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We theoretically investigated electron energy loss spectroscopy (EELS) ofultraviolet surface plasmon modes in aluminum nanodisks. Using full-wavesimulations, we studied the impact of diameter on the resonant modes of thenanodisks. We found that the mode behavior can be separately classified for twodistinct cases: (1) flat nanodisks where the diameter is much less than thethickness; and (2) thick nanodisks where the diameter is comparable to thethickness. While the multipolar edge modes and breathing modes of flatnanostructures have previously been interpreted using intuitive, analyticalmodels based on surface plasmon polariton (SPP) modes of a thin-film stack, ithas been found that the true dispersion relation of the multipolar edge modesdeviates significantly from the SPP dispersion relation. Here, we developed amodified intuitive model that uses effective wavelength theory to accuratelymodel this dispersion relation with significantly less computational overheadcompared to full-wave electromagnetic simulations. However, for the case ofthick nanodisks, this effective wavelength theory breaks down, and suchintuitive models are no longer viable. We found that this is because some modesof the thick nanodisks carry a polar (i.e. out of the substrate plane, or alongthe electron beam direction) dependence and cannot be simply categorized asradial breathing modes or angular (azimuthal) multipolar edge modes. This polardependence leads to radiative losses, motivating the use of simultaneous EELSand cathodoluminescence measurements when experimentally investigating thecomplex mode behavior of thick nanostructures.

Electron-Energy Loss of Ultraviolet Plasmonic Modes in Aluminum Nanodisks