Polyimide films with ultralow dielectric loss for 5G applications: Influence and mechanism of ester groups in molecular chains

Abstract

Polyimides are ideal candidates for 5G high-frequency communications due to their good thermal stability, mechanical properties and processability. However, the exploration of how to reduce their high-frequency dissipation factor (Df) remains an urgent and alluring challenge. Inspired by the molecular structure of liquid crystal polyester, which is insensitive to high-frequency electric fields, here we design two series of polyimides derived from diamines with multiple ester groups (AXEB, X = 1, 2 or 3) and 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) or p-phenylene bis (trimellitate anhydride) (TA2EB). We investigated the effects of ester number on the aggregation structure, water absorption, dielectric properties, heat resistance and mechanical properties of the polyimides and find that the Df of the multiple ester-containing polyimides decreases rapidly with increasing frequency and number of ester groups. Wide-angle X-ray diffraction analysis, polarized optical microscopy observations and molecular dynamics simulations show that the unique properties of these polyimides benefit from the tight packing of the molecular chain and the strong intermolecular interaction force caused by the ester group, as well as the resulting prolonged dipole relaxation time and the greatly reduced water absorption. Therefore, the polyimide films show extremely low Df values of 0.0030 for AXEB-6FDA and 0.0013 for AXEB-TA2EB. Furthermore, AXEB-TA2EB also shows excellent thermal stability, mechanical properties, electrical properties and permittivity. More importantly, their ultralow moisture rate (<0.83 %) ensures that the high-frequency Df remains stable in different humid environments, even after soaking in water. This method can also be extended to other polymers, thus providing a new strategy for the design of low dielectric loss materials.