| Summary: | Fullerene, as a novel building block of functional materials, possesses a wide range of intriguing properties, some of which are closely related to hierarchical structures. Advancing the methodology for manipulating fullerene hierarchical structures could facilitate developments of novel fullerene-based materials with desired properties. In the present work, we report our exploration of a series of fullerene-based unconventional spherical packing nanostructures, including Frank-Kasper (FK) A15 and σ phases as well as dodecagonal quasicrystalline (DDQC) phase in unary self-assembly systems of fullerene-based giant molecules. Also, in giant molecule binary blends, alloy-type spherical phases with high volume asymmetries such as FK Laves C14 (MgZn2) and C15 (MgCu2) phases and quasi-FK AlB2 phase can also be found. These observations showcase the feasibility of fabricating a wide range of fullerene-based superlattices through self-assembly of specifically designed giant molecules. Superlattice engineering offers a promising avenue for constructing specific structures and functions in order to achieve desired properties, in particular, for developing innovative fullerene-based materials.
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