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We report the rapid improvement in the carrier mobility of the electric double layer field-effect transistor based on the ionic liquid (IL)/pentacene single crystal interface. Generally, the surface oxidation of the pentacene single crystal is unavoidable, and the considerable degradation restricts the performance of the field-effect transistor. However, the formation of the IL/pentacene single crystal interface resolves this problem by increasing the carrier mobility by approximately twice the initial value within a few hours. Furthermore, frequency-modulation atomic force microscopy revealed that the aforementioned rapid improvement is attributed to the appearance of a clean and flat surface of the pentacene single crystal via the defect-induced spontaneous dissolution of pentacene molecules into the IL.

The structural properties of ionic liquid/rubrene single-crystal interfaces were investigated using frequency modulation atomic force microscopy. The spontaneous dissolution of rubrene molecules into the ionic liquid was triggered by surface defects such as rubrene oxide defects, and the dissolution rate strongly depended on the initial conditions of the rubrene surface. Dissolution of the second rubrene layer was slower due to the lower defect density, leading to the formation of a clean interface irrespective of the initial conditions. Molecular-resolution images were easily obtained at the interface, and their corrugation patterns changed with the applied force. Force curve measurements revealed that a few solvation layers of ionic liquid molecules formed at the interface, and the force needed to penetrate the solvation layers was an order of magnitude smaller than typical ionic liquid/inorganic solid interfaces. These specific properties are discussed with respect to electric double-layer transistors based on the ionic liquid/rubrene single-crystal interface.