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Abstract Two-dimensional (2D) ferroelectric semiconductors offer unique opportunities for ultrathin non-volatile memory and neuromorphic devices, yet the role of stacking order in intrinsic ferroelectric systems remains largely unexplored. Here we report the stacking-controlled growth of large-area 2D β′- and α-In2Se3 with distinct 2H and 3R configurations through chemical vapour deposition by regulating selenium kinetics and strain relaxation.
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