DNA origami is a novel self-assembly technique allowing one to form various 2D shapes and position matter with nanometer accuracy. It has been used to coordinate placement of nanoscale objects, both organic and inorganic; to make molecular motors and walkers; and to create optically active nanostructures. Here we use DNA origami templates to engineer Surfaced Enhanced Raman Scattering (SERS) substrates. Specifically, gold nanoparticles were selectively attached to the corners of rectangular origami and subsequently enlarged via solution-based metal deposition. The resulting assemblies were designed to form hot spots of enhanced electromagnetic field between the nanoparticles. We observed a significant enhancement of the Raman signal from molecules covalently attached to the assemblies, as compared to control nanoparticle samples which lack inter-particle hot spots. Our method opens up the prospects of using DNA origami to rationally engineer and assemble plasmonic structures for molecular spectroscopy.
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