Ferroelectric and negative piezoelectric properties in oxyhydroxide monolayers γ-XOOH (X = Al, Ga, and In)

Two-dimensional (2D) multiferroic materials with coexisting ferroelasticity (FA) and ferroelectricity (FE) have potential applications in high-density data storage and sonar detectors. Here, based on first-principles calculations, we predict a series of stable 2D FA-FE multiferroic structures, namely, γ-XOOH (X = Al, Ga, and In) monolayers. By analyzing the lattice symmetry and orientation distribution of hydroxyls, we find that XOOH monolayers possess both in-plane ferroelastic and ferroelectric polarization, as well as antiferroelectric ordering caused by the anti-parallel alignment of hydroxyls. Interestingly, the perpendicular reorientation of in-plane FE polarization accompanies 90° ferroelastic switching. Moreover, they show an unusual negative transverse piezoelectric effect originated from the clamped-ion term. The multiferroic properties of the XOOH monolayers provide an excellent platform to study electroelastic effects.