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Organic small-molecule semiconductors have higher carrier mobility compared to polymer semiconductors, while the actual performances of these materials are susceptible to morphological defects and misalignment of crystalline grains. Here, a new strategy is explored to control the crystallization and morphologies of a solution-processed organic small-molecule semiconductor 2,7-dioctyl[1]benzothieno[3,2- b ][1]benzothiophene (C8-BTBT) using soluble polymer films to control the wettability of substrates. Different from the traditional surface modification method, the polymer layer as a modification layer is soluble in the semiconductor solution during the fabrication of organic thin-film transistors (OTFTs). The dissolved polymer alters the state of the semiconductor solution, which in turn, changes the crystallographic morphologies of the semiconductor films. By controlling the solubility and thickness of the polymer modification layers, it is possible to regulate the grain boundary and domain size of C8-BTBT films, which determine the performances of OTFTs. The bottom-gate transistors modified by a thick PS layer exhibit a mobility of &gt;7 cm 2 /V·s and an on/off ratio of &gt;10 7 . It is expected that this new modification method will be applicable to high-performance OTFTs based on other small molecular semiconductors and dielectrics.

Wettability Control of Interfaces for High-Performance Organic Thin-Film Transistors by Soluble Insulating Polymer Films