“…Van der Waals layered CuInP 2 S 6 (CIPS) has generated great excitement in recent years because of its room temperature ferroelectricity with out-of-plane spontaneous polarization (1-3), making it an ideal candidate to develop two-dimensional (2D) heterostructures for microelectronic devices (4)(5)(6)(7). Ferroelectric field-effect transistors (6,8), negative capacitance field-effect transistors (9,10), ferroelectric tunneling junctions (1), and memristors (11) have all been demonstrated with CIPS, which are attractive for both logic and memory applications (6,12) enabling future neuromorphic computing (13)(14)(15). Besides technological potentials, CIPS is also fascinating from a materials point of view, exhibiting exotic properties such as giant negative piezoelectricity (16,17), tunable quadruple energy wells (18), large room temperature electrocaloric effect (16,19), and strong coupling between ferroelectric polarization and ionic conductivity (13,20,21).…”