Miyane, S.S.MiyaneChen, C.-K.C.-K.ChenLin, Y.-C.Y.-C.LinUeda, M.M.UedaWEN-CHANG CHEN2022-03-222022-03-22202126376105https://www.scopus.com/inward/record.uri?eid=2-s2.0-85108549319&doi=10.1021%2facsapm.1c00351&partnerID=40&md5=3dfeed51c224c974c6418e3fbeb360dfhttps://scholars.lib.ntu.edu.tw/handle/123456789/598260We developed highly thermally resistant and colorless polyimides (CPIs) with an ultralow coefficient of thermal expansion (CTE) and sufficient mechanical durability as a flexible substrate for organic field-effect transistors (OFETs). The CPIs were synthesized from trans-1,4-cyclohexyl diamine (t-CHDA) with different ratios of 3,3′,4,4′-biphenyltetracarboxylic dianhydride (s-BPDA) and pyromellitic dianhydride (PMDA). The effects of the composition of s-BPDA and PMDA on the thermal, mechanical, electrical, and optical properties of CPIs were investigated. The optimized CPI, PI-3 with 90 mol % s-BPDA and 10 mol % PMDA, showed a relatively high elongation at break (8%) with a low CTE of 14 ppm K-1, a high glass transition temperature (Tg) of 340 °C, and a large tensile modulus (E) of 4.1 GPa, respectively. Besides, PI-3 possessed a high transparency with a light transmittance at 400 nm (T400) of 81% and a low cutoff wavelength (λcutoff) of 349 nm. Next, the dimer diamine of DDA (Priamine 1074) was introduced into the PI-3 structure to reduce the dielectric constant and enhance the stretchability. For example, PI-6C, with 85 mol % t-CHDA and 15 mol % DDA, showed a low dielectric constant (Dk) of 2.8, a low dissipation factor (Df) of 0.004, and a high T400 of 86% with maintained thermal and mechanical properties. Finally, a flexible OFET device using PI-3 as the substrate and dielectric was fabricated and characterized and exhibited an outstanding performance preservation after 1000 bending cycles or the high-temperature heating test, suggesting its excellent durability. The experimental results indicate that the CPIs studied have potential applications for transparent organic electronic devices. ? 2021 American Chemical Society.colorless copolyimideflexible field-effect transistorlow dielectric constantlow dissipation factorlow thermal expansionAminesDurabilityGlass transitionOptical propertiesPolyimidesSubstratesThermal expansionDissipation factorsHigh temperature heatingHigh-glass transition temperaturesLow dielectric constantsMechanical durabilityOrganic electronic devicesPyromellitic dianhydrideThermal and mechanical propertiesOrganic field effect transistorsjournal article10.1021/acsapm.1c003512-s2.0-85108549319