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We demonstrate fast (0.25 s/pixel) nanoscale chemical imaging in aqueoussolution via tip-enhanced Raman scattering (TERS), with sub-15 nm spatialresolution. The substrate consists of 4-mercaptobenzonitrile-functionalizedmonocrystalline gold triangular platelets immersed in H2O, which we map using agold-coated AFM probe illuminated using a 633 nm laser source. We find that therecorded TERS images trace the enhanced local optical fields that are sustainedtowards the edges and corners of the triangles. In effect, we directly maplocal optical fields of a plasmonic substrate in aqueous solution throughmolecular TERS. Overall, our described platform and approach may generally beused for chemical and biological imaging, and potentially, to follow chemicaltransformations at solid-liquid interfaces through TERS.

Taking the Plunge: Nanoscale Chemical Imaging of Functionalized Gold Triangles in H2O via TERS