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<p>Self-assembly of nanocrystals into functional materials requires precise control over nanoparticle interactions in solution, which are dominated by organic ligands that densely cover the surface of nanocrystals. Recent experiments have demonstrated that small truncated-octahedral nanocrystals can self-assemble into a range of superstructures with different translational and orientational order of nanocrystals. The origin of this structural diversity remains unclear. Here, we use moleculardoi:10.26434/chemrxiv.7108769 fatcat:dki2d5rrevgvbpzpnvsmq7olgq