Van der Waals (vdW) assembly of layered materials is a promising paradigm for creating electronic and optoelectronic devices with novel properties. Ferroelectricity in vdW layered materials could enable nonvolatile memory and low-power electronic and optoelectronic switches, but to date, few vdW ferroelectrics have been reported, and few in-plane vdW ferroelectrics are known. We report the discovery of in-plane ferroelectricity in a widely investigated vdW layered material, b′-In2Se3. The in-plane ferroelectricity is strongly tied to the formation of one-dimensional superstructures aligning along one of the threefold rotational symmetric directions of the hexagonal lattice in the c plane. Surprisingly, the superstructures and ferroelectricity are stable to 200°C in both bulk and thin exfoliated layers of In2Se3. Because of the in-plane nature of ferroelectricity, the domains exhibit a strong linear dichroism, enabling novel polarization-dependent optical properties.
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