“…[1,5] The method has the potential to reach single-molecule sensitivity, as recently shown for molecules that are resonant at the excitation frequency. [3,6,7] However, tip-enhanced optical microscopy has so far been restricted to transparent [8,9] and semitransparent [1,2,10] samples with tip illumination from below. The first experimental demonstrations of tip-enhanced Raman spectroscopy (TERS) used rough silver films on transparent microscope slides supporting the molecules of interest.…”