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Self-assembled monolayers of microparticles encoding Archimedean andnon-regular tessellations promise unprecedented structure-propertyrelationships for a wide spectrum of applications in fields ranging fromoptoelectronics to surface technology. Yet, despite numerous computationalstudies predicting the emergence of exotic structures from simple interparticleinteractions, the experimental realization of non-hexagonal patterns remainschallenging. Not only kinetic limitations often hinder structural relaxation,but also programming the inteparticle interactions during assembly, and hencethe target structure, remains an elusive task. Here, we demonstrate how asingle type of soft polymeric microparticle (microgels) can be assembled into awide array of complex structures as a result of simple pairwise interactions.We first let microgels self-assemble at a water-oil interface into ahexagonally packed monolayer, which we then compress to varying degrees anddeposit onto a solid substrate. By repeating this process twice, we find thatthe resultant structure is not the mere stacking of two hexagonal patterns. Thefirst monolayer retains its hexagonal structure and acts as a template intowhich the particles of the second monolayer rearrange to occupy interstitialpositions. The frustration between the two lattices generates new symmetries.By simply varying the packing fraction of the two monolayers, we obtain notonly low-coordination structures such as rectangular and honeycomb lattices,but also rhomboidal, hexagonal, and herringbone superlattices which displaynon-regular tessellations. Molecular dynamics simulations show that thesestructures are thermodynamically stable and develop from short-ranged repulsiveinteractions, making them easy to predict, and thus opening new avenues to therational design of complex patterns.

Self-Templating Assembly of Soft Microparticles into Complex Tessellations