Generalizing the Chiral Self-Assembly of Spheres and Tetrahedra to Non-Spherical and Polydisperse Molecules in (C₇₀)_x(C₆₀)_1–x(SnI₄)₂

We describe the spontaneous chiral self-assembly of C₇₀ with SnI₄ as well as a mixture of C₆₀ and C₇₀ with SnI₄. Macroscopic single crystals with the formula (C₇₀)_x(C₆₀)_1–x(SnI₄)₂ (x = 0–1) are reported. C_60, which is spherical, and C₇₀, which is ellipsoidal, form a solid solution in these crystals, and the cubic lattice parameter of the chiral phase linearly increases as x grows from 0 to 1 in accordance with Vegard’s law. Our results demonstrate that nonspherical particles and polydispersity are not an impediment to the growth of chiral crystals from high-symmetry achiral precursors, providing a route to assemble achiral particles including colloidal nanocrystals and engineered nanostructures into chiral materials without the need to use external templates or forces.