Temperature Dependent Magnetic and Structural Properties of Al Substituted Nanostructured Ferrites with Large Coercive Fields

Abstract

We report a comprehensive study of the temperature-dependent structural, magnetic, vibrational, and dielectric properties of Al-substituted M-type hexaferrites SrFe$_{12-x}$Al$_x$O$_{19}$. Neutron powder diffraction and M\"ossbauer spectrometry show that Al$^{3+}$ preferentially replaces Fe$^{3+}$ at spin-up octahedral sites (2a, 12k), disrupting the exchange coupling with the spin-down 4f tetrahedral sites and leading to a progressive reduction of site-specific magnetic moments and a systematic decrease in the Curie temperature, supported by temperature dependent susceptibility measurements. Raman spectroscopy reveals pronounced phonon anomalies near $T_C$, particularly in modes associated with bipyramidal Fe-O vibrations, reflecting the weakening of both 4e-12k and 4e-4f exchange pathways. However, the coercive field exhibits a dramatic increase, reaching $\mu_0H_C$ $\sim$ 1.2 T for SrFe$_{9.6}$Al$_{2.4}$O$_{19}$, among the largest values reported for this class. Susceptibility measurements suggest that Al substitution, while weakening the superexchange network, contributes to the stabilization of single-domain behavior.