| Abstract: | The use in low‐power soft electronics of the appropriate insulating polymer materials with a high dielectric constant (k) is considered a practical alternative to that of inorganic dielectric materials, which are brittle and have high processing temperatures. However, the polar surfaces of typical high‐k polymer insulators are problematic. Further, it is a huge challenge to control their surface properties without damage because of their soft and chemically fragile nature. Here, a heat‐assisted photoacidic oxidation method that can be used to effectively oxidize the outermost surfaces of high‐k rubbery polymer films without degradation is presented. The oxidized surfaces prepared with the developed method contain large numbers of hydroxyl groups that enable the subsequent growth of dense and ordered self‐assembled monolayers (SAMs) consisting of organosilanes. The whole process modifies the surface characteristics of polymer dielectrics effectively. The mechanisms of the oxidation of polymer surfaces and the subsequent SAM growth process are investigated. The resulting surface‐tailored rubbery dielectrics exhibit superior electrical characteristics when used in organic transistors. These results demonstrate that this method can be used to realize practical soft organic electronics based on high‐k polymer dielectrics. |
