We report a detailed study on the electronic structure and temperature (1.9K≤T≤900K) dependence of magnetization in Zn diluted cuprospinel [Cu1−xZnxFe2O4 (0≤x≤0.6)]. The electronic structure determined from the x-ray photoelectron spectroscopy and Rietveld analysis of the x-ray diffraction patterns reveals the structure to be (Cu(1−x)/5ZnxFe4(1−x)/5)A [Cu4(1−x)/5Fe2−4(1−x)/5]BO4. Beyond a specific dilution limit (0.05≤xp≤0.1), a sudden phase-change from tetragonal (I41/amd) to cubic (Fd3m) is noticed with an alteration in the A–O–A (3.29%) bond angle and A–O bond length (0.67%). Our analysis shows that all these compounds order ferrimagnetically below the Néel temperature (TFN) due to dissimilar site-specific magnitudes of spins, yet, they undergo a second transition at low temperatures T1∼66K with asymptotic Curie temperature TA(=C/χ0) as high as −547.2K for the undoped case. Dilution with Zn cause quadratic decay (b2x2+b1x+yo) of the ferrimagnetic ordering temperature from 743 K to 370.5 K for x=0 and 0.6, respectively. On the contrary, a significant increase in the saturation magnetization (MS) was observed with increasing x until the critical composition xc∼0.4 beyond which MS decreases continuously (MS=1.64μB and 4.73μB for x=0 and 0.4, respectively). From the temperature dependence of inverse paramagnetic susceptibility [χ−1(T>TFN)] data and Néel’s expression for ferrimagnets, we evaluated the molecular field constants and exchange interactions (J) between the tetrahedral A- and octahedral B-sites. A systematic compositional dependence of this analysis yields that JAB (∼25kB for x=0) is the dominant exchange interaction in comparison to JBB and JAA; however, JAB decreases significantly with increasing the composition (JAB∼−5.5kB for x=0.6). The isothermal magnetization data and law of approach to saturation analysis reveals that the investigated system possesses very high anisotropy field HK ≥5.5kOe with cubic anisotropy constant K1≥1.6×106erg/cc at xc.
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