Co-existence of tetragonal and monoclinic phases and multiferroic properties for x ⩽ 0.30 in the (1 − x)Pb(Zr0.52Ti0.48)O3–(x)BiFeO3 system

• Synthesis of (1 − x)PbZr0.52Ti0.48O3–(x)BiFeO3 with x ⩽ 0.30 by sol–gel method.
• Structural phase transformation with x has been revealed by Rietveld analysis.
• Raman analysis supports structural phase transition.
• Occurrence of MC is a strong evidence of magneto-electric coupling.
• Enhance magnetization is obtained in the dominant monoclinic phase for x ⩾0.15.

Compositions with x ⩽ 0.30 in the system (1 − x)Pb(Zr0.52Ti0.48)O3–(x)BiFeO3 were synthesized by sol–gel method. Rietveld analysis of X-ray diffraction data reveals tetragonal structure (P4mm) for x ⩽ 0.05 and monoclinic (Cm) phase along with the existence of tetragonal phase for 0.10 ⩽ x ⩽ 0.25 and monoclinic phase for x = 0.30. Transformation of E(2TO) and E + B1 vibrational modes in the range 210–250 cm−1 (present for x ⩽ 0.25) into A′ + A″ modes at ∼236 cm−1 for x = 0.30, and occurrence of new vibrational modes A′ and A″ in Raman spectra for x ⩾ 0.10 unambiguously support the presence of monoclinic phase. Occurrence of remnant polarisation and enhanced magnetization with concentration of BiFeO3 indicates superior multiferroic properties. Variation of magneto-capacitance with applied magnetic field is a strong evidence of magneto-electric multiferroic coupling in these materials.