Transparent Alicyclic Polyimides Prepared via Copolymerization or Crosslinking: Enhanced Flexibility and Optical...

Transparent polyimides with excellent mechanical properties and high optical transmittance have been widely used in various optical and electrical applications. However, due to the rigidity of their aromatic structure, their flexibility is limited, making them unsuitable for applications requiring different form factors, such as flexible display cover windows. Furthermore, the refractive index of most transparent polyimides is approximately 1.57, which differs from that of the optically clear adhesives (OCAs) and window materials that have values typically around 1.5, resulting in visual distortion. This study employed 4,4'-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) and 2,2'-bis(trifluoromethyl)benzidine (TFMB) as the base structure of polyimides (6T). Additionally, 1,3-bis(aminomethyl)cyclohexane (BAC) with a monocyclic structure and bis(aminomethyl)bicyclo[2,2,1]heptane (BBH) with a bicyclic structure were introduced as co-monomers or crosslinking agents to 6T. The mechanical, thermal, and optical properties of the obtained copolymers (6T-BAC and 6T-BBH series) and crosslinked polymers (6T-CL-BAC and 6T-CL-BBH series) were compared. Both the copolymer series (6T-BAC and 6T-BBH) and the crosslinked series (6T-CL-BAC and 6T-CL-BBH) exhibited improved optical properties compared to the conventional 6T, with maximum transmittance exceeding 90% and refractive indices ranging from approximately 1.53 to 1.55. Notably, the copolymer series achieved transmittance levels above 95% and exhibited lower refractive indices (~1.53), demonstrating superior optical performance relative not only to the 6T baseline but also to the crosslinked series. The alicyclic polyimides synthesized in this study exhibited mechanical flexibility, high optical transmittance, and a refractive index approaching 1.5, demonstrating their applicability for use as flexible display cover window materials.