Dynamic DNA Origami-Based Gold Nanoparticle Dimerization: Design and Assembly of a Hybrid Platform for Nanophotonics

Revolutionary discoveries and developments of new techniques have led to a paradigm shift in the field of nanotechnology in the last two decades. The unique interaction of noble metal nanoparticles with light and their exploration and optimization enabled even the vibrational spectroscopic detection of even single molecules. However, this requires precise control over the geometry and arrangement of nanoparticles down to the sub-nanometer level. This became possible in 2006 with the development of DNA origami, the programmable folding and driving of long strands of DNA into 3D shapes.

In this work, the development and construction of a complex nanophotonic hybrid platform for analytical applications in the field of Raman spectroscopy was carried out. The platform consists of three single origami and two gold nanoparticles. The basic idea of the design relies on the implementation of a new thiol-based coupling strategy for the attachment of gold nanoparticles (≥ 8 nm) to DNA origami structures as well as the detergent-based stabilization of these complexes in commonly used DNA origami buffers. For the nanophotonic hybrid platform, two different origami shapes, a 3D DNA origami box and a planar dynamic platform, were developed and characterized. The origami box was designed to allow not only site-specific functionalization of the internalized gold nanoparticles, but also dimerization of the gold nanoparticles with nanometer precision. Precise dimerization using the dynamic origami platform is achieved by the exchange of single-stranded DNA strands that can move the two halves of the platform toward or away from each other.

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