We have investigated the electric field-induced microscopic structural changes in polycrystalline pentacene-based organic transistors by using in situ micro-Raman spectroscopy. Extra vibrational modes resulting from molecular coupling effect in pentacene film were studied. The herringbone packing of pentacene molecules in solid film is affected by external field and the process is proven to be partially irreversible. In the meantime, in-phase coupling of the C-H bending mode was found to be highly related to the carrier transport of pentacene film. Obtained results suggest that optimal intermolecular π -orbital overlap of pentacene molecules is still a critical factor impacting the carrier transportation for pentacene film featuring polycrystalline morphology.
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