Flexoelectricity-stabilized ferroelectric phase with enhanced reliability in ultrathin La:HfO2 films

TL;DR

This study demonstrates that the flexoelectric effect induces a rhombohedral distortion in La:HfO2 thin films, significantly enhancing their fatigue endurance and stability for integrated ferroelectric applications.

Contribution

It reveals that flexoelectricity can stabilize ferroelectric phases in ultrathin doped HfO2 films, improving their reliability and phase stability.

Findings

Flexoelectric effect induces rhombohedral distortion in La:HfO2 films.

Distorted structure is more stable under electric fields.

Enhanced fatigue endurance of ferroelectric phase.

Abstract

Doped HfO2 thin films exhibit robust ferroelectric properties even for nanometric thicknesses, are compatible with current Si technology and thus have great potential for the revival of integrated ferroelectrics. Phase control and reliability are core issues for their applications. Here we show that, in (111)-oriented 5%La:HfO2 (HLO) epitaxial thin films deposited on (La0.3Sr0.7)(Al0.65Ta0.35)O3 substrates, the flexoelectric effect, arising from the strain gradient along the films normal, induces a rhombohedral distortion in the otherwise Pca21 orthorhombic structure. Density functional calculations reveal that the distorted structure is indeed more stable than the pure Pca21 structure, when applying an electric field mimicking the flexoelectric field. This rhombohedral distortion greatly improves the fatigue endurance of HLO thin films by further stabilizing the metastable ferroelectric phase against the transition to the thermodynamically stable non-polar monoclinic phase during repetitive cycling. Our results demonstrate that the flexoelectric effect, though negligibly weak in bulk, is crucial to optimize the structure and properties of doped HfO2 thin films with nanometric thicknesses for integrated ferroelectric applications.