Multifunctional Hybrid Multilayer Gate Dielectrics with Tunable Surface Energy for Ultralow-Power Organic and Amorphous Oxide Thin-Film Transistors.

For large-area, printable, and flexible electronic applications using advanced semiconductors, novel dielectric materials with excellent capacitance, insulating property, thermal stability, and mechanical flexibility need to be developed to achieve high-performance, ultralow-voltage operation of thin-film transistors (TFTs). In this work, we first report on the facile fabrication of multifunctional hybrid multilayer gate dielectrics with tunable surface energy via a low-temperature solution-process to produce ultralow-voltage organic and amorphous oxide TFTs. The hybrid multilayer dielectric materials are constructed by iteratively stacking bifunctional phosphonic acid-based self-assembled monolayers combined with ultrathin high-k oxide layers. The nanoscopic thickness-controllable hybrid dielectrics exhibit the superior capacitance (up to 970 nF/cm2 ), insulating property (leakage current densities <10-7 A/cm2 ), and thermal stability (up to 300 °C) as well as smooth surfaces (root-mean-square roughness <0.35 nm). In addition, the surface energy of the hybrid multilayer dielectrics are easily changed by switching between mono- and bifunctional phosphonic acid-based self-assembled monolayers for compatible fabrication with both organic and amorphous oxide semiconductors. Consequently, the hybrid multilayer dielectrics integrated into TFTs reveal their excellent dielectric functions to achieve high-performance, ultralow-voltage operation (< ± 2 V) for both organic and amorphous oxide TFTs. Because of the easily tunable surface energy, the multifunctional hybrid multilayer dielectrics can also be adapted for various organic and inorganic semiconductors, and metal gates in other device configurations, thus allowing diverse advanced electronic applications including ultralow-power and large-area electronic devices.