Surface-enhanced Raman spectroscopy: nonlocal limitations

Giant field enhancement and field singularities are a natural consequence of the commonly employed local-response framework. We show that a more general nonlocal treatment of the plasmonic response leads to new and possibly fundamental limitations on field enhancement with important consequences for our understanding of surface-enhanced Raman spectroscopy (SERS). The intrinsic length scale of the electron gas serves to smear out assumed field singularities, leaving the SERS enhancement factor finite, even for geometries with infinitely sharp features. For silver nanogroove structures, mimicked by periodic arrays of half-cylinders (up to 120 nm in radius), we find no enhancement factors exceeding 10 orders of magnitude (10(10)). (C) 2012 Optical Society of America