Vibrational surface EELS probes confined Fuchs-Kliewer modes

Abstract

Recently, two reports have demonstrated the amazing possibility to probe vibrational excitations from nanoparticles with a spatial resolution much smaller than the corresponding free-space phonon wavelength using electron energy loss spectroscopy (EELS). While Lagos et al. evidenced a strong spatial and spectral modulation of the EELS signal over a nanoparticle, Krivanek et al. did not. Here, we show that discrepancies among different EELS experiments as well as their relation to optical near- and far-field optical experiments can be understood by introducing the concept of confined bright and dark Fuchs-Kliewer modes, whose density of states is probed by EELS. Such a concise formalism is the vibrational counterpart of the broadly used formalism for localized surface plasmons; it makes it straightforward to predict or interpret phenomena already known for localized surface plasmons such as environment-related energy shifts or the possibility of 3D mapping of the related surface charge densities.

References in corpus (5)

• Optical excitations in electron microscopy
• Probing the photonic local density of states with electron energy loss spectroscopy
• Simulating electron energy loss spectroscopy with the MNPBEM toolbox
• Probing the symmetry of the potential of localized surface plasmon resonances with phase-shaped electron beams
• Tomography of particle plasmon fields from electron energy loss spectroscopy

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