Giant room-temperature magnetodielectric coupling in spark plasma sintered brownmillerite ceramics
The dielectric, magnetic, and magnetodielectric properties of Ca{sub 2}FeAO{sub 5+δ} (A = Al, Ga) ceramics were investigated together with their crystal structures. Rietveld refinement of the X-ray diffraction data indicated that the space group of the Ca{sub 2}FeAlO{sub 5+δ} ceramic was Ibm2, whereas that of the Ca{sub 2}FeGaO{sub 5+δ} ceramic was Pcmn. Dielectric relaxation above room temperature, originating from the Maxwell–Wagner effect and polaronic hole hopping between Fe{sup 3+} and Fe{sup 4+} ions, was observed in both ceramics. Weak ferrimagnetic behavior was identified from the magnetic-field-dependent magnetization in these ceramics, which was attributed to the non-cancelled spins of the antiferromagnetic-ordered Fe{sup 3+} and Fe{sup 4+} ions. An intrinsic, giant, room-temperature magnetodielectric coefficient of up to −23.3% was achieved in the Ca{sub 2}FeAlO{sub 5+δ} ceramic at 50 MHz, which was attributed to the suppression of charge fluctuations of Fe{sup 3+} and Fe{sup 4+} ions in the magnetic field.