Hierarchical assembly of metal nanoparticles, quantum dots and organic dyes using DNA origami scaffolds

Abstract

The self-assembly of nanoscale elements into three-dimensional structures with precise shapes and sizes is important in fields such as nanophotonics, metamaterials and biotechnology. Short molecular linkers have previously been used to create assemblies of nanoparticles, but the approach is limited to small interparticle distances, typically less than 10 nm. Alternatively, DNA origami can precisely organize nanoscale objects over much larger length scales. Here we show that rigid DNA origami scaffolds can be used to assemble metal nanoparticles, quantum dots and organic dyes into hierarchical nanoclusters that have a planet-satellite-type structure. The nanoclusters have a tunable stoichiometry, defined distances of 5-200 nm between components, and controllable overall sizes of up to 500 nm. We also show that the nanoscale components can be positioned along the radial DNA spacers of the nanostructures, which allows short- and long-range interactions between nanoparticles and dyes to be studied in solution. The approach could, in the future, be used to construct efficient energy funnels, complex plasmonic architectures, and porous, nanoengineered scaffolds for catalysis.

Programmable disorder in random DNA tilings

“…Branched structure of silver nanowires that implement simple logic gates controlled by laser beams can be fabricated using chemical synthesis followed by structural rearrangement using a micromanipulator, 31 but this method would not scale well for building more complex photonic circuits. A single DNA origami can be used to organize carbon nanotubes 32 and polymers 33 for building functional components of molecular electronics, and to organize metal nanoparticles, 34 nanorods 35, 36 and organic dyes 37 for building functional components of molecular plasmonics and photonics. Using these approaches as building blocks, and using the principle of programmable disorder in random DNA origami arrays, it would be possible to create complex networks of molecular devices with controlled size distributions, branching properties, and circuit functions.…”

A design strategy for the hierarchical fabrication of colloidal hybrid mesostructures

“…In contrast, there are only rare examples of colloidal mesoscale structures that combine self-assembled organic building blocks and large inorganic NPs, particularly with the inorganic NP as the central structural unit 19,20 . One example that we are aware of consists of DNA origami assemblies attached to a central gold NP, forming 'core-satellite' architectures with smaller gold NPs at the periphery.…”

Optical trapping and manipulation of plasmonic nanoparticles: fundamentals, applications, and perspectives

“…molecules or nanoparticles, to spontaneously arrange with spacings and positions governed by interparticle and particle-substrate interactions. [76][77][78] Inherent drawbacks of this method are a nite amount of defects and also an inability to use molecules whose interactions do not permit self-assembly. This can be overcome by using directed self-assembly, in which a structure is pre-patterned, directing the building blocks to specic locations on the substrate.…”