Hierarchical Colloidal Self-Assembly on Lattice-Mismatched Moiré Patterns

Extending atomic epitaxy concepts to colloidal systems for realizing functional surface structures has recently piqued scientific interest. Akin to the growth of ordered metal clusters on graphene moiré, spatially ordered colloidal crystals have been realized on soft lithographically fabricated moiré patterns. In addition to moiré periodicity, lattice misfit strain can bring about a further level of hierarchy in colloidal self-assembly, although its role in self-organization remains unexplored. Here, we demonstrate the self-organized growth of micrometer-sized colloidal pyramid arrays with lateral order extending over millimeter length scales on lattice-mismatched moiré patterns. By probing the film growth dynamics with single-particle resolution, we uncovered the interplay between lattice misfit strain and topographically varying surface potential within the moiré unit cell, which significantly alters the nucleation process. We also show that the structural organization of colloids within moiré regions primarily depends on the moiré angle, and by tuning it, multiple levels of hierarchy can be achieved.