Abstract

The structure and dynamics of ferroelectric domain walls are essential for polarization switching in ferroelectrics, which remains relatively unexplored in two-dimensional ferroelectric α-In2Se3. Interlayer interactions engineering via selecting the stacking order in two-dimensional materials allows modulation of ferroelectric properties. Here, we report stacking-dependent ferroelectric domain walls in 2H and 3R stacked α-In2Se3, elucidating the resistance switching mechanism in ferroelectric semiconductor-metal junction devices. In 3R α-In2Se3, the in-plane movement of out-of-plane ferroelectric domain walls yield a large hysteresis window. Conversely, 2H α-In2Se3 devices favor in-plane domain walls and out-of-plane domain wall motion, producing a small hysteresis window. High electric fields induce a ferro-paraelectric phase transition of In2Se3, where 3R In2Se3 reaches the transition through intralayer atomic gliding, while 2H In2Se3 undergoes a complex process comprising intralayer bond dissociation and interlayer bond reconstruction. Our findings demonstrate tunable ferroelectric properties via stacking configurations, offering an expanded dimension for material engineering in ferroelectric devices.

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