Solid State Sciences 113 (2021) 106553 Contents lists available at ScienceDirect Solid State Sciences journal homepage: http://www.elsevier.com/locate/ssscie Electromagnetic and radar absorbing properties of γ Fe2O3/ Ba4Co2Fe36O60-epoxy polymeric composites for stealth applications Vivek Pratap a, *, Amit K. Soni b, Himangshu B. Baskey b, S.M. Abbas b, A.M. Siddiqui a, N. Eswara Prasad b a b Department of Physics, Jamia Millia Islamia, New Delhi, 110025, India Defence Materials and Stores Research and Development Establishment, Kanpur, 208013, India A R T I C L E I N F O A B S T R A C T Keywords: Strategic materials Barium hexaferrite Gamma iron oxide Magnetic properties Electromagnetic properties Reflection loss Microwave absorbers Various constituent ratios with 50:30, 40:40 and 30:50 wt % of U-type barium hexaferrite (Ba4Co2Fe36O60) and Gamma iron oxide (γ Fe2O3) have been used to designing the radar absorbing composites within epoxy resin system. In the current work, studies are done on electromagnetic and absorbing properties of γ Fe2O3 powder dispersed Ba4Co2Fe36O60-epoxy composites. X-Ray Diffraction (XRD), Field Emission Scanning Electron Micro­ scope (FESEM) and Vibrating Sample Magnetometer (VSM) tools have been used for structural, surface morphology and magnetic properties respectively of the synthesized powder and fabricated composites. The electromagnetic properties (ε′ , ε", μ’ & μ") of fabricated composites were retrieved from measured reflection (S11 & S22) and transmission (S12 & S21) parameters in 2–18 GHz frequency range. Experimental finding show that the fabricated composite having 50 wt % of γ Fe2O3 of designed Ba4Co2Fe36O60/γ Fe2O3-epoxy composites possesses maximum absorption of 98.8% (RLmin of − 19.89 dB) at 13.2 GHz for sample thickness of 3.2 mm. The fabricated microwave absorbers confirm the effective absorption performance which has potential for strategic applications and stealth technology. 1. Introduction Electromagnetic spectrums having a part of frequency range between 0.3 GHz and 300 GHz known microwaves are important for smooth functioning electronic devices and system, and also for design and development of microwave absorbers in this frequency region. Due to the tremendous advancement in wireless communication, electronics and aviation sectors, microwave absorbers are working in various sys­ tems and subsystems level under different frequencies region. Conse­ quently, electromagnetic compatibility is a major issue as the radio frequency (RF) radiation causes concern for human health. In order to mitigate such issues, it is of paramount importance for the synthesis of microwave/radar absorbing filler materials which can be used for electromagnetic interference/shielding applications. On the other hand for military applications, microwave/radar absorbing materials can be used in various forms such as paints and composites for reducing the radar cross section (RCS) of various strategic targets such as aircrafts, missiles etc [1,2]. From the past decades, microwave/radar absorbing materials (MAMs/RAMs) have been designed and intensively explored to remove such problems with scientific interest [3,4]. Single domain iron oxide nanoparticles with super paramagnetic behavior; maghemite (γ Fe2O3) is individually most demanding materials among the oxides and are used in various applications such as; magnetic tape, recording chip, motors, transformer cores, refrigerators and medical applications [5,6]. While, U-type barium hexaferrite (Ba4Co2Fe36O60; BaU) have been extensively used as radar/EM wave absorbers. Due to wide range of application of these magnetic materials, scientific community has been working tremendously in the field of microwave absorbing coatings and composites. It has been observed from literature findings that particle size and morphology of synthesized filler particulates influence the EM properties to a large extent [7–9]. The particle size and structural properties of synthesized materials can be controlled significantly by optimizing various parameters of solid state synthesis technique as a result, which ultimately helps in improving the overall microwave absorber performances of synthesized composites [10]. Literature studies also reveals that ferrites serve as more potential electromagnetic * Corresponding author. E-mail addresses: vivek.can.pratap@gmail.com (V. Pratap), amitsoni.kgp@gmail.com (A.K. Soni), himanshudmsrde@gmail.com (H.B. Baskey), abbas93@ rediffmail.com (S.M. Abbas), amsiddiqui@jmi.ac.in (A.M. Siddiqui), neswarap@rediffmail.com (N.E. Prasad). https://doi.org/10.1016/j.solidstatesciences.2021.106553 Received 9 November 2020; Received in revised form 22 January 2021; Accepted 24 January 2021 Available online 30 January 2021 1293-2558/© 2021 Elsevier Masson SAS. All rights reserved. V. Pratap et al. Solid State Sciences 113 (2021) 106553 Fig. 1. XRD patterns (a) for U type BHF powder sintered at 1300 ◦ C temperature for 4 h, (b) for γ Fe2O3 powder and (c) for various wt. % ratios of Ba4Co2Fe36O60 & γ Fe2O3 within epoxy matrix. interference (EMI) shielding/radar absorbing materials than their dielectric counterparts. Ferrite based absorbers consist various losses such as; magnetic loss factor by natural, exchange resonance and dielectric loss factor from interfacial polarization and relaxation results it can be suitably used for scientific and industrial applications [11–13]. In this proposed scientific work, BaU and γ Fe2O3 have been used as potential filler materials for microwave absorber, further in order to improve its EM properties, a solid state reaction technique is employed for synthesis of barium hexagonal U-type ferrite (Ba2Co2Fe36O60). Further various microwave absorber composites have been fabricated using synthesized U type ferrite along with maghemite powder in resin system. Magnetic absorbing materials and fabricated composites have also been characterized for structural, surface and magnetic properties using X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM), and Vibrating Sample Magnetometer (VSM) respectively. Further under this frame work of current research, EM properties such as complex permittivity and complex permeability have also been retrieved in the frequency range of 2–18 GHz using measured reflection and trans­ mission coefficients of test specimen. Moreover, studies on the micro­ wave absorption performance of various fabricated composites have been caused entire the frequency region of 2–18 GHz. Sigma Aldrich, USA consisting of analytical grade were used for syn­ thesis of U type hexagonal ferrite material. All starting materials have been weighted in stoichiometric proportion for the synthesis of U-type hexaferrite. The other prominent filler material Gamma iron oxide; γ Fe2O3 nano particles purchased from M/s Alfa Aesar, USA along with epoxy resin; (trade name: Araldite® LY 5052 and Aradur® HY 5052) was purchased from M/s Huntsman Ltd., USA, used to design the absorbing composites. 2.2. Synthesis of Ba4Co2Fe36O60 powder U-type barium hexaferrite (Ba4Co2Fe36O60) powder was synthesized using solid state reaction route having high purity starting materials; BaCO3, Co3O4, Fe2O3 as previously described. Starting materials were used as received and further mixture was prepared in stoichiometric proportion of Ba4Co2Fe36O60 in acetone medium using ball milling for 18 h. Further wet mixture was dried and further sintered at 1300 ◦ C in air medium using high temperature box furnace. Finally, synthesized powder were sieved using a standard mesh in order to achieve particle size having dimension in range lesser than 40 μm. 2.3. Fabrication of Ba4Co2Fe36O60/γ Fe2O3 -epoxy composite 2. Experimental details A series of microwave absorbing composites was fabricated using wet mixing technique having various compositions of 50:30, 40:40 and 30:50 wt % (Ba4Co2Fe36O60: γ Fe2O3) in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. The thermosetting resin system were used to fabricate the 2.1. Materials The starting materials such as BaCO3, Co3O4 and Fe2O3 from M/s 2 V. Pratap et al. Solid State Sciences 113 (2021) 106553 Fig. 2. Scanned micrographs of (a) synthesized Ba4Co2Fe36O60 powder sintered at 1300 ◦ C temperature for 4 h (b) γ Fe2O3 powder, (c–e) morphological images of various wt. % ratio (50:30, 40:40 and 30:50 wt %) of Ba4Co2Fe36O60 and γ Fe2O3 within epoxy matrix. polymeric composites based on two pack of Araldite® LY 5052 and Aradur® 5052 purchased from Huntsman Ltd., USA. The wet mixture with proportionate ratios of filler materials and resin system was embedded in desired toroidal shaped steel mould for preparation of samples having inner and outer diameter of 3.0 mm and 7.0 mm respectively. Subsequently, the loaded mould was kept in hot press at 60 ◦ C temperature under pressure of 10 MPa (MPa) for 2 h for finished test specimens [14]. dispersive spectrometer (EDS) detector was employed to analyze the chemical composition and crystallographic nature of sample with the elemental attachment available together with scanning electron micro­ scope. Magnetic properties of synthesized powder and prepared com­ posite specimens were characterized using Vibrating sample magnetometer (VSM, MicroSense, LLC technologies) at room tempera­ ture under an applied magnetic field ranging from − 18 to +18 kilo Oersted (kOe). Further, the electromagnetic properties in terms of complex permittivity (εr) and complex permeability (μr) for designed composites were computed from measured scattering (reflection and transmission) parameters using Agilent vector network analyzer (VNA) employing a co-axial transmission line technique for the frequency range of 2–18 GHz. 2.4. Characterization and measurement of properties The synthesized BaU (Ba4Co2Fe36O60) powder was characterized using X-ray diffractometer (XRD, PANalytical make, Xpert-Pro model) in the diffraction angle (2θ) ranging from 20◦ to 60◦ with scanning rate of 0.0167◦ /s. Field emission scanning electron microscope (FE-SEM, FEI make, Quanta 200 model) was used to examine the grain size and morphology of synthesized powder and prepared composites. Energy 3 V. Pratap et al. Solid State Sciences 113 (2021) 106553 Fig. 3. Corresponding EDS analysis of (a) synthesized Ba4Co2Fe36O60 powder sintered at 1300 ◦ C temperature for 4 h (b) γ Fe2O3 powder, (c–e) various wt. % ratio (50:30, 40:40 and 30:50 wt %) of Ba4Co2Fe36O60 and γ Fe2O3 within epoxy matrix. 3. Results and discussion of magnetic filler (50:30, 40:40 & 30:50 wt % of Ba4Co2Fe36O60 and γ Fe2O3) in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites as shown in Fig. 1 (c). 3.1. Phase confirmation and crystal structure The structural characteristics of synthesized Ba4Co2Fe36O60, γ Fe2O3 powder and prepared composites were identified using XRD pattern and shown in Fig. 1(a–c). It can be observed from the corresponding figure that the synthesized powder gives evidence for U-type hexagonal phase formation with space group of ‘R3m’. As per the literature from previous findings, no other phase was identified and all diffraction peaks consistently reveal the hexagonal structure. The PANalytical’s X’pert-Pro scanning tool has been used to identify the peaks under the angle 2θ in degree in the region from 20◦ to 60◦ . Further, XRD peaks were indexed and the lattice parameters (a & c) were obtained through formula (1) as given below; ) ( 2) ( 1 4 h2 + hk + k2 l = + 2 (1) d2 3 a2 c 3.2. Surface morphology The size and morphology of synthesized Ba4Co2Fe36O60 and γ Fe2O3 powder were characterized by field emission electron microscope (FESEM) in Fig. 2 (a & b) while, the surface and fractured morphology of lower to higher dispersion of γ Fe2O3 filler in Ba4Co2Fe36O60/γ Fe2O3epoxy composites shown in Fig. 2(c–e). These images depicts that there is uniform dispersion between fillers and epoxy matrix. The optimum value of Ba4Co2Fe36O60 particles size is less than 50 μm and grain size varies from 100 nm to 120 μm. The micrographs show that the absorbing filler materials have hexagonal platelet like morphology which is most suitable for radar absorbing purpose. Based on these initial findings, the proposed composites can be suitably used for the designing of electro­ magnetic interference shielding materials and radar absorbers [16–20]. According to EDS analysis of Fig. 3(a–e), the percentage of the chemical elements was closer to the estimated theoretical stoichiometry in U-type barium hexaferrites and gamma iron oxide also for the designed composites. For a comparison, in a recent study of filler ma­ terials and its composites studied through EDS detector, which unable to identified other elements. The characteristics EDS spectra of filler ma­ terials and its composites are shown in Fig. 3(a and b) and Fig. 3(c–e) respectively. Consequently, observed elemental composition ratio of metallic ions are consisting expected stoichiometry is well maintained Using the above formula (1), calculated values of lattice parameter are: a = 5.86 Å and c = 113.7 Å; these values are shown in the same range as previous reported in literatures for the U-type barium hex­ aferrite powder [15]. Although γ Fe2O3 powder shows cubic structure with almost equal lattice constant (0.834 nm) as shown in Fig. 1(b), which are due to the ordered occupancy of octahedral sites by Fe+3. The estimated cuboids shape enhances the shape anisotropy which results in the increased magnetic loss. Its XRD patterns are reproducible with the various ratios 4 V. Pratap et al. Solid State Sciences 113 (2021) 106553 Fig. 3. (continued). during synthesis process of material and designing composites. its composites have shown a narrow hysteresis loop. Definite combina­ tion of saturation magnetization (Ms) and low coercivity (Hc) are suit­ able for high frequency in gigahertz applications. It is observed that the saturation magnetization (Ms) value was increased from 49.32 to 55.49 emu/g of increasing the γ Fe2O3 contents in Ba4Co2Fe36O60/γ Fe2O3epoxy composites. The low coercivity of ≤153 Oe and low squareness ratio (Mr/Ms) ratio of ≤0.051, categorize the prepared Ba4Co2Fe36O60/γ Fe2O3-epoxy composites as soft ferrites based absorber. It can be noted that the densification of magnetic powders results in grain growth which evolves the multi domain particle regime. These multi domain natures of 3.3. Study of magnetic properties The magnetic properties of both, magnetic fillers and fabricated composites have been measured using vibrating sample magnetometer (VSM) under the applied magnetic field from − 18 kOe to +18 kOe. The γ Fe2O3 powder and its composites were characterized for its histogram and properties at room temperature as shown in Fig. 4 with values tabulated in Table 1. Synthesized Ba4Co2Fe36O60, γ Fe2O3 powder and 5 ­ V. Pratap et al. Solid State Sciences 113 (2021) 106553 optimized level for prepared series of Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. Here, we have been found a hysteresis loop and an arrangement of saturation magnetization with low coercive values suitable for gigahertz frequency applications. 4. Electromagnetic parameters and absorption phenomena Electromagnetic (EM) properties of prepared composites are gener­ ally characterized in terms of is functional parameters such as complex permittivity (ε′ -jε") and complex permeability (μ’-jμ"). These parameters can be tuned for desired microwave absorption when the incident EM wave interacts with the surface of absorbing materials. Absorbers are capable to absorb the incident radar/EM energy significantly and convert this energy into other forms (heat), which thermal imagers are unable to detect. When an incident EM wave fall on the absorber’s surface; attenuation, reflection and transmission of EM waves are three major phenomena take place, as shown in Fig. 5. The complex permit­ tivity (ε′ -jε") and complex permeability (μ’-jμ") parameters of composite specimen have been computed from the measured scattering parameters using Agilent VNA E8364B in the 2–18 GHz frequency range. The real parts of complex permittivity and complex permeability (ε′ and μ’) represents the storage of electric and magnetic energy respectively. Whereas, the imaginary parts of complex permittivity and imaginary parts of complex permeability (ε" and μ") are responsible for the lossy manners corresponding to dielectric and magnetic energy respectively. Fig. 4. Magnetic hysteresis loop of (a) γ Fe2O3 as maghemite powder, (b) 30 wt % and (c) 50 wt % dispersion of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3 -epoxy composites. Table 1 Magnetic properties of synthesized U-type hexaferrite [14], γ Fe2O3 powder and prepared composites for lower (30 wt %) and higher (50 wt %) dispersion of γ Fe2O3 in Ba4Co2Fe36O60/γ-Fe2O3-epoxy composites. System Magnetization; Ms (emu/g) Coercivity; Hc (Oe) Remanence; Mr (emu/g) Squareness ratio; Mr/Ms Ba4Co2Fe36O60 powder γ Fe2O3 powder 50:30 wt % of ferrite and γ Fe2O3 in composite 30:50 wt % of ferrite and γ Fe2O3 in composite 55.81 107.31 2.17 0.038 [15] 74.70 49.32 243.09 96.34 4.09 1.591 0.054 0.032 55.49 153.84 2.872 0.051 4.1. Complex permittivity Fig. 6(a, b and c) shows the real and imaginary values of permittivity for fabricated Ba4Co2Fe36O60/γ Fe2O3 epoxy composites with respect to the variation in filler content. It can be observed that the values of real permittivity increases as the filler content of γ Fe2O3 in the composites has been increased from 30 wt % to 50 wt % with constant wt. % of epoxy matrix. It is obvious from the corresponding figure that all the composites show almost constant values of real permittivity through the whole frequency region for particular filler content. The increase of real permittivity with the high loading of γ Fe2O3 can be interpreted by the hopping mechanism which is established for electric polarization and dielectric loss, increases with maximum wt. % of filler materials. The maximum value achieved of real permittivity (ε′ ) achieved 4.23 for higher dispersion (30:50 ratio of U-ferrite and γ Fe2O3) of γ Fe2O3 in prepared Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. The imaginary part of complex permittivity or dielectric loss factors (ε′′ ) is also constant throughout the 2–18 GHz frequency region for an individual loading. The increase of dielectric constant at lower frequencies is remarkable. Such types of frequency dependent dielectric constants have improved loss mechanism of electrical energy inside the Ba4Co2Fe36O60/γ Fe2O3epoxy composites. This is because γ Fe2O3 nano-particle having the greater surface to volume ratio than Ba4Co2Fe36O60 particles and sub­ sequently, high dielectric permittivity. These phenomena could be attributed to the inhomogeneity of used magnetic absorbing (micro and nano) materials. In case of Ba4Co2Fe36O60/γ Fe2O3-polymer composites, the contribution to real permittivity (ε′ ) and imaginary permittivity (ε′′ ) rise to heterogeneity due to interfacial polarization and interfacial relaxation as the electric charge particles are separated by insulating matrix grains which enhanced heterogeneity. The resonance peak at 6.2 GHz frequency is preliminary attributed to the dipole-dipole interaction as well as interfacial polarization by adding the γ Fe2O3 content [14,21, 22]. The dielectric constant and relaxation parameters of filler disper­ sion are changed with the gradual transformation between Ba4Co2 Fe36O60 and γ Fe2O3. However, as γ Fe2O3 increases in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites from 30 wt % to 50 wt %, high and smooth complex permittivity curves {Fig. 6(a, b and c)} are obtained and no further peak is observed above 13.2 GHz frequency. Fig. 5. Schematic diagram of designed toroidal shape composites for absorp­ tion mechanism. the magnetic fillers are responsible for a lowered coercivity value of fabricated Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. It can be observed that, increasing the γ Fe2O3 content depicts the increased values of saturation magnetization (Ms) and coercivity (Hc) at 6 V. Pratap et al. Solid State Sciences 113 (2021) 106553 Fig. 6. Frequency response of the complex permittivity for different loading; (a) 30 wt %, (b) 40 wt % and (c) 50 wt % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3epoxy composites. 4.2. Complex permeability frequencies. It is to be noted, that the electromagnetic properties of the fabricated composites depends upon the fillers contents of hexagonal ferrite obeying with the ferromagnetic materials which creates vacuum phenomena such as eddy current effect, natural and exchange resonance rather than magnetic permeability and space charge polarization [19, 23]. Fig. 7(a, b and c) represents the frequency versus complex perme­ ability (μ’- jμ") characteristics of fabricated Ba4Co2Fe36O60/γ Fe2O3 composites in the frequency range of 2–18 GHz. The aim of incorpo­ rating Ba4Co2Fe36O60/γ Fe2O3 into the epoxy matrix is to increases real permeability value above the unity and to increase the magnetic loss in the working frequency region. It can be observed from Fig. 7(a) that real permeability for 30 wt % of γ Fe2O3 loaded composite decreases sharply from 2 to 6.4 GHz, further remains at constant value in the frequency range of 6.4–18 GHz. The highest value of real part of complex perme­ ability is observed in the range of 1.73–0.72, whereas its imaginary part varies in the range of 0.72–0.24 across the entire 2–18 GHz frequency. Fig. 7(b) shows that for the real permeability for 40 wt % of γ Fe2O3 loaded composite is in the range of 1.63–0.82, whereas its imaginary part is in the range of 0.71–0.09. High (50 wt %) filler concentration of γ Fe2O3 in designed composite as depicted in Fig. 7(c), the real part of permeability increased substantially in the range of 2.06–0.85 between the frequency ranges from 2 to 5.02 GHz, whereas magnetic loss factor (μ") is in the range of 1.5–0.085 in the whole frequency range of 2–18 GHz. The dispersion of γ Fe2O3 nano-particles minimize the eddy current of designed composites due to small size than skin depth, which in turns is optimize the electromagnetic parameters. The optimized complex permeability is present in Ba4Co2Fe36O60/γ Fe2O3-epoxy polymeric composites; which gives rise to the circumferential demagnetizing field as a result, diminishes the real permeability (μ′ ) at resonance 4.3. Loss tangent Fig. 8(a and b) shows the nonlinear deviation of the dielectric tangent loss (tanδe = ε"/ε′ ) and magnetic tangent loss (tanδμ = μ"/μ’) with frequency. In Fig. 8(a), at starting frequency of 2.0 GHz, the nu­ merical value of dielectric tangent loss (0.023) remains almost same up to 9.8 GHz for all wt. % of γ Fe2O3 dispersion in Ba4Co2Fe36O60/γ Fe2O3 polymer composite. However, this value is obtained greater than 0.03 for 30, 40 and 50 wt % loaded in Ba4Co2Fe36O60/γ Fe2O3-epoxy com­ posites. Maximum value of tanδe achieved was 0.34 for 50 wt % dispersed γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites at the corresponding frequency of 10.2–11.9 GHz. In Fig. 8(b), at starting frequency of 2–8 GHz, the numerical value of magnetic tangent loss increases to 1.2 for 50 wt % dispersed γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. Further the value of magnetic tangent loss (tanδμ) was found to be decreasing sharply for all prepared composites in the frequency range of 8.0–18 GHz. It can be observed from the corresponding figure that highest value of tanδμ; 1.2 for 50 wt % was greater than 0.68 & 5.6 for 30 wt % & 40 wt % loaded γ Fe2O3 in 7 V. Pratap et al. Solid State Sciences 113 (2021) 106553 Fig. 7. Frequency response of the complex permeability for different loading; (a) 30 wt %, (b) 40 wt % and (c) 50 wt % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3epoxy composites. Fig. 8. Frequency response of dielectric loss tangent (a) and magnetic loss tangent (b) of Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. The prepared composites are the heterogeneous combination of conducting/magnetic particles in the insulated epoxy grains. Further the complex permittivity and complex permeability are mainly attributed to the amount of dielectric polari­ zation and magnetic polarization for the prepared composites. The well dispersion of hexaferrite (Ba4Co2Fe36O60) and maghemite (γ Fe2O3) in epoxy matrix induces the mobility of charge carriers and spin of elec­ trons that produce polarization and magnetization respectively. As a result of this, the governing polarization and magnetization with the loss mechanism comprise the association of relaxation and resonance 8 V. Pratap et al. Solid State Sciences 113 (2021) 106553 layer absorber by using the following equation (2) proposed by Naito and Suetake [24]: [ ] z− 1 (2) RL(dB) = − 20log 10 z+1 The ratio of material’s impedance (Zin) to impedance of free space (Zo) is accepted as normalized impedance (Z) calculated through following equation (3). √̅̅̅̅̅̅̅̅̅̅̅ { ( )̅ }√̅̅̅̅̅̅̅̅̅̅̅̅ zin μr − j2πf .d where, z = = tanh (3) (μr εr ) c zo εr In the above expression RL is the reflection loss represented in √̅̅̅̅̅̅̅ decibel (dB), j is an imaginary unit for the value of − 1, μr and εr are the complex permeability and complex permittivity respectively, f is the frequency of the incident EM wave, c is speed of light in free space and d being thickness of the composite specimens. Fig. 9(a, b and c) shows the calculated reflection loss for fabricated Ba4Co2Fe36O60/γ Fe2O3-epoxy composites as a function of thickness in the frequency range of 2–18 GHz. These results are analyzed by metal backing model as proposed by Naito and Suetake. RL has been calcu­ lated for various thicknesses (2.6, 2.9 and 3.2 mm) of fabricated com­ posites through a MATLAB codes. Consequently, dip of RL gets shifted towards the lower frequency region by increasing the absorbers thick­ ness from 2.6 to 3.2 mm. The impedance matching condition can be justified to the microwave absorption mechanism. RL performance for 30 wt % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composite shows that the minimum RL (Maximum Absorption) of − 8.86 dB, − 10.36 dB and − 11.86 dB have been observed corresponding to matching fre­ quency of 6.48 GHz, 5.84 GHz and 4.88 GHz respectively. Fig. 9 (b) depict RL performance for 40 wt % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composite at 4.7 GHz has been observed from the corre­ sponding graphs that the minimum reflection minima of − 10.02 dB, − 13.82 dB and − 14.8 dB have been observed corresponding to match­ ing frequency of 13.3 GHz, 13.0 GHz and 12.3 GHz respectively. It can be also observed from the corresponding graphs that the 10 dB ab­ sorption bandwidth (11.7–13.3 GHz) has improved substantially by adding equal wt. % of γ Fe2O3 and Ba4Co2Fe36O60 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. Similarly Fig. 9 (c) shows the variation of RL performance for 50 wt % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composite, it can be analyzed from corresponding figure that the mini­ mum reflection loss of − 13.89 dB, − 15.39 dB and − 19.89 dB have been observed corresponding matching thickness 14.5 mm, 13.8 mm and 13.2 mm respectively. The optimum performance in RLmin as compared to maximum bandwidth 4.8 GHz (RL ≤ − 10 dB) was observed for the absorber having composite thickness of 3.2 mm (RLmin ≤ − 19.89 dB implies 98.9% absorption). Consequently, Ba4Co2Fe36O60/γ Fe2O3 loaded absorbers with maximum (50 wt % of γ Fe2O3) content can be used as effective microwave absorbers for the X-band and Ku-band fre­ quency region. Fig. 9. (a, b and c) calculated reflection loss of different percentage loading; (a) 30 wt %, (b) 40 wt % and (c) 50 wt % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3epoxy composites. 5. Conclusions In summary, U-type barium hexaferrite (Ba4Co2Fe36O60) powder was synthesized based on solid state reaction route, the polycrystalline phase of synthesized powder was validated using XRD technique. The surface morphology and elemental composition of used absorbing powder and composites were scanned together with the elemental attachment available with the FESEM. Further, radar absorbers were fabricated through wet mixing method based on various wt. % of magnetic filler contents. The magnetic properties were also studied for the composites with increasing wt. % of γ Fe2O3 in Ba4Co2Fe36O60/γ Fe2O3-epoxy composites. The intrinsic electromagnetic parameters of prepared polymeric composites were significantly improved with increasing the wt. % of γ Fe2O3. It is found that the matching frequency of prepared absorbing sample shifted towards the lower frequency band with phenomena which are subsequently responsible for increasing the dielectric tangent loss and magnetic tangent loss governing the ab­ sorption phenomena. 4.4. Reflection loss The microwave absorption which is quantified in terms of reflection loss (RL) can be estimated from measured value of complex permittivity and complex permeability of fabricated Ba4Co2Fe36O60/γ Fe2O3-epoxy composites using metal backed coaxial line measurement technique using the transmission line approach. It can be measured as the single 9 V. Pratap et al. Solid State Sciences 113 (2021) 106553 increasing the thickness of absorbers. The minimum RL was observed as − 19.89 dB for designed absorber having the thickness of 3.2 mm (RLmin ≤ − 19.89 dB implies 98.8% absorption) corresponding its matching frequency 13.2 GHz. The optimized absorber with highest loading in wt. % of γ Fe2O3 nano powder in designed composites seems strong candi­ date as radar absorber and in high frequency devices for stealth applications. [7] R.S. Meena, S. Bhattacharya, R. Chatterjee, Complex permittivity, permeability and microwave absorbing studies of (Co2− xMnx) U-type hexaferrite for X-band (8.212.4 GHz) frequencies, Mater. Sci. Eng. B 171 (2010) 133–138. [8] D. Lisjak, V.B. Bregar, M. Drofenik, The influence of microstructure on the microwave absorption of Co–U hexaferrites, J. Magn. Magn Mater. 310 (2007) 2558–2560. [9] S.M. Abbas, A.K. Dixit, R. Chatterjee, T.C. Goel, Complex permittivity, complex permeability and microwave absorption properties of ferrite-polymer composites, J. Magn. Magn Mater. 309 (2007) 20–24. [10] C.R.K. Mohan, P.K. Bajpai, Effect of sintering optimization on the electrical properties of bulk BaxSr1-xTiO3 ceramics, Physica B 403 (2008) 2173–2188. [11] H. Bayrakdar, Electromagnetic propagation and absorbing property of ferrite polymer nanocomposite structure, Prog. Electromag. Res. Mat. 25 (2012) 269–281. [12] K. Singh, A. Ohlan, P. Saini, S.K. Dhawan, Poly (3,4-ethylenedioythiophene) γ Fe2O3 polymer composite-super paramagnetic behavior and variable range hooping 1D conduction mechanism-synthesis, Poly, Adv. Tech. 19 (2008) 229–236. [13] R.S. Meena, S. Bhattacharya, R. Chatterjee, Development of “tuned microwave absorbers” using U-type hexaferrite, Mater. Des. 31 (2010) 3220–3226. [14] V. Pratap, A.K. Soni, A.M. Siddiqui, S.M. Abbas, R. Katiyar, N.E. Prasad, Dielectric and radar absorbing properties of exfoliated graphite dispersed epoxy composites, J. Electron. Mater. 49 (2020) 3972–3981. [15] V. Pratap, A.K. Soni, S. Dayal, S.M. Abbas, A.M. Siddiqui, N.E. Prasad, Electromagnetic and absorption properties of U-type barium hexaferrite epoxy composites, J. Magn. Magn Mater. 465 (2018) 540–545. [16] S.R. Shannigrahi, W.Q. Au, V. Suresh Kumar, L. Liu, Z.H. Yang, C. Cheng, C.K. I. Tan, R.V. Ramanujan, Synthesis and electromagnetic properties of U-type hexaferrites Ba4B2Fe36O60 (B: Co, Ni, Cu), J. Magn. Magn Mater. 325 (2013) 63–68. [17] R. Dosoudil, M. Usakova, J. Franek, J. Slama, V. Olah, RF electromagnetic wave absorbing properties of ferrite polymer composite materials, J. Magn. Magn Mater. 304 (2006) e755–e757. [18] P. Singh, V.K. Babbar, A. Razdan, R.K. Puri, T.C. Goel, Complex permittivity, permeability, and X-band microwave absorption of CaCoTi ferrite composites, J. Appl. Phys. 87 (2000) 4362–4366. [19] S.M. Abbas, A.K. Dixit, R. Chatterjee, T.C. Goel, Complex permittivity, complex permeability and microwave absorption properties of ferrite-polymer composites, J. Magn. Magn Mater. 309 (2007) 20–24. [20] S.M. Abbas, R. Chatterjee, A.K. Dixit, A.V.R. Kumar, T.C. Goel, Electromagnetic and microwave absorption properties of (Co2+-Si4+) substituted barium hexaferrites and its polymer composite, J. Appl. Phys. 101 (2007), 074105. [21] V. Pratap, A.K. Soni, S.M. Abbas, A.M. Siddiqui, N.E. Prasad, J. Alloys Compd. (2021), https://doi.org/10.1016/j.jallcom.2020.158280. [22] J. Yacubowicz, M. Narkis, Dielectric properties of medium thermal blackpolyethylene systems, Polym. Eng. Sci. 28 (1988) 1581–1585. [23] S.S. Kim, S.T. Kim, Y.C. Yoon, K.S. Lee, Magnetic, dielectric, and microwave absorbing properties of iron particles dispersed in rubber matrix in gigahertz frequencies, J. Appl. Phys. 97 (2005) 10F905 1–3. [24] Y. Naito, K. Suetake, Application of ferrite to electromagnetic wave absorber and its characteristics, IEEE Trans. Microw. Theor. Tech. 19 (1971) 65–72. Credit author’s contribution statement Vivek Pratap: Conceptualization, Design of study, Analytic and interpretation of data, Writing review and editing investigation, Writing – original draft preparation. Amit K. Soni: Validation, Investigation, Formal analysis. Himangshu B. Baskey: Validation, Formal analysis. S. M. Abbas: Methodology, Formal analysis, Supervision. A. M. Siddiqui: Formal analysis, Supervision. N. Eswara Prasad: Resources, Formal analysis. Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. References [1] S.E.M. Ghahfarokhi, M. Ahmadi, I. Kazeminezhad, Fabrication of the SrFe11MnO19/CoFe1.9Bi0.1O4 ferrite nanocomposites and investigation the properties of its microwave absorption in X-band, Phys. B Condens. Matter 594 (2020) 412290. [2] R. Jaiswal, K. Agarwal, V. Pratap, A. Soni, S. Kumar, K. Mukhopadhyay, N. E. Prasad, Microwave-assisted preparation of magnetic ternary core-shell nanofiller (CoFe2O4/rGO/SiO2) and their epoxy nanocomposite for microwave absorption properties, Mater. Sci. Eng. B 262 (2020) 114711. [3] F.M. Idris, M.H. Hashim, Z. Abbas, I. Ismail, R. Nazlan, I.R. Ibrahim, Recent developments of smart electromagnetic absorbers based polymer-composites at gigahertz frequencies, J. Magn. Magn Mater. 405 (2016) 197–208. [4] P.J. Liu, Z.J. Yao, V.M.H. Ng, J.T. Zhou, Z.H. Yang, L.B. Kong, Enhanced microwave absorption properties of double layer absorbers based on spherical NiO and Co0.2Ni0.4Zn0.4Fe2O4 ferrite composites, Acta Metall. Sin. 31 (2018) 171–179. [5] H.E. Horng, C.Y. Hong, S.Y. Yang, H.C. Yang, Novel properties and applications in magnetic fluids, J. Phys. Chem. Solid. 62 (2001) 1749–1764. [6] D.M. Pozar, Microwave Engineering, John Wiley & Sons, New York, 2004. 10