Abstract

The multiferroic Y-type hexaferrites BaxSr2−xMe2Fe12−yAlyO22 (Me = Zn2+, Co2+, Mg2+, etc.) have attracted much attention due to their giant magnetoelectric (ME) effect up to room temperature and low modulated magnetic field by the chemical doping control of the complex magnetic phases. However, the research of substitution between the Me ions is rare. As doping at the Me ion site can combine the advantages of both, e.g., higher magnetic ordering temperature in Co2 and stronger ME coefficient in Mg2 Y-type hexaferrites, herein, we report the stability and switching of magnetoelectric states in the Y-type hexaferrites Ba0.5Sr1.5CoMgFe11AlO22 single crystals. Our results demonstrate that substituting half of the Mg2+ with Co2+ enhances the transition temperature of the alternating longitudinal conical phase to proper screw spin order up to room temperature compared to those Mg2 Y-type hexaferrites. Simultaneous occurrence of in-plane and out-of-plane ferroelectric polarization is observed, alongside comparable spontaneous magnetization. It was found that the in-plane spin-driven polarization can be reversible below 50 K with a substantial ME coefficient α = −8000 ps/m but becomes irreversible at 100 K. This reversal in the sign of the ME coefficient signifies the transition between two distinct ME states at high temperature. The reversibility and irreversibility of spin-induced polarization are discussed within the framework of free energy based on the ferroelectric phase, which prevail in numerous Y-type hexaferrites. Our results provide insights into understanding the role of the Me ions in the magnetoelectric coupling in Y-type hexaferrites.

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