Polyimide (PI) films with simultaneously low dielectric
loss (Df) values at high frequencies and excellent general
properties
are urgently needed with the rapid development of high frequency communication
technology. Herein, we proposed that dielectric loss can be decreased
by reducing intermolecular friction work. Inspired by liquid crystals
with low intermolecular frictions, novel liquid-crystal-like PI films
were designed by simultaneously introducing mesogen units and promoting
groups (−CF3) and then being thermally imidized
via a unique solvent-assisted continuous ramping process without any
stretching or shearing process. The liquid-crystal-like PI films exhibited
ultralow Df values such as 0.00365 at 1 MHz, 0.00184 at
10 GHz, and 0.0027 at 0.75THz, which were 28.7%, 45.4%, and 97.0%
lower, respectively, than those of PI films without liquid-crystal-like
structures. The results of molecule simulations further demonstrated
that liquid-crystal-like structures can reduce intermolecular friction
work by slowing dipole rotation, leading to ultralow Df values of PI films. The liquid-crystal-like PI films also exhibited
thermal expansion coefficients of 11.4 ppm/K, tensile strengths of
228.7 MPa, Young’s moduli of 6.15 GPa, and elongations at break
of 16.4%.