Directional Light Scattering In Mie‐Resonant Si Particles With Ultra‐Thin Au Shells

Metamaterial research has sought to create nanostructures with strong directional optical scattering to control light propagation at the nanoscale. Core–shell architectures comprised of both resonant cores and resonant shells are suggested as candidate particles in which the spectral overlap of the electric and magnetic dipoles is controlled to create strong directional scattering. In this study, Au‐decorated Si core–shell (Si@Au) particles are presented, studying the role of the architecture (particulate, discontinuous shells vs continuous) and dimensions of the shell. The core–shell particles are synthesized by first creating Si particles, through the thermal disproportionation of hydrogen silsesquioxane (HSQ), which are then decorated with ≈4 nm diameter Au nanoparticles. The resonant behavior of the core–shell particles is characterized using electron energy‐loss spectroscopy mapping and optical single‐particle scatter spectroscopy. These observations are supported by T‐matrix simulations and Mie‐theory calculations of the scattering spectra, which show that, compared to Si, Si@Au particles demonstrate a dampened magnetic dipole resonance for smaller Si core diameters (100–130 nm) and an enhanced magnetic dipole resonance for larger Si core sizes (150–200 nm). The study indicates that the previously reported hybridized modes do not exist in particulate Au shells around a Si core and can only exist in continuous plasmonic shells. Thus, it is shown here how important it is to be as precise as possible regarding the nanomaterial architecture used in simulations. No configuration of Si@Au core–shell particles with a particulate shell could be found that strongly enhanced directional scattering, and a continuous shell may do so only modestly. However, the simulations show that the synthesis of thin, continuous Ag shells might represent an alternative route towards achieving good directional scattering properties.