Breakdown of MagicNumbers in Spherical Confinement

Magic numbers in finite particle systems correspond to specific system sizes that allow configurations with low free energy, often exhibiting closed surface shells to maximize the number of nearest neighbors. Since their discovery in atomic nuclei, magic numbers have been essential for understanding the number-structure–property relationships in finite clusters across different scales. However, as the system size increases, the significance of magic numbers diminishes, and the precise system size at which magic number phenomena disappear remains uncertain. In this study, we investigate colloidal clusters formed through confined self-assembly. Small magic number clusters display icosahedral symmetry with closed surface shells, corresponding to pronounced free energy minima. Our findings reveal that beyond a critical system size, closed surface shells disappear, and free energy minima become less pronounced. Instead, we observe a distinct type of colloidal cluster, termed a football cluster, which retains icosahedral symmetry but features lower-coordinated facets disconnected by terraces. A sphere packing model demonstrates that forming closed surface shells becomes impossible beyond a critical system size, explaining the breakdown of magic numbers in large confined systems.