Dual-Scattering Near-Field Microscope for Correlative Nanoimaging of SERS and Electromagnetic Hotspots

Surface-enhanced Raman spectroscopy (SERS) enables sensitive chemical studies and materials identification, relying on electromagnetic (EM) and chemical-enhancement mechanisms. Here we introduce a tool for the correlative nanoimaging of EM and SERS hotspots, areas of strongly enhanced EM fields and Raman scattering, respectively. To that end, we implemented a grating spectrometer into a scattering-type scanning near-field optical microscope (s-SNOM) for mapping of both the elastically and inelastically (Raman) scattered light from the near-field probe, that is, a sharp silicon tip. With plasmon-resonant gold dimers (canonical SERS substrates) we demonstrate with nanoscale spatial resolution that the enhanced Raman scattering from the tip is strongly correlated with its enhanced elastic scattering, the latter providing access to the EM-field enhancement at the illumination frequency. Our technique has wide application potential in the correlative nanoimaging of local-field enhancement and SERS efficiency as well as in the investigation and quality control of novel SERS substrates.