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Nanoscale gaps between adjacent metallic nanostructures give rise toextraordinarily large field enhancements, known as "hot spots", uponillumination. Incident light with the electric field polarized across the gap(along the interparticle axis) is generally known to induce the strongestsurface enhanced Raman spectroscopy (SERS) enhancements. However, here we showthat for a nanogap located within a nanowire linking extended Au electrodes,the greatest enhancement and resulting SERS emission occurs when the electricfield of the incident light is polarized along the gap (transverse to theinterelectrode axis). This surprising and counterintuitive polarizationdependence results from a strong dipolar plasmon mode that resonatestransversely across the nanowire, coupling with dark multipolar modes arisingfrom subtle intrinsic asymmetries in the nanogap. These modes give rise tohighly reproducible SERS enhancements at least an order of magnitude largerthan the longitudinal modes in these structures.

Dark plasmons in hot spot generation and polarization in interelectrode nanoscale junctions