Ultralarge polarization in ferroelectric hafnia-based thin films

Abstract: Hafnia-based ferroelectrics have become a valuable class of electronic functional materials at the nanoscale, showing great potential for next-generation memory and logic devices. However, more robust ferroelectric properties and better understanding of the polarization mechanisms are currently needed both in technology and science. Herein, we report the properties of oxygen-deficient Hf0.5Zr0.5O2 films with ultralarge remanent polarization (Pr) of 387 uC cm-2 at room temperature (1 kHz). Structure characterizations identify a new ferroelectric monoclinic Pc phase in these Hf0.5Zr0.5O2 films. The in-situ STEM measurements evidence polar displacements of the oxygen atoms, which move up and down in the Pc structure under applied DC bias fields, showing a huge displacement (1.6 A). DFT calculations optimized the Pc structure and also predicted a large polarization. The coexistence of the ferroelectric monoclinic (Pc) phases and orthorhombic (Pca21) is responsible for this superior ferroelectric properties. These findings are promising for hafnia-based ferroelectric applications in integrated ferroelectric devices, energy harvesting and actuators, etc.