“…Plasmonic noble metal nanostructures have been of broad interest in recent years, since their unique optical properties can enhance important properties of nearby molecules such as absorption, , fluorescence, , and Raman spectroscopy. − In a classical electrodynamics picture, the plasmonic states involve coherent oscillation of all of the conduction band electrons within the nanostructure. − Although the majority of interest has been in the dipolar plasmon resonances where the full electron cloud responds in phase with the electric field of light (Figure ), higher-order plasmon resonances such as quadrupoles have long been known to occur and in the past several years have gained attention for various applications. − The quadrupolar modes are typically optically dark in small nanostructures, but can be excited via near-field radiation − or, in larger nanostructures where the retardation of light across the nanostructure is significant, by far-field radiation. ,− Electrodynamics simulations ,, and experimental studies ,, consistently show that the quadrupolar modes are higher in energy and have much narrower absorption peaks than the corresponding dipolar modes. In rod-shaped nanostructures, electron energy loss spectroscopy (EELS) experiments have revealed the spatial distribution of the longitudinal plasmon modes with various multipolar character.…”