Three-dimensional directed assembly of organic charge-transfer heterostructure.

Multicomponent crystalline heterostructures are a powerful approach to integrate different functional materials into the ordered structures. Here we describe three-dimensional spherical assembly of binary organic solids that consist of electron donor and acceptor molecules. A mechanistic study of heterostructure formation reveals that the dewetting and drying-mediated assembly processes are responsible for the spherical crystallite formation. The assembled spherical heterostructures are highly tunable, crystalline and chemically stable, exhibiting phase separation controlled optoelectronic behavior. This simple, generalizable three-dimensional assembly can be modified for the formation of ordered functional organic multicomponent heterostructures for emerging applications.