No abstract

Ferroelectric van der Waals CuInP2S6 possesses intriguing quadruple-well states and negative piezoelectricity. Its technological implementation has been impeded by the relatively low Curie temperature (bulk T C ∼ 42 °C) and the lack of precise domain control. Here we show that CuInP2S6 can be immune to the finite size effect and exhibits enhanced ferroelectricity, piezoelectricity, and polar alignment in the ultrathin limit when it is interfaced with ferroelectric oxide PbZr0.2Ti0.8O3 films. Piezoresponse force microscopy studies reveal that the polar domains in thin CuInP2S6 fully conform to those of the underlying PbZr0.2Ti0.8O3, where the piezoelectric coefficient changes sign and increases sharply with reducing thickness. High temperature in situ domain imaging points to a significantly enhanced T C of >200 °C for 13 nm CuInP2S6 on PbZr0.2Ti0.8O3. Density functional theory modeling and Monte Carlo simulations show that the enhanced polar alignment and T C can be attributed to interface-mediated structure distortion in CuInP2S6. Our study provides an effective material strategy to engineer the polar properties of CuInP2S6 for flexible nanoelectronic, optoelectronic, and mechanical applications.