Enhanced dielectric permittivity of hierarchically double-gyroid nanocomposites via macromolecular engineering of block copolymers.

It is a challenging task to realize the periodically bicontinuous gyroid nanostructures of flexible nanocomposites with high loading of functionalized nanoparticles, which could exhibit high dielectric permittivity for energy storage and electronic devices. Herein, with the aid of the concept of macromolecular engineering, we propose novel nanocomposites, composed of A'(A''B) n miktoarm star copolymers and nanoparticles, to obtain a double-gyroid structure through self-consistent field theory coupled with density functional theory. By tailoring the architecture of this copolymer, a large window of the double-gyroid phase extending to a high loading concentration of nanoparticles is achieved, leading to a hierarchical structure of a percolation network of nanoparticles within the gyroid channels. Furthermore, the finite difference quasielectrostatic method is integrated to reveal an enhanced dielectric permittivity of the structured nanocomposites by increasing the loading concentration of nanoparticles. The simultaneous achievement of an ordered double-gyroid phase and high loading nanoparticles represents a crucial step toward the realization of fully three-dimensional network-like metamaterials via a rational molecular design of nanocomposites.