Domain nucleation kinetics and polarization-texture-dependent electronic properties in two-dimensional α-In2Se3 ferroelectrics

Two-dimensional (2D) ferroelectric semiconductors, such as α-In2Se3 with switchable spontaneous polarization and superior optoelectronic properties, exhibit large potential for functional device applications. The electric transport properties and device performance of 2D α-In2Se3 are strongly sensitive to the ferroelectric domain structures and polarization textures, but they are rarely explored at the atomic scale. Herein, by a combination of first-principles calculations and a developed domain switching theory, we report the domain nucleation kinetics and polarization-texture dependent electronic properties in α-In2Se3 ferroelectrics. Our calculated results reveal that the reversed domains characterized by armchair boundaries tend to form triangular or stripped shape. The energy barrier for propagating domain boundaries is ∼1.42 eV and can be reduced by loading external electric field, which is responsible for driving the evolution of domain structures. Moreover, the domain switching leads to notable changes in the band gap and carrier spatial distribution of α-In2Se3 monolayer, resulting in higher electric resistance of multi-polarization domain structures than that of single-polarization state. The domain structures of multilayer α-In2Se3 follow a layer-by-layer switching mechanism, which causes the transition of electronic structures from self-doped p-n junctions to type-II semiconductor homojunctions. This study not only provides an in-depth insight into the domain switching mechanisms of α-In2Se3 but also opens up the possibility to tailor their electronic and transport properties.