Printable Ultra‐Flexible Fluorinated Organic–Inorganic Nanohybrid Sol–Gel Derived Gate Dielectrics for Highly Stable Organic Thin‐Film Transistors and Other Practical Applications

A novel fluorinated organic–inorganic (O–I) hybrid sol—gel based material, named FAGPTi, is successfully synthesized and applied as a gate dielectric in flexible organic thin‐film transistors (OTFTs). The previously reported three‐arm‐shaped alkoxysilane‐functionalized amphiphilic polymer yields a stable O–I hybrid material consisting of uniformly dispersed nanoparticles in the sol‐state. Here, a fluorinated precursor is introduced into the system, making it possible to realize more stable spherical composites. This results in long‐term colloidal stability (≈1.5 years) because composite growth is strongly inhibited by the presence of fluorine groups with intrinsically strong repulsive forces. Additionally, the FAGPTi film is easily deposited via thermally annealed sol–gel reactions; the films can be successfully fabricated through the printing method, and exhibit excellent flexibility and enhanced insulating properties compared to existing materials. OTFTs with FAGPTi layers show highly stable driving characteristics under severe bending conditions (1.9% strain). Integrated logic devices are also successfully operated with these OTFTs. Additionally, it can facilely be applied to amorphous indium‐gallium‐zinc‐oxide (a‐IGZO) TFT devices other than OTFT. Therefore, this synthetic strategy can provide useful insights into the production of functional O–I hybrid materials, enabling the efficient fabrication of electronic materials and devices exhibiting these properties. New fluorinated organic–inorganic hybrid dielectric materials are synthesized with an amphiphilic three‐arm structured polymeric precursor, fluorinated precursor, and conventional inorganic precursors. This synthetic strategy provides long‐term stability in the sol state and enables the fabrication of a variety of highly flexible and electrically stable electronic devices along with facile thin film formation and printing processes through solution‐based sol–gel reactions.