Disentangling Cathodoluminescence Spectra in Nanophotonics: Particle Eigenmodes vs Transition Radiation.

Cathodoluminescence spectroscopy performed in an electron microscope has proven a versatile tool for analyzing the near- and far-field optical response of plasmonic and dielectric nanostructures. Nevertheless, the transition radiation produced by electron impact is often disregarded in the interpretation of the spectra recorded from resonant nanoparticles. Here we show, experimentally and theoretically, that transition radiation can by itself generate distinct resonances that, depending on the time-of-flight of the electron beam inside the particle, can result from constructive or destructive interference in time. Superimposed on the eigenmodes of the investigated structures, these resonances can distort the recorded spectrum and lead to potentially erroneous assignment of modal characters to the spectral features. We develop an intuitive analogy that helps distinguish between the two contributions. As an example, we focus on the case of silicon nanospheres and show that our analysis facilitates the unambiguous interpretation of experimental measurements on Mie-resonant nanoparticles.

Mode Hybridization in Silicon Core-Gold Shell Nanosphere.

A dielectric core-metal shell nanosphere has attracted scientific and technological interests due to the unique optical resonances arising from the hybridization of surface plasmon modes and cavity modes. The previous studies focus on a low-index dielectric core without its own optical resonances. Here, optical resonances of a core-shell nanosphere with a high refractive index (n ≈ 4) core with the lowest order Mie resonances in the visible range are investigated theoretically and experimentally. Scattering and absorption spectra of a core-shell nanosphere for different values of the core refractive index are first analyzed, and there is a transition of the hybridization scheme around n ≈ 2. Above the value, a characteristic hybridized mode with strong absorption and weak scattering emerges in the near-infrared range. A core-shell nanosphere composed of a silicon core and a gold shell is prepared, and the resonance modes are studied by single particle scattering spectroscopy and electron energy loss spectroscopy (EELS) in a transmission electron microscope. The core-shell nanospheres exhibit the hybridized modes depending on the core diameter. The hybridized mode as well as the higher order one that is not observable in the scattering spectroscopy is observed in the EELS.