Anomalous reverse mechanical polarization switching in negative piezoelectric CuInP2S6.

van der Waals ferroelectric CuInP₂S₆ (CIPS) has drawn significant attention not only because of its unique properties but also owing to its technological potential for nanoelectronics. Mechanical polarization switching provides a new approach to modulating polarization states through flexoelectricity. This approach is particularly favourable for CIPS to avoid surface damage under an electric field due to the coupling between polarization switching and ionic motion. Here, we report anomalous downward-to-upward polarization switching under tip force in CIPS nanoflakes, which is believed to stem from the competition between piezoelectric and flexoelectric fields induced by tip pressure, together with the unique quadruple-well state present in CIPS. This work provides novel insights into the polarization switching mechanism of CIPS, elucidating the interplay between competing piezoelectric and flexoelectric fields, and it may pave the way for the design of electromechanical devices based on flexoelectric engineering.