Engineering Ferroelectric Hf0.5Zr0.5O2 Thin Films by Epitaxial Stress

TL;DR

This study demonstrates that epitaxial stress significantly influences the stabilization of the ferroelectric orthorhombic phase in Hf0.5Zr0.5O2 thin films, enabling enhanced ferroelectric properties for device applications.

Contribution

It reveals how epitaxial strain controls phase stabilization in Hf0.5Zr0.5O2 films, advancing the understanding of ferroelectric behavior in these materials.

Findings

Tensile strain stabilizes the orthorhombic ferroelectric phase.

Substrate choice affects phase and polarization levels.

Enhanced ferroelectric polarization observed on specific substrates.

Abstract

The critical impact of epitaxial stress on the stabilization of the ferroelectric orthorhombic phase of hafnia is proved. Epitaxial bilayers of Hf0.5Zr0.5O2 and La0.67Sr0.33MnO3 electrodes were grown on a set of single crystalline oxide 001-oriented, cubic or pseudocubic setting, substrates with lattice parameter in the 3.71 - 4.21 A range. The lattice strain of the La0.67Sr0.33MnO3 electrode, determined by the lattice mismatch with the substrate, is critical in the stabilization of the orthorhombic phase of Hf0.5Zr0.5O2. On La0.67Sr0.33MnO3 electrodes tensile strained most of the Hf0.5Zr0.5O2 film is orthorhombic, whereas the monoclinic phase is favored when La0.67Sr0.33MnO3 is relaxed or compressively strained. Therefore, the Hf0.5Zr0.5O2 films on TbScO3 and GdScO3 substrates present substantially enhanced ferroelectric polarization in comparison to films on other substrates, including the commonly used SrTiO3. The capability of having epitaxial doped HfO2 films with controlled phase and polarization is of major interest for a better understanding of the ferroelectric properties and paves the way for fabrication of ferroelectric devices based on nanometric HfO2 films.