Folding of flexible colloidal polymers into colloidal clusters*

The self-assembly of complex materials is a search in high-dimensional space for the desired structure. Borrowing a concept from biology, here we reduce the dimensionality of the problem by folding 1-D colloidomer chains into compact architectures. Tuning DNA-mediated secondary interactions along the length of the colloidal droplet polymer allows us to optimize the yield and fidelity of the fold. More specifically, we compare the collapse dynamics of homo- and hetero-colloidomers, in which all or alternating bead-to-bead interactions are allowed. The strength of these interactions is temperature-dependent with protocols that govern the temporal order of interactions. We study how changes in the interaction matrix of an alternating folding sequence affect the pathways of colloidomers of different lengths. Furthermore, we show results comparing the folding of quenched versus annealed colloidomers. This study builds toward the programmable sequence design of colloidal polymers that fold into a unique stable structure of a functional complex material.