Low-voltage Organic Thin Film Transistors (OTFTs) with Solution-processed High-k Dielectric cum Interface Engineering

Although impressive progress has been made in improving the performance of organic thin film transistors (OTFTs), the high operation voltage resulting from the low gate areal capacitance of traditional SiO 2 remains a severe limitation that hinders OTFTs’ development in practical applications. In this regard, developing new materials with high- k characteristics at low cost is of great scientific and technological importance in the area of both academia and industry.;In this thesis, we first describe a simple solution-based method to fabricate a high-k bilayer Al2Oy/TiOx (ATO) dielectric system at low temperature. Then the dielectric properties of the ATO are characterized and discussed in detail. Furthermore, by employing the high-k ATO as gate dielectric, low-voltage copper phthalocyanine (CuPc) based OTFTs are successfully developed. Interestingly, the obtained low-voltage CuPc TFT exhibits outstanding electrical performance, which is even higher than the device fabricated on traditional low-k SiO2. The above results seem to be contradictory to the reported results due to the fact that high-k usually shows adverse effect on the device performance. This abnormal phenomenon is then studied in detail. Characterization on the initial growth shows that the CuPc molecules assemble in a “rod-like” nano crystal with interconnected network on ATO, which probably promotes the charge carrier transport, whereas, they form isolated small islands with amorphous structure on SiO2. In addition, a better metal/organic contact is observed on ATO, which benefits the charge carrier injection. Our studies suggest that the low-temperature, solution-processed high-k ATO is a promising candidate for fabrication of high-performance, low-voltage OTFTs.;Furthermore, it is well known that the properties of the dielectric/semiconductor and electrode/semiconductor interfaces are crucial in controlling the electrical properties of OTFTs. Hence, investigation the effects of interfaces engineering on improving the electrical characteristics of OTFTs is of great technological importance. For the dielectric/semiconductor interface, an octadecylphosphonic acid (ODPA) self-assembled monolayer (SAM) is used to modify the surface of ATO (ODPA/ATO). For the electrode/semiconductor interface, a simple in-situ modified Cu (M-Cu) is employed as source-drain (S/D) electrodes in stead of commonly used Au. The electrical characteristics of pentacene TFT are drastically enhanced upon interfaces modification. Moreover, by encapsulating the M-Cu with a thin layer of Au (Au/ M-Cu), the device performance is further improved. The detailed mechanism is systematically explored.;Finally, organic electronic devices on flexible plastic substrates have attracted much attention due to their low-cost, rollability, large-area processability, and so on. One of the most critical issues in realization flexible OTFTs is the integration of gate dielectrics with flexible substrates. We have successfully incorporated the ODPA/ATO with Au coated flexible polyimide (PI) substrate. By using Au/M-Cu as S/D electrode, the flexible pentacene TFTs show outstanding electrical performance. In addition, the mechanical flexibility and reliability of the devices are studied in detail. Our approach demonstrates an effective way to realize low-cost, high-performance flexible OTFTs.