Nanoscale 3D spatial addressing and valence control of quantum dots using wireframe DNA origami

• Published in: Nature communications 2022-08, Vol.13 (1), p.4935-15, Article 4935
• Main Authors: Chen, Chi, Wei, Xingfei, Parsons, Molly F., Guo, Jiajia, Banal, James L., Zhao, Yinong, Scott, Madelyn N., Schlau-Cohen, Gabriela S., Hernandez, Rigoberto, Bathe, Mark
• Format: Article
• Language: English
• Subjects: 119/118; 147/143; 639/925/357/1017; 639/925/926/1050; Assemblies; Binding sites; Circuit design; Coloring Agents; Copy number; Deoxyribonucleic acid; DNA; DNA - chemistry; DNA, Single-Stranded; Dyes; Electron microscopy; Fabrication; Functional materials; Humanities and Social Sciences; Molecular dynamics; multidisciplinary; Nanomaterials; Nanostructures - chemistry; Nanotechnology; Quantum dots; Quantum Dots - chemistry; Science; Science (multidisciplinary); Single-stranded DNA; Spectroscopy; Surface chemistry
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-022-32662-w

Control over the copy number and nanoscale positioning of quantum dots (QDs) is critical to their application to functional nanomaterials design. However, the multiple non-specific binding sites intrinsic to the surface of QDs have prevented their fabrication into multi-QD assemblies with programmed spatial positions. To overcome this challenge, we developed a general synthetic framework to selectively attach spatially addressable QDs on 3D wireframe DNA origami scaffolds using interfacial control of the QD surface. Using optical spectroscopy and molecular dynamics simulation, we investigated the fabrication of monovalent QDs of different sizes using chimeric single-stranded DNA to control QD surface chemistry. By understanding the relationship between chimeric single-stranded DNA length and QD size, we integrated single QDs into wireframe DNA origami objects and visualized the resulting QD-DNA assemblies using electron microscopy. Using these advances, we demonstrated the ability to program arbitrary 3D spatial relationships between QDs and dyes on DNA origami objects by fabricating energy-transfer circuits and colloidal molecules. Our design and fabrication approach enables the geometric control and spatial addressing of QDs together with the integration of other materials including dyes to fabricate hybrid materials for functional nanoscale photonic devices. Programming the 3D spatial organization of quantum dots requires precise control over their individual valence, but this is challenging due to the possible presence of multiple binding sites. Here, authors develop a general approach that uses highly programmable wireframe DNA origami structures to control the 3D spatial relationships between QDs and other non-nucleic-acid molecules.