Programmed Self‐Assembly of Single Colloidal Gyroids for Chiral Photonic Crystals

Abstract

AbstractGyroid structures are of extensive interest because they provide a rich platform for chiroptics as well as topological photonics. While the double‐gyroid morphology as a bicontinuous structure is not uncommon in self‐assembled soft materials, direct self‐assembly of single‐network gyroids has proven elusive. Here, an enantiomorphic pair of single‐gyroid crystals comprising colloidal spheres is presented, and two distinct routes are demonstrated for programmed self‐assembly of each single colloidal gyroid enantiomorph from rationally designed patchy spheres. The designer colloidal patchy spheres, which closely hew to their synthetic feasibility, are chiral, having either two staggered rectangular patches at opposite poles or four circular patches arranged in a well‐defined geometry. The single colloidal gyroid, as well as its inverse structure, is shown to support a wide complete photonic bandgap in addition to exhibiting rich chiroptical properties, making them attractive chiral photonic crystals. The versatility of this single colloidal gyroid, the bottom‐up routes devised here in silico, and the robustness of the design space for the chiral colloidal patchy spheres together make a strong case for single colloidal gyroids to supersede colloidal diamond, as a target for programmed self‐assembly, in the quest for photonic crystals operating at optical frequencies.