMICs).     

Annealing effect on soft magnetic properties and magnetoimpedance of Finemet Fe73.5Si13.5B9Nb3Au1 alloy

Effect of annealing on the soft magnetic properties of Fe_73.5Si_13.5B₉Nb₃Au₁ amorphous ribbon has been investigated by means of structure examination, magnetoimpedance ratio (MIR) and incremental permeability ratio (PR) spectra measured in the frequency range of 1–10 MHz at a fixed current of 10 mA X-ray diffraction analysis showed that the as-cast sample was amorphous and it became nanocrystalline under a proper heat treatment. When annealing amorphous alloy at 530 °C for 30, 60, 90 min, soft magnetic properties have been improved drastically. Among the samples investigated, the sample annealed at 530 °C for 90 min showed the softest magnetic behavior. The MIR and PR curves revealed the desirable changes in anisotropy field depending upon annealing.     

Preparation and characterization of ZnSn-substituted barium ferrite thin films

The preparation of ZnSn-substituted barium ferrite films by sputtering deposition was studied. The as-sputtered films were amorphous, and annealing at a minimum of 750 °C was required to crystallize the films, based on the X-ray diffraction analysis and the magnetic measurements. Scanning electron microscopy combined with energy-dispersive X-ray spectroscopic microanalysis confirmed that the films were single phase with the composition BaZn_xSn_xFe_12−2xO₁₉, x=0.2−0.3, and their thicknesses were 0.4-1.0 μm when annealed at 750-900 °C. Atomic and magnetic force microscopy studies showed no significant grain growth upon annealing and that the films consisted of single-domain grains forming interaction-cluster-type domains. The natural ferromagnetic resonance frequency was determined at around 4 GHz, together with substantial magnetic losses that make these films promising candidates for microwave absorbers.     

Synthesis and characterization of NiCoMnCuFe1.96O4 for circulator application

Modern accelerator design practice includes the use of high-quality ferrites for circulator applications with ever-increasing requirements on power handling ability. Modeling studies of new designs are of increasing economic importance, but are frequently hindered by lack of measured values of the ceramic loss factors. We have developed a nanocrystalline ferrite material with composition Ni_0.94Co_0.03Mn_0.04Cu_0.03Fe_1.96O₄. Nanocrystalline NiCoMnCu ferrite powders were synthesized using a microwave-hydrothermal method at 160 °C for 40 min. The ferrite formation conditions, such as pH, temperature and time, were optimized. The phase of the samples was identified by X-ray diffraction and was characterized by Fourier transformation infrared spectroscopy. The size of the nanocrystalline ferrite of as-synthesized powders was 10 nm. The powder was densified at different temperatures using a microwave sintering method. The complex permittivity and permeability of the sintered samples were measured over a frequency range from 10 kHz to 1.8 GHz at room temperature. The applicability of the samples for circulators was tested via the measurement of the ferromagnetic resonance linewidth and the results are presented.     

Nanocrystalline gadolinium iron garnet for circulator applications

Due to high resistivity and low microwave losses, gadolinium iron garnets (GdIG) are useful materials for non-reciprocal devices such as circulators or isolators. Keeping the miniaturization and cost reduction in mind, the trend is to modify the conventional methods of preparation of samples. In this connection we have synthesized nanocystalline GdIG by using the Microwave Hydrothermal method at 160 °C/45 min. As synthesized powders were characterized by using X-ray diffraction (XRD), transmission electron microscopy and Fourier Transform Infrared Spectroscopy. XRD patterns show the formation of a garnet phase with crystallite size varying between 19 nm and 40 nm. Differential Thermal Analysis studies were also carried out on the nanopowders. The powders were densified at a lower sintering temperature of 1100 °C/45 min using a microwave sintering method. The sintered samples were characterized by XRD and atomic force microscopy. The frequency dependence of complex permittivity and ferromagnetic resonance were measured in the K_a band frequency (27–40 GHz). Magnetic properties were also measured at room temperature.     

Influence of deposition temperature on the structural and morphological properties of Be3N2 thin films grown by reactive laser ablation

Be₃N₂ thin films have been grown on Si(1 1 1) substrates using the pulsed laser deposition method at different substrate temperatures: room temperature (RT), 200 °C, 400 °C, 600 °C and 700 °C. Additionally, two samples were deposited at RT and were annealed after deposition in situ at 600 °C and 700 °C. In order to obtain the stoichiometry of the samples, they have been characterized in situ by X-ray photoelectron (XPS) and reflection electron energy loss spectroscopy (REELS). The influence of the substrate temperature on the morphological and structural properties of the films was investigated using scanning electron microscopy (SEM), atomic force microscopy (AFM) and X-ray diffraction (XRD). The results show that all prepared films presented the Be₃N₂ stoichiometry. Formation of whiskers with diameters of 100-200 nm appears at the surface of the films prepared with a substrate temperature of 600 °C or 700 °C. However, the samples grown at RT and annealed at 600 °C or 700 °C do not show whiskers on the surface. The average root mean square (RMS) roughness and the average grain size of the samples grown with respect the substrate temperature is presented. The films grown with a substrate temperature between the room temperature to 400 °C, and the sample annealed in situ at 600 °C were amorphous; while the αBe₃N₂ phase was presented on the samples with a substrate temperature of 600 °C, 700 °C and that deposited with the substrate at RT and annealed in situ at 700 °C.     

Microstructure evolution and electromagnetic properties improvement of Al18B4O33w/Co composite powders through heat-treatment

Al₁₈B₄O₃₃w/Co composite powders were prepared through electroless depositing Co on Al₁₈B₄O₃₃ whiskers and the microstructure of the prepared composite powders was adjusted through heat-treatment. The included Co oxide is reduced and the density as well as the crystal perfection of the coatings is improved when annealed at 400 °C in H₂ atmosphere. An increase of 10⁵ S m⁻¹ in conductivity together with an increase of 28% in M_s is obtained, resulting in a prominent increase of the permittivity and the permeability. The increase of permittivity, specifically the dielectric relaxation is attributed to the increase of conductivity. The increase of permeability is attributed to the increase of M_s and the microstructure evolution. The increase of electromagnetic parameters in 2-18 GHz band is believed to enhance the electromagnetic wave absorbing performance of the Al₁₈B₄O₃₃w/Co composite powders.     

Recoilless fraction, structural, magnetic and thermal properties of Fe73.5Cu1Nb3Si13.5B9 alloy

Differential scanning calorimetry, X-ray diffraction and room temperature Mössbauer spectrum measurements of Fe_73.5Cu₁Nb₃Si_13.5B₉ (Finemet) alloy have been carried out in order to study its structural and magnetic properties as a function of annealing temperature. The DSC profile of as-quenched Finemet showed two exothermic peaks at 530 and 702 °C, corresponding to two crystallization processes. The Finemet alloy remains amorphous at 450 °C with one broad peak in XRD pattern and one broad sextet in Mössbauer spectrum. When the Finemet alloy was annealed at 550 °C, only well indexed body-center-cubic phase was detected. After being annealed at 650 and 750 °C, the XRD patterns showed the coexistence of α-Fe(Si) and Fe-B intermetallic phases with the increase in XRD peak intensities, indicating the growth of crystallites and the decomposition of Fe_73.5Cu₁Nb₃Si_13.5B₉ alloy at elevated temperatures. The Mössbauer spectra of annealed Finemet alloy could be fitted with 4 or 5 sextets and one doublet at higher annealing temperatures, revealing the appearance of different crystalline phases corresponding to the different Fe sites above the crystallization temperature. The appearance of the nanocrystalline phases at different annealing temperatures was further confirmed by the recoilless fraction measurements.     

Heat treatment effects on microstructure and magnetic properties of Mn-Zn ferrite powders

Mn-Zn ferrite powders (Mn_0.5Zn_0.5Fe₂O₄) were prepared by the nitrate-citrate auto-combustion method and subsequently annealed in air or argon. The effects of heat treatment temperature on crystalline phases formation, microstructure and magnetic properties of Mn-Zn ferrite were investigated by X-ray diffraction, thermogravimetric and differential thermal analysis, scanning electron microscopy and vibrating sample magnetometer. Ferrites decomposed to Fe₂O₃ and Mn₂O₃ after annealing above 550 °C in air, and had poor magnetic properties. However, Fe₂O₃ and Mn₂O₃ were dissolved after ferrites annealing above 1100 °C. Moreover, the 1200 °C annealed sample showed pure ferrite phase, larger saturation magnetization (M_s=48.15 emu g⁻¹) and lower coercivity (H_c=51 Oe) compared with the auto-combusted ferrite powder (M_s=44.32 emu g⁻¹, H_c=70 Oe). The 600 °C air annealed sample had the largest saturation magnetization (M_s=56.37 emu g⁻¹) and the lowest coercivity (H_c=32 Oe) due to the presence of pure ferrite spinel phase, its microstructure and crystalline size.     

Synthesis,characterization and magnetic properties of MFe2O4 (M=Co,Mg, Mn,Ni) nanoparticles using ricin oil as capping agent

We focused on obtaining MFe₂O₄ nanoparticles using ricin oil solution as surfactant and on their structural characterization and magnetic properties. The annealed samples at 500 °C in air for 6 h were analyzed for the crystal phase identification by powder X-ray diffraction using CuKα radiation. The particle size, the chemical composition and the morphology of the calcinated powders were characterized by scanning electron microscopy. All sintered samples contain only one phase, which has a cubic structure with crystallite sizes of 12–21 nm. From the infrared spectra of all samples were observed two strong bands around 600 and 400 cm⁻¹, which correspond to the intrinsic lattice vibrations of octahedral and tetrahedral sites of the spinel structure, respectively, and characteristic vibration for capping agent. The magnetic properties of fine powders were investigated at room temperature by using a vibrating sample magnetometer. The room temperature M–H hysteresis loops show ferromagnetic behavior of the calcined samples, with specific saturation magnetization (M_s) values ranging between 11 and 53 emu/g.     

Characterization and luminescent properties of SiO2:ZnS:Mn and ZnS:Mn nanophosphors synthesized by a sol-gel method

ZnS and SiO₂-ZnS nanophosphors, with or without different concentration of Mn²⁺ activator ions, were synthesized by using a sol-gel method. Dried gels were annealed at 600 °C for 2 h. Structure, morphology and particle sizes of the samples were determined by using X-ray diffraction (XRD), highresolution transmission electron microscopy (HRTEM) and field emission scanning electron microscopy (FESEM). The diffraction peaks associated with the zincblende and the wurtzite structures of ZnS were detected from as prepared ZnS powders and additional diffraction peaks associated with ZnO were detected from the annealed powders. The particle sizes of the ZnS powders were shown to increase from 3 to 50 nm when the powders were annealed at 600 °C. An UV-Vis spectrophotometer and a 325 nm He-Cd laser were used to investigate luminescent properties of the samples in air at room temperature. The bandgap of ZnS nanoparticles estimated from the UV-Vis data was 4.1 eV. Enhanced orange photoluminescence (PL) associated with ⁴T₁→⁶A₁ transitions of Mn²⁺ was observed from as prepared ZnS:Mn²⁺and SiO₂-ZnS:Mn²⁺ powders at 600 nm when the concentration of Mn²⁺ was varied from 2-20 mol%. This emission was suppressed when the powders were annealed at 600 °C resulting in two emission peaks at 450 and 560 nm, which can be ascribed to defects emission in SiO₂ and ZnO respectively. The mechanism of light emission from Mn²⁺, the effect of varying the concentration on the PL intensity, and the effect of annealing are discussed.     

Li0.5Fe2.5−xMnxO4 ferrite sintered from microwave-induced combustion

Li_0.5Fe_2.5−xMn_xO₄ (0≦x≦1.0) powders with small and uniformly sized particles were successfully synthesized by microwave-induced combustion, using lithium nitrate, ferric nitrate, manganese nitrate and carbohydrazide as the starting materials. The process takes only a few minutes to obtain as-received Mn-substituted lithium ferrite powders. The resultant powders annealed at 650 ^°C for 2 h and were investigated by thermogravimeter/differential thermal analyzer (TG/DTA), X-ray diffractometer (XRD), transmission electron microscopy (TEM), vibrating sample magnetometer (VSM), and thermomagnetic analysis (TMA). The results revealed that the Mn content were strongly influenced the magnetic properties and Curie temperature of Mn-substituted lithium ferrite powder. As for sintered Li_0.5Fe_2.5−xMn_xO₄ specimens, substituting an appropriate amount of Mn for Fe in the Li_0.5Fe_2.5−xMn_xO₄ specimens markedly improved the complex permeability and loss tangent.     

Sintering temperature dependence of room temperature magnetic and dielectric properties of Co0.5Zn0.5Fe2O4 prepared using mechanically alloyed nanoparticles

Co_0.5Zn_0.5Fe₂O₄ nanoparticles were prepared using mechanical alloying (MA) and sintering. The crystallite size, coercivity, retentivity and saturation magnetization were also measured. The frequency dependence of dielectric and the magnetic parameters, namely, real permittivity ε′, loss tanget tan δ, real permeability μ′ and loss factor μ″ were measured at room temperature for samples sintered from 600 to 1000 °C, in the frequency range 10 MHz to 1.0 GHz. The results show that the crystallite size of the resulting products ranges between 16 and 67 nm for as-milled sample and the sample sintered at 1000 °C, respectively. The sample sintered at 1000 °C, measured at room temperature exhibited a saturation magnetization of 37 emu g⁻¹. The values of permittivity remain constant within the measured frequency, but vary with sintering temperature. The permeability values, on the other hand however vary with both the sintering temperature and the frequency, thus, the absolute value of the permeability decreased after the natural resonance frequency.