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Carrier mobifity enhancement from 0.09 to 0.59cm2/Vs is achieved for pentacene-based thin-film transistors (TFTs) by modifying the HfO2 gate dielectric with a polystyrene (PS) thin film. The improvement of the transistors performance is found to be strongly related to the initial film morphologies of pentacene on the dielectrics. In contrast to the three-dimensional island-like growth mode on the HfO2 surface, the Stranski-Krastanov growth mode on the smooth and nonpolar PS/HfO2 surface is believed to be the origin of the excellent carrier mobifity of the TFTs. A large well-connected first monolayer with fewer boundaries is formed via the Stranski-Krastanov growth mode, which facilitates a charge transport parallel to the substrate and promotes higher carrier mobility.