Ladder-Type Silsesquioxane Copolymer Gate Dielectrics for High-Performance Organic Transistors and Inverters

A ladder-type poly(phenyl-co-methacryl silsesquioxane) (PPMSQ) copolymer was developed for use as a gate dielectric in high-performance organic field-effect transistors (OFETs). The ladder-type PPMSQ copolymer was synthesized via the hydrolysis of two types of monomers, methacryloxypropyltrimethoxysilane and phenyltrimethoxysilane, followed by a condensation polymerization. The phenyl groups in one monomer were introduced to enhance the structural ordering of the overlying organic semiconductors, whereas the methacryloxypropyl groups in the other monomer were introduced to cross-link the polymer chains via thermal- or photocuring. The curing process enhanced the electrical strength of the gate dielectric layer due to the formation of a network structure with a reduced free volume. Thermal curing reduced the surface energy of the gate dielectrics, which improved the structural order of the overlying organic semiconductors and promoted the formation of large grains. The ladder-type PPMSQ was used as a gate dielectric to produce benchmark p- and n-channel OFETs based on pentacene and N,N′-dioctyl-3,4,9,10-perylenedicarboximide (PTCDI-C₈), respectively. The resulting OFETs exhibited excellent electrical performances, including a high carrier mobility (0.53 cm² V^-1s^-1 for the p-type pentacene OFET and 0.17 cm² V^-1s^-1 for the n-type PTCDI-C₈ OFET) and a high ON/OFF current ratio exceeding 10⁴. The photocured patterned PPMSQ film was successfully used to fabricate complementary OFET-based inverters that yielded high gains. The use of the ladder-type PPMSQ gate dielectrics provides a novel approach to realizing next-generation organic electronics.