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In this work, we have prepared intergrowth of multiferroic compounds namely Bi4RTi3Fe0.7Co0.3O15-Bi3RTi2Fe0.7Co0.3O12−δ (BRTFCO15-BRTFCO12) (rare earth (R) = Dy, Sm, La) by solid-state reaction method. From the X-ray diffraction Rietveld refinement, the structure of the intergrowths was found to be orthorhombic in which satisfactory fittings establish the existence of three-layered (space group: b 2 c b) and four-layered compounds (space group: A21am). Analysis of magnetic measurements confirmed a larger magnetization for theSm-modified intergrowth compound (BSTFCO15-BSTFCO12) compared to Dy- and La-doped ones. The emergence of higher magnetic properties can be due to distortion in the unit cell when some Bi3+ ions are replaced with the Sm3+, bonding of Fe3+-O-Co3+ as well as a possible mixture of FexCoy-type nanoparticles that are formed generally in the synthesis of intergrowths. The changes in the magnetic state of the Aurivillius intergrowths have been reflected in the magnetoelectric (ME) coupling: higher ME coefficient (~30 mV/Cm-Oe) at lower magnetic fields and is constant up to 3 kOe. The results were corroborated by Raman spectroscopy and variation of temperature with magnetization data. The results revealed that the RE-modified intergrowth route is an effective preparative method for higher-layer Aurivillius multiferroic ceramics.

Development of lead-free BaTiO3/NiFe2O4/BaTiO3 (BTO/NFO/BTO) trilayer structure thin films is significant for the realization of eco-friendly and implantable microelectromechanical systems (MEMS)-based devices. In the present work, we report BTO/NFO/BTO trilayer structure as a representative ferroelectric/ferromagnetic/ferroelectric (FE/FM/FE) system deposited on Pt(111)/TiO2/SiO2/Si using Pulsed Laser Deposition (PLD) technique. We report the ferroelectric, magnetic, and ME properties of BTO/NFO/BTO trilayer nanoscale heterostructure having dimensions 140/80/140 nm, at room temperature. High room temperature dielectric constant ~2145 at 100 Hz with low dielectric loss ~0.05 at 1 MHz is observed. Further, the deposited (BTO/NFO/BTO) tri-layered thin films showed magnetoelectric, multiferroic behavior with remanent polarization of 8.63 μCcm−2 at about 0.25 MV/cm and a reasonably high saturation magnetization of ~16 emu/cm3 at ~10 kOe is witnessed at room temperature. Tri-layered films have shown interesting magnetoelectric (ME) coupling coefficient (αE) ~54.5 mV/cm Oe at room temperature.