Hybrid plasmonic gap modes in metal film-coupled dimers and their physical origins revealed by polarization resolved dark field spectroscopy

Plasmonic gap modes sustained by metal film-coupled nanostructures have recently attracted extensive research attention due to flexible control over their spectral response and significantly enhanced field intensities at the particle-film junction. In this work, by adopting an improved dark field spectroscopy methodology-polarization resolved spectral decomposition and colour decoding-we are able to "visualize" and distinguish unambiguously the spectral and far field radiation properties of the complex plasmonic gap modes in metal film-coupled nanosphere monomers and dimers. Together with full-wave numerical simulation results, it is found that while the monomer-film system supports two hybridized dipole-like plasmon modes having different oscillating orientations and resonance strengths, the scattering spectrum of the dimer-film system features two additional peaks, one strong yet narrow resonant mode corresponding to a bonding dipolar moment and one hybridized higher order resonant mode, both polarized along the dimer axis. In particular, we demonstrate that the polarization dependent scattering radiation of the film-coupled nanosphere dimer can be used to optically distinguish from monomers and concurrently determine the spatial orientation of the dimer with significantly improved accuracy at the single-particle level, illustrating a simple yet highly sensitive plasmon resonance based nanometrology method.