Disentangling stress and strain effects in ferroelectric HfO2

Abstract

Ferroelectric HfO2 films are usually polycrystalline and contain a mixture of polar and nonpolar phases. This challenges the understanding and control of polar phase stabilization and ferroelectric properties. Several factors, such as dopants, oxygen vacancies, or stress, among others, have been investigated and shown to have a crucial role on optimizing the ferroelectric response. Stress generated during deposition or annealing of thin films is a main factor determining the formed crystal phases and influences the lattice strain of the polar orthorhombic phase. It is difficult to discriminate between stress and strain effects on polycrystalline ferroelectric HfO2 films, and the direct impact of orthorhombic lattice strain on ferroelectric polarization has yet to be determined experimentally. Here, we analyze the crystalline phases and lattice strain of several series of doped HfO2 epitaxial films. We conclude that stress has a critical influence on metastable orthorhombic phase stabilization and ferroelectric polarization. On the contrary, the lattice deformation effects are much smaller than those caused by variations in the orthorhombic phase content. The experimental results are confirmed by density functional theory calculations on HfO2 and Hf0.5Zr0.5O2 ferroelectric phases.