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Surface-enhanced Raman spectroscopy (SERS) sensing of DNA sequences byplasmonic nanopores could pave a way to new generation single-moleculesequencing platforms. The SERS discrimination of single DNA bases dependscritically on the time that a DNA strand resides within the plasmonic hot spot.However, DNA molecules flow through the nanopores so rapidly that the SERSsignals collected are not sufficient for single-molecule analysis. In thiswork, we report an approach to control the time that molecules reside in thehot spot by physically adsorbing them onto a gold nanoparticle and thentrapping the single nanoparticle in a plasmonic nanohole. By trapping thenanoparticle for up to minutes, we demonstrate single-molecule SERS detectionof all 4 DNA bases as well as discrimination of single nucleobases in a singleoligonucleotide. Our method can be extended easily to label-free sensing ofsingle-molecule amino acids and proteins.

Single-molecule DNA Bases Discrimination in Oligonucleotides by Controllable Trapping in Plasmonic Nanoholes