Multi-plasmon effects and plasmon satellites in photoemission from nanostructures

Abstract

Plasmons can be excited during photoemission and produce spectral photoelectron features that yield information on the nanoscale optical response of the probed materials. However, these so-called plasmon satellites have so far been observed only for planar surfaces, while their potential for the characterization of nanostructures remains unexplored. Here, we theoretically demonstrate that core-level photoemission from nanostructures can display spectrally narrow plasmonic features, reaching relatively high probabilities similar to the direct peak. Using a nonperturbative quantum-mechanical framework, we find a dramatic effect of nanostructure morphology and dimensionality as well as universal scaling laws for the plasmon-satellite probabilities. In addition, we introduce a pump–probe scheme in which plasmons are optically excited prior to photoemission, leading to plasmon losses and gains in the photoemission spectra and granting us access to the ultrafast dynamics of the sampled nanostructure. These results emphasize the potential of plasmon satellites to explore multi-plasmon effects and ultrafast electron–plasmon dynamics in metal-based nanoparticles and two-dimensional nanoislands.