“…The spatial configuration of matter and surface ligands in colloidal crystals, which control many physical and chemical properties, can be tailored in a nanometer precision by adjusting the subunit composites, sizes, shapes, and crystal structures (5)(6)(7)(8). Therefore, the colloidal assembly has become an effective strategy in producing many functional materials in photonics (9)(10)(11)(12), structural materials (13,14), robotics (15)(16)(17), and catalysis (18,19). The assembly of either spherical or highly faceted colloids is mainly dominated by entropic processes that involve depletion, hydrophobic forces, and polymer "elasticity," producing densely packed colloidal crystals with close surface contact (3,20,21).…”