Gallium substituted Z-type hexagonal ferrites with chemical composition Sr3Co2-xGaxFe24O41 (x = 0.0,0.4, 0.8, 1.2, 1.6, and 2.0) were successfully synthesised in air at 1200 °C for 5 h using the sol-gel auto-combustion technique, in order to investigate the effect of gallium substitution on structural, magnetic and dielectric properties. X-ray Diffraction (XRD) analysis of all samples reveals the formation of mixed hexaferrite phases, with Z ferrite as the major phase (72–90%).The average crystallite size of heated powders was found to be in the range of 21–40 nm. The saturation magnetisation decreases after gallium substitution, with the lowest values of 64 Am2 kg−1 for composition x = 1.6, which also hasthe highest value of coercivity (28.3 kA m−1). Nevertheless, all were soft ferrites, with Hc between 3.4 and 28.3 kA m−1.The Mr/MS ratio of all samples was found to be less than 0.5, suggesting that all the compositions possess multi-domain microstructures. Mössbauer spectroscopic analysis confirmed that the Fe ions were found in the 3 + high spin state for compositions below x ≤ 0.4, whereas ∼1.5% of the Fe ions were converted into Fe2+ high spin state beyond x ≥ 0.8 compositions, as Ga3+ began to substitute for Fe3+, forming Fe2+ in the cobalt positions. The average hyperfine magnetic field (<Hhf>) was found to be decreased with Ga-substitution. Dielectric parameters such as dielectric constant and loss factor were studied as a function of frequency, and their results show normal behaviour for ferrimagnetic materials. In complex measurements at microwave frequencies (8 GHz–12.5 GHz, the X-band), all samples had a real permittivity of around 8–14. For sample x = 2.0, a dielectric resonance peak was observed around 12.15 GHz. All showed a real permeability of around 1.0–1.4 over the frequency of 8 GHz–12.5 GHz range, and ferromagnetic resonance (FMR) was observed in x = 0.0 and 2.0 samples, at around 11 and 12 GHz, respectively. This suggests that the prepared samples can be used as microwave absorbers/EMI shielding at specific microwave frequencies. The co-existence of FMR and dielectric resonance at the same frequency of 12.15 GHz for x = 2.0 could lead to the coupling of these resonances and the development of potential metamaterials.
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