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Surface-enhanced Raman spectroscopy (SERS) is enabled by local surfaceplasmon resonances (LSPRs) in metallic nanogaps. When SERS is excited by directillumination of the nanogap, the background heating of lattice and electronscan prevent further manipulation of the molecules. To overcome this issue, wereport SERS in electromigrated gold molecular junctions excited remotely:surface plasmon polaritons (SPPs) are excited at nearby gratings, propagate tothe junction, and couple to the local nanogap plasmon modes. Like directexcitation, remote excitation of the nanogap can generate both SERS emissionand an open-circuit photovoltage (OCPV). We compare SERS intensity and OCPV inboth direct and remote illumination configurations. SERS spectra obtained byremote excitation are much more stable than those obtained through directexcitation when photon count rates are comparable. By statistical analysis of33 devices, coupling efficiency of remote excitation is calculated to be around10%, consistent with the simulated energy flow.

Quantifying efficiency of remote excitation for surface enhanced Raman spectroscopy in molecular junctions