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

Chi Chen, Xingfei Wei, Molly F. Parsons, Jiajia Guo, James L. Banal, Yinong Zhao, Madelyn N. Scott, Gabriela S. Schlau-Cohen, Rigoberto Hernandez and Mark Bathe ()
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Chi Chen: Massachusetts Institute of Technology
Xingfei Wei: Johns Hopkins University
Molly F. Parsons: Massachusetts Institute of Technology
Jiajia Guo: Massachusetts Institute of Technology
James L. Banal: Massachusetts Institute of Technology
Yinong Zhao: Johns Hopkins University
Madelyn N. Scott: Massachusetts Institute of Technology
Gabriela S. Schlau-Cohen: Massachusetts Institute of Technology
Rigoberto Hernandez: Johns Hopkins University
Mark Bathe: Massachusetts Institute of Technology

Nature Communications, 2022, vol. 13, issue 1, 1-15

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-32662-w

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