Excitation of surface and volume plasmons in metal nanocluster by fast electrons

TL;DR

This study models the excitation and damping of surface and volume plasmons in metal nanoclusters by fast electrons, analyzing their spectral features and comparing results with electron microscopy data.

Contribution

It introduces a hydrodynamic approach that accounts for surface, volume, and radiative damping mechanisms, providing detailed insights into plasmon excitation spectra.

Findings

Surface and volume plasmons significantly influence the loss spectra.

Damping mechanisms depend differently on multipole mode order.

Spectral features vary with impact parameter and electron passage time.

Abstract

Surface and volume plasmons excited in a metal cluster by moving electron and corresponding inelastic scattering spectra are studied based on the hydrodynamic approach. Along with the bulk losses traditionally taken into account, the surface and radiative ones are also considered as the physical mechanisms responsible for the plasmon damping. The second and third mechanisms are found to be essential for the surface plasmons and depend very differently on the multipole mode order. The differential equations are obtained which describe the temporal evolution of every particular mode as that one of a linear oscillator excited by the given external force, and the electron energy loss spectra are calculated. The changes in spectrum shape with the impact parameter and with the electron passage time are analyzed and found to be in good enough agreement with the data of scanning transmission electron microscopy (STEM) experiments. It is shown that, in the general case, a pronounced contribution to the formation of the loss spectrum is given by the both surface and volume plasmons with low and high multipole indices. In particular, at long electron passage time, the integral loss spectrum which is calculated for the free-electron cluster model contains two main peaks: a broad peak from merging of many high-order multipole resonances of the surface plasmons and a narrower peak of nearly the same height from merged volume plasmons excited by the electrons that travel through the central region of the cluster. Comparatively complex dependences of the calculated excitation coefficients and damping constants of various plasmons on the order of the excited multipole result in wide diversity of possible types of the loss spectrum even for the same cluster material and should be taken into account in interpretation of corresponding electron energy loss spectroscopy (EELS) experiments.