Circular dichroism in nanoparticle helices as a template for assessing quantum-informed models in plasmonics
in: ACS Photonics (2018)
As characteristic lengths in plasmonics rapidly approach the sub-nm regime, quantum-informed models that can capture those aspects of the quantum nature of the electron gas that are not accessible by the standard approximations of classical electrodynamics, or even go beyond the free-electron description, become increasingly more important. Here we propose a template for comparing and validating the predictions of such models, through the circular dichroism signal of a metallic nanoparticle helix. Theoretical spectra calculated with three different models, each governed by its own physical mechanism, namely the hydrodynamic Drude model, the generalised nonlocal optical response theory, and the quantum-corrected model, show that each case is characterized by a fundamentally distinctive response, always dissimilar to the predictions of the local optical response approximation of classical electrodynamics. These striking differences, that overcome experimental resolution limitations, enable efficient evaluation of the relevance, validity, and range of applicability of quantum-informed theories for extreme-nanoscale plasmonics.