Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering

Tailoring and enhancing the functional properties of materials at reduced dimension is critical for continuous advancement of modern electronic devices. Here, the discovery of local surface induced giant spontaneous polarization in ultrathin BiFeO₃ ferroelectric films is reported. Using aberration-corrected scanning transmission electron microscopy, it is found that the spontaneous polarization in a 2 nm-thick ultrathin BiFeO₃ film is abnormally increased up to ≈90–100 µC cm⁻² in the out-of-plane direction and a peculiar rumpled nanodomain structure with very large variation in c/a ratios, which is analogous to morphotropic phase boundaries (MPBs), is formed. By a combination of density functional theory and phase-field calculations, it is shown that it is the unique single atomic Bi₂O_3−x layer at the surface that leads to the enhanced polarization and appearance of the MPB-like nanodomain structure. This finding clearly demonstrates a novel route to the enhanced functional properties in the material system with reduced dimension via engineering the surface boundary conditions.

A giant enhancement of ferroelectric polarization in ultrathin 2 nm BiFeO₃ film is reported. With the addition of a Bi₂O_3−x monolayer on the surface of ferroelectric BiFeO₃ thin films, the ferroelectric polarization of the ultrathin BiFeO₃ film is stabilized and dramatically increased up to ≈150 µC cm⁻², demonstrating the possibility of enhancing the performance of ferroelectric materials at the reduced dimension.

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