Two-Dimensional Antiferroelectricity in Nanostripe-Ordered In2Se3

Two-dimensional (2D) layered materials have been an exciting frontier for exploring emerging physics at reduced dimensionality, with a variety of exotic properties demonstrated at 2D limit. Here, we report the first experimental discovery of in-plane antiferroelectricity in a 2D material β′-In2Se3, using optical and electron microscopy consolidated by first-principles calculations. Different from conventional 3D antiferroelectricity, antiferroelectricity in β′-In2Se3 is confined within the 2D layer and generates the unusual nanostripe ordering: the individual nanostripes exhibit local ferroelectric polarization, whereas the neighboring nanostripes are antipolar with zero net polarization. Such a unique superstructure is underpinned by the intriguing competition between 2D ferroelectric and antiferroelectric ordering in β′-In2Se3, which can be preserved down to single-layer thickness as predicted by calculation. Besides demonstrating 2D antiferroelectricity, our finding further resolves the true nature of the β′-In2Se3 superstructure that has been under debate for over four decades.