Antiferroelectricity in thin film ZrO2 from first principles

Abstract

Density functional calculations are performed to investigate the experimentally-reported field-induced phase transition in thin-film ZrO2 (J. Muller et al., Nano. Lett. 12, 4318). We find a small energy difference of ~ 1 meV/f.u. between the nonpolar tetragonal and polar orthorhombic structures, characteristic of antiferroelectricity. The requisite first-order transition between the two phases, which atypically for antiferroelectrics have a group-subgroup relation, results from coupling to other zone-boundary modes, as we show with a Landau-Devonshire model. Tetragonal ZrO2 is thus established as a previously unrecognized lead-free antiferroelectric with excellent dielectric properties and compatibility with silicon. In addition, we demonstrate that a ferroelectric phase of ZrO2 can be stabilized through epitaxial strain, and suggest an alternative stabilization mechanism through continuous substitution of Zr by Hf.

arXiv comment5 pages, 5 figures

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• Effects of Growth Orientations and Epitaxial Strains on Phase Stability of HfO${}_2$ Thin Films
• Piezoelectricity in hafnia
• Stabilization of competing ferroelectric phases of HfO${}_2$ under epitaxial strain
• Deep Learning of Accurate Force Field of Ferroelectric HfO${}_2$
• Enhanced ferroelectricity in epitaxial Hf0.5Zr0.5O2 thin films integrated with Si(001) using SrTiO3 templates
• Impact of Four-Valent Doping on the Crystallographic Phase Formation for Ferroelectric HfO${}_2$ from First-Principles: Implications for Ferroelectric Memory and Energy-Related Applications
• Causes of ferroelectricity in HfO${}_2$-based thin films: An $\text{ab initio}$ perspective
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• First-principles re-investigation of bulk WO3
• Phase Competition in HfO${}_2$ with Applied Electric Field from First Principles
• High-throughput first principles search for new ferroelectrics
• A computational study of hafnia-based ferroelectric memories: from ab initio via physical modeling to circuit models of ferroelectric device
• A CMOS-compatible morphotropic phase boundary
• The impact of charge compensated and uncompensated strontium defects on the stabilization of the ferroelectric phase in HfO${}_2$
• Theoretical approach to ferroelectricity in hafnia and related materials
• Effect of dopant ordering on the stability of ferroelectric hafnia
• Origin of ferroelectricity in magnesium doped zinc oxide
• Symmetry of ferroelectric switching and domain walls in hafnium dioxide
• Ferroelectric HfO${}_2$-ZrO${}_2$ multilayers with reduced wake-up
• Triggered ferroelectricity in HfO${}_2$ from hybrid phonons and higher-order dynamical charges