Effects of Plasmon Modes on Resonant Raman Images of a Single Molecule.

Localized surface plasmons (LSPs) are excellent light sources at the nanoscale. How to precisely describe the interaction between LSPs and molecules has become an important issue. We present here a comprehensive study on the dependence of resonant Raman images on LSP modes generated by two typical nanostructures. Theoretical calculations demonstrate that the Raman images are sensitive to not only the spatial distribution but also the phase of the localized field, which should be attributed to the quantum nature of the interaction between LSP modes and molecules. We also find that the rotation of noncylindrical symmetry modes could affect the details of images, which offers an extra means to extract molecular information. Our findings extend the understanding of the LSP–matter interaction, which would be useful for the rational design of nanostructures and thus further applications of LSPs.