Abstract

Moiré structures have gained attention for their ability to regulate material properties and drive phenomena such as superconductivity, topological effects, and the quantum Hall effect. This tunability also extends to Moiré ferroelectricity, which is essential for high‐performance, multistate electronic devices. However, most studies focus on few‐layer twisted materials from mechanical exfoliation. Although chemical vapor deposition (CVD) theoretically enables the direct growth of twisted multilayer materials with sliding Moiré ferroelectricity, this has yet to be achieved. The characteristics of van der Waals‐layered SnSe2, such as multiphase and broad bandgap, make it well suited for the direct growth of multilayer structures. Herein, multilayer Moiré‐twisted SnSe2 is synthesized using a non‐steady‐state CVD method. Layered and screw twists lead to Moiré structures, inducing ferroelectricity. Increasing the number of twists and layers enhances ferroelectric properties and signal feedback. These devices exhibit clear hysteresis and multistate ferroelectric performance under varying voltage drives.

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