Localized Raman enhancement from a double-hole nanostructure in a metal film

An isolated double-hole indentation, with concentric rings, in a metal film was used to obtain highly localized surface-enhanced Raman scattering (SERS) from regions much smaller than the optical wavelength. The structure was created by a focused ion beam (FIB) milling partially through the 100 nm thick gold film to a depth of 50 nm. Significant SERS enhancement was observed for both oxazine 720 and rhodamine 6G. The SERS was polarization-dependent because of the biaxial symmetry of the double-hole at the apexes where the indentations overlap; these apexes were responsible for the strong subwavelength focusing. The finite-difference time-domain method was used to calculate the electromagnetic field of the nanostructure, and it showed strong polarization-dependent focusing, in agreement with the experimentally observed SERS enhancement. On the basis of these calculations, it is estimated that the 60% polarization-dependent SERS enhancement is the result of only similar to 1300 molecules in the region of the apexes, and it is estimated that the limit of detection is 20 molecules for the best-case configuration. This work is an important step toward single-molecule SERS from tailored nanostructures designed for predictable field enhancement.