To ensure consistency, we ran the simulations five times which lead to the formation of two different crystal structures, as shown in Fig. . These clusters were formed of a racemic mixture of the truncated tetrahedra with different chirality interactions. Both clusters had layers of cages where each cage was surrounded by three cages with interactions of opposing chirality. As the interactions between the particles were unbiased, such that it was equally likely to form a homochiral or racemic crystal structure, this result suggests that to maximise the π -π overlap between neighbouring cages, the interactions occur between cages of opposite chirality, which is in agreement with the experimentally reported structure. Perpendicular to the planes, the cages form columns that are packed in a window-to-arene fashion. The two clusters differ in the orientation of the cages between the layers. Due to the equivalent energy of the window-to-arene dimers for different alignment between the cages, our interactions between the windows and arenes had no preference in orientation.