DOI: 10.1021/acsaelm.6c01341 ISSN: 2637-6113

High Energy-Storage Density in Ferroelectric La:HfO2-Based Thin-Film Capacitors

Nuno Estrócio, Wenjing Dong, Ampattu R. Jayakrishnan, Marian C. Istrate, Corneliu Ghica, Luís Marques, Ignasi Fina, Florencio Sánchez, José P. B. Silva

Abstract

Ferroelectric and antiferroelectric hafnium and zirconium oxides have attracted considerable attention for the development of next-generation energy-storage capacitors owing to their high energy-storage density (ESD), high power density, moderately high efficiency (η), and scalability down to the ultrathin limit. Most research on dielectric energy-storage capacitors focuses on antiferroelectric hafnium oxide- and zirconium oxide-based capacitors, while ferroelectric hafnium oxide-based capacitors have been less extensively investigated. This work highlights the enhancement of the energy-storage characteristics of epitaxial ferroelectric orthorhombic lanthanum-doped hafnium oxide-based two-dimensional capacitors by introducing a thin dielectric amorphous alumina capping layer. It is revealed that the inclusion of a dielectric layer influences both the ESD and η of the fabricated capacitors due to the increased depolarization effect resulting from the presence of the alumina layer. The best balance between ESD and η is achieved through the insertion of a 2.3 nm-thick alumina layer, providing an ultra-high ESD of 142 J/cm3, with an η of 69% for an electric field of 7.7 MV/cm. Additionally, the capacitor displays an ESD greater than 120 J/cm3 after 106 cycles and a stable performance up to 120 °C. Therefore, this work foresees the potential of ferroelectric epitaxial hafnium oxide-based capacitors in energy-storage technologies.