Assembly of Prescribed 3D Nanoparticle Organizations Using Inverse Design of Programmable DNA Bonds

The ability to fabricate functional materials and devices by-design at small scales has led to tremendous technological progress over the last decades, primarily through lithographic and additive manufacturing technologies. However, there remains a need for a platform approach for the fabrication of materials with ordered three-dimensional (3D) nanoscale matter with emergent functions, by-design. Here, we will demonstrate the concept and experimental realization of the encoded assembly of nanoparticles into prescribed, hierarchically ordered 3D organizations using DNA programmable bonds. These directional bonds are encoded onto 3D nanoscale DNA origami frames or “voxels”. Our information-constrained, inverse design approach allows for encoding of targeted 3D hierarchical architectures with programmable bonds through identification of repeating mesoscale motifs and their elemental blocks, nanoscale “voxels”, that can also carry a wide variety of encoded nano-cargo. As examples of this approach, we assemble spatially ordered, low-dimensional arrays with coupled plasmonic and photonic scales, a nanoscale analog of face-perovskite lattice, and a hierarchically organized lattice of spiral motifs, each with domain sizes on the order of several microns. Detailed X-ray scattering and electron microcopy studies confirm the correspondence between the designed and realized architectures. We also demonstrate that dynamic DNA nanotechnology elements can be integrated into the bonds to selectively control bond activity and determine the structure of the resultant assembly. This design strategy was shown to selectively regulate the assembly of multiple crystal symmetries from the same pool of “voxels” depending on the particular DNA signal given to the system.