2D Perovskite Nanosheet‐Driven Polymeric Nanocomposites as Gate Dielectrics for Flexible Negative‐Capacitance Applications

Abstract Designing composite gate dielectrics tailored by incorporating inorganic perovskite nanofillers into a polymer matrix to develop flexible low‐voltage transistors can be challenging because homogeneous dispersion of nanomaterials in the matrix is difficult to achieve; thus, degradation of the electrically insulating properties of nanocomposite layers is often observed. In this study, nanocomposite dielectrics are presented that consist of 2D Ba ₅ Ta ₄ O ₁₅ nanosheets (BTO NSs) for the first time. Perovskite BTO is introduced using the Langmuir–Blodgett method to construct a precise and pinhole‐free interface for the homogeneous assembly of 2D nanosheets. Its high k value and ferroelectric properties, which arise from the perovskite structure, can be harnessed to achieve attractive polarization and remarkable electronic properties. The 2D BTO NSs can also be utilized as phase crystallization fillers to enhance the ferroelectric properties of polyvinylidene fluoride (PVDF). Additionally, the multilayer PVDF/perovskite nanosheet hybrid dielectric, which reaches an unprecedentedly high dielectric constant of 22.4, exhibits effective dielectric relaxation related to the interfacial induced ferroelectric polarization and decisive negative‐capacitance response.