Two-dimensional Ferroelectric Ga2O3 Bilayers with Unusual Strain-engineered Interlayer Interactions

TL;DR

This study uses ab-initio calculations to explore the structural, electronic, and optical properties of 2D ferroelectric Ga2O3 bilayers, revealing strain-induced phase transitions and tunable interlayer interactions with potential for future applications.

Contribution

It provides a systematic analysis of the ferroelectric and antiferroelectric configurations and uncovers a strain-driven phase transition from van der Waals to ionic interlayer interactions.

Findings

Identification of three dipole models in Ga2O3 bilayers.

Reversible polarization transition between stacking configurations.

Strain-induced phase transition from vdW to ionic interlayer bonding.

Abstract

Two-dimensional (2D) van der Waals (vdW) materials and their bilayers have stimulated enormous interests in fundamental researches and technological applications. Recently, a group of 2D vdW III2-VI3 materials with out-of-plane ferroelectricity have attracted substantial attentions. In this work, the structural, electronic and optical properties of 2D ferroelectric Ga2O3 bilayer system are systematically studied using ab-initio computational method. Intrinsic dipoles of the two freestanding monolayers lead to three distinct dipole models (one ferroelectric and two antiferroelectric models). The stable stacking configurations of ferroelectric and antiferroelectric dipole models can be transferred with polarization reversal transition of the monolayers without additional operation. Interlayer perturbation effects combined with biaxial-strain engineering lead to high tunablility of the electronic and optical properties of the bilayer systems. Surprisingly, the results reveal a phase transition from vdW to ionic interlayer interaction induced by in-plane biaxial tensile strain. Detailed analyses suggest a transition mechanism based on the ionic bonding nature of the Ga2O3 system, involving interlayer rearrangement of anions to compensate the symmetry breaking of the heavily distorted ionic folding configurations. These insights can open new prospects for future experimental synthesis, characterization and application of 2D Ga2O3 atomic-thin layered systems.