Symmetry Breaking in Gold−Silica−Gold Multilayer Nanoshells

We present a computational study of the plasmonic properties of gold−silica−gold multilayer nanoshells with the core offset from the center. Symmetry breaking, due to the core offset, makes plasmon resonances that are dark in concentric geometries visible. Applying plasmon hybridization theory, we explain the origin of these resonances from the interactions of an admixture of both primitive and multipolar modes between the core and the shell. The interactions introduce a dipole moment into the higher order modes and significantly enhance their coupling efficiency to light. To elucidate the symmetry breaking effect, we link the geometrical asymmetry to the asymmetrical distribution of surface charges and demonstrate illustratively the diminishing multipolar characteristic and increasing dipolar characteristic of the higher order modes. The relative amplitudes of the modes are qualitatively related by visual examination of the dipolar component in the surface charge distributions. Using polarization-dependent surface charge plots, we illustrate two distinct mode configurations despite their spectral similarities. We further demonstrate a trend of increasing absorption relative to scattering as the resonant wavelength red shifts in response to a larger core offset.