Above room temperature multiferroic and magnetoelectric properties of (1‐Φ) PZTFT‐Φ CZFMO particulate composites

Abstract Magnetoelectric (ME) composites of suitable ferroelectric and magnetic materials can display elevated magnetic and ferroelectric operational temperatures, along with substantial ME coupling, compared to conventional single‐phase multiferroics. Herein, we describe the synthesis of (1‐Φ) PZTFT‐Φ CZFMO, Φ = 0.1, 0.2, 0.3 (PZTFT: [0.6(PbZr 0.53 Ti 0.47 O 3 )–0.4(PbFe 0.5 Ta 0.5 )O 3 ] CZFMO: Co 0.6 Zn 0.4 Fe 1.7 Mn 0.3 O 4 )] particulate (0–3) composites and report on the magnetic as well as ferroelectric phase transitions and magnetoelectric coupling. The phase formation and the induced strain in these composites are investigated via Raman spectroscopy. A large bifurcation of the zero‐field cooled‐field cooled magnetization curves confirms the highly anisotropic behavior of the composites. These curves also identify spin glass behavior in the CZFMO phase at ≈230 K. The magnetic phase transition of the composite (Φ = 0.2) is reported to be ≈532 (± 10) K. The temperature dependent dielectric data displays the ferroelectric phase transitions from the PZTFT phase and the broad relaxation peak from the CZFMO phase. The quadratic relationship between the magneto‐capacitance and the magnetization confirms the existence of biquadratic magnetoelectric coupling in the systems. The collective results are consistent with the presence of a direct magneto‐electric effect in the composites, i.e., by the application of magnetic field, the magnetic phase is strained, and this induced strain is responsible for changes of ferroelectric order parameter in the piezoelectric phase. This attribute makes the current composite structure a promising candidate for multiferroic data storage and processing technologies.