Lead palladium zirconate titanate: A room temperature nanoscale multiferroic thin film

Abstract

The discovery of single-phase multiferroic materials and the understanding of intriguing physics of the coupling mechanisms between their spin and polarization are important for the next generation of multifunctional devices. In this work, we report dielectric, ferroelectric, and magnetization results of Pd-substituted room-temperature magnetoelectric multiferroic Pb(Zr0.20Ti0.80)0.7Pd0.3O3 (PZTPd) thin films. Highly c axis oriented PZTPd thin films were grown on {(LaAlO3)0.3(Sr2AlTaO6)0.7} substrates using the pulsed laser deposition technique. These films were phase pure and stabilized in a tetragonal phase. Atomic force microscopic studies indicated a homogeneous distribution of grains on the films' surface with a surface roughness (RQ) of ∼5.4 nm. A large dielectric constant of ∼1780 and a low loss tangent value of ∼0.52 were observed at 1 kHz measured at room temperature. Temperature dependent dielectric studies on Pt/PZTPd/La0.7Sr0.3MnO3 metal–insulator–metal heterostructure capacitors between 80 and 660 K indicated a diffused ferroelectric to paraelectric phase transition around 515 K. The polarization hysteresis loops observed at room temperature were attributed to its ferroelectric behavior. Saturated magnetization hysteresis loop with remanent magnetization of 1.54 emu/cm3 was obtained at room temperature. Ferromagnetic ordering in thin films was found to sustain in the entire temperature range from 5 to 395 K, as revealed from the constant behavior of the dM/dT curve with temperature. The mixed oxidation states of palladium (Pd2+/Pd4+) dispersed in the polar Pb(Zr0.20Ti0.80)O3 matrix were revealed from our high resolution x-ray photoelectron spectroscopic studies and is ascribed to the origin of ferromagnetic ordering in the film. These findings suggest that PZTPd thin films are multiferroic (ferroelectric–ferromagnetic) at room temperature.