Co-Ni ferrite is one of the crucial materials for the electronic industry. A partial substitution with a rare-earth metal brings about modification in crystal lattice and broadens knowledge in the discovery of new magnetic material. Current work reports a Ga3+ substitution in the Co-Ni ferrite with composition Co0.5Ni0.5Fe2−xGaxO4 (where x = 0.0, 0.2, 0.4, 0.6, 0.8, and 1.0), herein referred to as spinel ferrite microspheres (CoNiGa-SFMCs). The samples were crystallized hydrothermally showing a hollow sphere morphology. The crystal phase, magnetic, morphology, and optical behaviour were examined using various microscopy and spectroscopic tools. While the XRD confirmed the phase of SFMCs, the crystallite size varied between 9 and 12 nm. The Tauc plot obtained from DRS (diffuse reflectance spectroscopy) shows the direct optical energy bandgap (Eg) of the products, with the pristine reading having the value of 1.41 eV Eg; the band gap increased almost linearly up to 1.62 eV along with rising the Ga3+ amount. The magnetic features, on the other hand, indicated the decrease in coercivity (Hc) as more Ga3+ is introduced. Moreover, there was a gradual increase in both saturation magnetization (Ms) and magnetic moment () with increasing amount of Ga3+ till x = 0.6 and then a progressive decline with increases in the x content; this was ascribed to the spin-glass-like behavior at low temperatures. It was detected that magnetic properties correlate well with crystallite/particle size, cation distribution, and anisotropy.
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