Macroscale-area patterning of three-dimensional DNA-programmable frameworks

DNA, owing to its adaptable structure and sequence-prescribed interactions, provides a versatile molecular tool to program the assembly of organized three-dimensional (3D) nanostructures with precisely incorporated inorganic and biomolecular nanoscale components. While such programmability allows for self-assembly of lattices with diverse symmetries, there is an increasing need to integrate them onto planar substrates for their translation into applications. In this study, we develop an approach for the growth of 3D DNA-programmable frameworks on arbitrarily patterned silicon wafers and metal oxide surfaces, as well as study the leading effects controlling these processes. We achieve the selective growth of DNA origami superlattices into customized surface patterns with feature sizes in the tens of microns across macroscale areas using polymer templates patterned by electron-beam lithography. We uncover the correlation between assembly conditions and superlattice orientations on surfaces, lattice domain sizes, twining, and surface coverage. The demonstrated approach opens possibilities for bridging self-assembly with traditional top-down nanofabrication for creating engineered 3D nanoscale materials over macroscopic areas with nano- and micro-scale controls.