Near-field and SERS enhancement from rough plasmonic nanoparticles

The lithographic fabrication of metal nanoparticles usually involves the thermal vacuum deposition of metals, which leads to polycrystallinity and surface roughness. In recent years, strong efforts have been made to clarify the role of such roughness in surface-enhanced Raman scattering (SERS). In this paper, we provide a systematic experimental and theoretical study of single lithographically fabricated nanoparticles to unravel the role of surface roughness and morphology on the optical far-and near-field properties. We find that the experimentally observed reduction of the SERS signal upon thermal annealing of particle arrays is caused by a complex interplay of changes in the dielectric response of gold, the resonance wavelength, and the reduced nanoscopic roughness.