Fluorinated hybrid materials were synthesized for a solution-processable gate insulator. The surface energy was modified by perfluoroalkyl chains contained in the hybrid gate insulator itself. We investigated the initial morphology and growth mode of pentacene and the characteristics of organic thin-film transistors ͑OTFTs͒ to determine how these characteristics depend on the surface energy. Pentacene growth was changed from a layer-by-layer mode to a three-dimensional ͑3D͒ island growth mode at low surface energy. Tightly and uniformly grown pentacene grains at 3D island mode induced good OTFT performance, but the carrier mobility was degraded at very low surface energy due to the large amount of grain boundaries.Organic thin-film transistors ͑OTFTs͒ attract great interest due to their ease of processing, low cost, and wide applicability. The characteristics of OTFTs are very dependent on the gate insulators because the majority of the charge carriers in the OTFTs are located close to the interface between the gate insulator and the organic semiconductor. 1-3 The surface energy of the gate insulator has an effect on the initial growth behavior, the morphology, and the crystallinity of the pentacene layer; these are critical performance factors for OTFTs. The hydrophobic surface of the gate insulator, which induces the pentacene crystallinity and the interconnection between pentacene grains, enhances OTFT performance. To this end, surface treatments on the gate insulator using hexamethyldisilazane, octadecyltrichlorosilane, and other self-assembled monolayers ͑SAMs͒ were employed. [4][5][6] In this study, we considered methacrylate siloxane hybrid materials ͑hybrimers͒ simply synthesized by a sol-gel process of organoalkoxysilane. The perfluoroalkyl chain was introduced in the design of the hybrimer to tune the surface energy of the gate insulator. Instead of using an additional surface treatment on the gate insulators, we added long perfluoroalkyl chains to the hybrimer gate insulator. These chains were concentrated on the insulator surface, leading to better growth of the pentacene. We added various amounts of perfluoroalkylsilane to the hybrimer to control the surface energy of the gate insulator. Next we observed the growth behavior of the pentacene on the hybrimer gate insulator. We investigated the electrical characteristics of the fabricated OTFT to determine how these characteristics depend on the content of perfluoroalkyl chains.
ExperimentalWe synthesized fluorinated hybrid materials ͑hybrimers͒ via a sol-gel process using 3-͑trimethoxysilyl͒propyl methacrylate, titanium͑IV͒ butoxide, and 1H,1H,2H,2H-perfluorodecyltrimethoxysilane ͑PFAS͒. Instead of using an additional surface treatment, we added long perfluoroalkyl chains to the hybrimer gate insulator itself. These chains were concentrated on the insulator surface, leading to better growth of the pentacene. To control the surface energy of the gate insulator, the amounts of PFAS, which contained the hydrophobic perfluoroalkyl chain, were adjusted as f...