Phase and polarization modulation in two-dimensional In₂Se₃ via in situ transmission electron microscopy

Phase transitions in two-dimensional (2D) materials promise reversible modulation of material physical and chemical properties in a wide range of applications. 2D van der Waals layered In₂Se₃ with bistable out-of-plane ferroelectric (FE) α phase and antiferroelectric (AFE) β' phase is particularly attractive for its electronic applications. However, reversible phase transition in 2D In₂Se₃ remains challenging. Here, we introduce two factors, dimension (thickness) and strain, which can effectively modulate the phases of 2D In₂Se₃. We achieve reversible AFE and out-of-plane FE phase transition in 2D In₂Se₃ by delicate strain control inside a transmission electron microscope. In addition, the polarizations in 2D FE In₂Se₃ can also be manipulated in situ at the nanometer-sized contacts, rendering remarkable memristive behavior. Our in situ transmission electron microscopy (TEM) work paves a previously unidentified way for manipulating the correlated FE phases and highlights the great potentials of 2D ferroelectrics for nanoelectromechanical and memory device applications.