We harness amphiphilic DNA origami nanostructures (DONs), whose broken symmetry, realized through surface patterns of polynucleotide brushes that can exert different non-specific interactions, induces aggregation into micellar architectures. To synthesize patterned brushes we employed surface-initiated TdT-catalyzed enzymatic polymerization of nucleotides and nucleotide analogues. We show that brush functionalization can be precisely controlled by the site-specific location of initiation sites on the origami core and by controlling brush height and composition. We show how this molecular level control over composition and location on the DON surface can be used to program the chemical patchiness of the building blocks which regulates their interactions and drives self-assembly. Our experiments are aided by molecular simulations which help to explore the rules that underlie the observed supramolecular self-assembly.<br/><br/>The combination of chemically patterned origami with principles of colloidal self-assembly using nonspecific interactions is new and provides exciting synergies at the interface of DNA nanotechnology and colloid science. Our entropy-based assembly approach enables dynamic and reversible control over hierarchical materials assembly directed by a large number of weak cooperative interactions. This increases tolerance for morphological and structural defects which promotes structura resilience. We believe that our approach has the potential to extend DNA nanotechnology to accomplish the organization of rationally-designed nanomaterials at the mesoscale. Such materials are needed in emerging applications where resilience for operation in adverse conditions is of practical importance.

Resilient materials through spatiotemporal control of polynucleotide brush growth and mesoscale assembly of DNA origami

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ACS Fall 2022

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