It is demonstrated that treating dielectrics with fluorinated polymers, which have excellent hydrophobicity, chemical inertness, and the lowest polarizability, yields a semiconductor‐compatible surface energy and excellent charge detrapping characteristics. Fluorocopolymers, polystyrene‐random‐poly(2,3,4,5,6‐pentafluorostyrene) (PS‐r‐PPFS) copolymers with different 2,3,4,5,6‐pentafluorostyrene (PFS) loadings, are synthesized to modify a SiO2 gate dielectric using radical polymerization. Surface energy (γ) of the copolymer‐treated SiO2 dielectrics decreases from 40.7 to 24.0 mJ m−2 with increasing PFS mol% in the copolymer. Pentacene organic field‐effect transistors (OFETs) show field‐effect mobility (μFET) values ranging from 0.82 (for 0 mol% PFS) to 0.25 cm2 V−1 s−1 (for 100 mol% PFS). Enhancing the bias stress stability without affecting the μFET value is achieved via the introduction of a small mol% fluorocarbon segments onto the PS‐r‐PPFS backbone. 15 mol% PFS‐loaded fluorocopolymer‐coated SiO2 substrate yields a γ value of 35 mJ m−2, close to that (38 mJ m−2) of the lowest‐γ crystal surface of pentacene, and the corresponding OFETs have μFET values up to 0.81 cm2 V−1 s−1 and excellent gate‐bias stress stability in comparison to the rich fluorinated dielectric systems, which has degraded μFET values ranging from 0.2 to 0.4 cm2 V−1 s−1.

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Mi Jang, Minjung Lee, and co‐workers clearly demonstrate how much the balancing surface hydrophobicity and polarizability of gate dielectrics is important to achieve excellent environmental, gate‐bias stability, and mobility of organic field‐effect transistors, specifically, based on pentacene layers grown on hydrophobicity‐controlled fluorinated copolymer‐treated dielectrics in article 1600284.