Control of Concentration of Nonhydrogen-Bonded Hydroxyl Groups in Polymer Dielectrics for Organic Field-Effect Transistors with Operational Stability

Poly(4-vinylphenol) (PVP) is a promising gate dielectric material for organic field-effect transistors (OFETs) and circuits fabricated on plastic substrates. Thermal cross-linking of PVP with a cross-linker, such as poly(melamine-co-formaldehyde) methylated (PMF), at a high temperature (above 170 °C) is widely considered an effective method to remove residual hydroxyl groups that induce polarization effects in the dielectric bulk. However, the threshold voltage shift in transfer characteristics is still observed for an OFET with a PVP-PMF dielectric when it is operated at a slow gate voltage sweep rate. The present study examines the cause of the undesired hysteresis phenomenon and suggests a route to enable a reliable operation. We systematically investigate the effect of the PVP-PMF weight ratio and their annealing temperature on the transfer characteristics of OFETs. We discover that the size of the hysteresis is closely related to the concentration of nonhydrogen-bonded hydroxyl groups in the dielectric bulk and this is controlled by the weight ratio. At a ratio of 0.5:1, a complete elimination of hysteresis was observed irrespective of the annealing temperature. We finally demonstrate a highly reliable operation of small-molecule-based OFETs fabricated on a plastic substrate at a low temperature.