Footprints of atomic-scale features in plasmonic nanoparticles as revealed by electron energy loss spectroscopy

Citations Over Time

Abstract

We present a first-principles theoretical study of the atomistic footprints in the valence electron energy loss spectroscopy (EELS) of nanometer-size metallic particles. Charge density maps of excited plasmons and EEL spectra for specific electron paths through a nanoparticle (Na₃₈₀ atom cluster) are modeled using ab initio calculations within time-dependent density functional theory. Our findings unveil the atomic-scale sensitivity of EELS within this low-energy spectral range. Whereas localized surface plasmons (LSPs) are particularly sensitive to the atomistic structure of the surface probed by the electron beam, confined bulk plasmons (CBPs) reveal quantum size effects within the nanoparticle's volume. Moreover, we prove that classical local dielectric theories mimicking the atomistic structure of the nanoparticles reproduce the LSP trends observed in quantum calculations, but fall short in describing the CBP behavior observed under different electron trajectories.

Related Papers

• Sweet plasmonics： Sucrose macrocrystals of metal nanoparticles(2015)
• → Spatio‐spectral metrics in electron energy loss spectroscopy as a tool to resolve nearly degenerate plasmon modes in dimer plasmonic antennas(2023)2 cited
• → Spatio-spectral metrics in electron energy loss spectroscopy as a tool to resolve nearly degenerate plasmon modes in dimer plasmonic antennas(2023)1 cited
• → Electron Energy Loss Spectroscopy of Plasmons in Individual Silver Nanowires and Gold Nanorods(2008)
• High-order plasmonic modes on aluminum nanoantennas unveiled by electron energy loss spectroscopy(2014)