Large-area plasmonic hot-spot arrays: sub-2 nm interparticle separations with plasma-enhanced atomic layer deposition of Ag on periodic arrays of Si nanopillars

Initial reports of plasmonic 'hot-spots' enabled the detection of single molecules via surface-enhanced Raman scattering (SERS) from random distributions of plasmonic nanoparticles. Investigations of systems with near-field plasmonically coupled nanoparticles began, however, the ability to fabricate reproducible arrays of such particles has been lacking. We report on the fabrication of large-area, periodic arrays of plasmonic 'hot-spots' using Ag atomic layer deposition to overcoat Si nanopillar templates leading to reproducible interpillar gaps down to <2 nm. These plasmonic 'hot-spots' arrays exhibited over an order of magnitude increase in the SERS response in comparison to similar arrays with larger interpillar separations.