Designing the Self‐Assembly of Disordered Materials Via Color Frustration

Abstract

Abstract The ability to control self‐assembly with atomic‐level precision has led to remarkable advances in the rational design of crystalline materials. However, similar design strategies have yet to be developed for amorphous materials. Here, a strategy is devised for programming the self‐assembly of amorphous structures by encoding frustration into the building block design. The building blocks are tailored to locally favor the formation of five‐member rings and yield a network of face‐sharing dodecahedral cages whose icosahedral symmetry prevents long‐range order. Surprisingly, unlike geometrically frustrated glasses that form through kinetic arrest, the network nucleates spontaneously from the liquid phase, representing a novel type of thermodynamically stable disordered phase. The stabilization of this frustrated phase via programmable interactions paves the way for a new generation of disordered materials.