Light-Directed DNA-Programmable Assembly of 3D Superlattices on Surfaces

Functional nanomaterials hold significant potential due to their unique properties, impacting fields such as biosensing, optical metamaterials, and many advanced manufacturing applications. However, creating a broadly applicable fabrication platform to harness these properties in functional devices remains challenging. Herein, we present a scalable method for nanomaterial fabrication, establishing a reliable foundation for constructing complex, reconfigurable nano- to macro-scale architectures on solid supports. By integrating DNA self-assembly with light-directed DNA lithography, we engineer patterned substrates with site-specific precision, thus controlling the spatial placement and alignment of self-assembled 3D nanomaterials.<br/>Our approach utilizes light-directed covalent surface patterning of unmodified DNA to nucleate site-specifically and promote the growth of self-assembling structures. In contrast to conventional photo-crossing linking methods relying on pre-labeled docking strands and biotin-streptavidin binding, our approach eliminates the need for docking DNA strands and chemical modification of complementary strands. By introducing a photoreactive moiety via a heterobifunctional crosslinking reagent, we immobilize DNA through a photochemical reaction in designated surface location over macroscale areas, thus, enabling site-specific programmable assembly of nanomaterial components. The method is promising for developing photonic and electronic devices, and spatially-controlled catalytic surfaces.