DNA Origami‐Based Nanoprinting for the Assembly of Plasmonic Nanostructures with Single‐Molecule Surface‐Enhanced Raman Scattering

Metallic nanocube ensembles exhibit tunable localized surface plasmon resonance to induce the light manipulation at the subwavelength scale. Nevertheless, precisely control anisotropic metallic nanocube ensembles with relative spatial directionality remains a challenge. Here, we report a DNA origami based nanoprinting (DOBNP) strategy to transfer the essential DNA strands with predefined sequences and positions to the surface of the gold nanocubes (AuNCs). These DNA strands ensured the specific linkages between AuNCs and gold nanoparticles (AuNPs) that generating the stereo‐controlled AuNC‐AuNP nanostructures (AANs) with controlled geometry and composition. By anchoring the single dye molecule in hot spot regions, the dramatic enhanced electromagnetic field aroused stronger surface enhanced Raman scattering (SERS) signal amplification. Our approach opens the opportunity for the fabrication of stereo‐controlled metal nanostructures for designing highly sensitive photonic devices. DNA origami‐based nanoprinting can transfer DNA strands with predefined sequences and positions to gold nanocube surfaces to create the stereo‐controlled metallic nanostructures with controlled geometry and composition. By anchoring the single dye molecule in hot spot regions, the dramatic enhanced electromagnetic field aroused stronger SERS signal amplification.