The programmability and predictable nature of of DNA makes it an attractive structure-directing ligand for the self-assembly of nanoparticle superlattices with unique structure-dependent physical phenomena. While DNA base pairing has enabled the development of materials with predetermined nanoscale structures, manipulating the macroscopic shape of the lattices with the same level of predictive accuracy remains challenging. Additionally, the measurement of specific properties or fabrication of devices enabled by these intentionally designed structures remain underexplored areas compared to advancements in their synthesis. Here, we examine at-equilibrium deposition processes capable of generating single crystals with well-defined shapes that ultimately allow for the synthesis of complex mechanical and optical materials. We will demonstrate both experimental evidence and simple models based on fundamental principles collective explain and allow for intentional control of material mesoscale shape. We will also demonstrate how this control allows for predetermined manipulation of the hierarchical mechanical properties of DNA-assembled materials, and one of the first examples of a DNA-nanoparticle superlattice optical device for angular dependent reflectance for the purpose of coupling out-of-plane light sources. Finally, we will demonstrate how stabilization of these superlattices in gels allows for their structures to be dynamically altered as a function of different chemical and physical stimuli. Together, these experiments show that fundamental scientific understanding of nanoscale assembly with DNA results in a powerful tool for the synthesis of complex hierarchical structures with beneficial physical characteristics for device engineering.

DNA-directed assembly of materials and devices with intentionally programmed structure-property relationships

ACS Spring 2022

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