Circular Dichroism in Nanoparticle Helices as a Template for Assessing Quantum-Informed Models in Plasmonics

Abstract

As characteristic lengths in plasmonics rapidly approach the sub-nanometer 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. For illustration purposes, we compare three widely used models, each dominant at different nanoparticle separations and governed by its own physical mechanism, namely, the hydrodynamic Drude model, the generalized nonlocal optical response theory, and the quantum-corrected model for tunneling. Our calculations show that, indeed, each case is characterized by a fundamentally distinctive response, always dissimilar to the predictions of the local optical response approximation of classical electrodynamics, dominated by a model-sensitive absorptive double-peak feature. In circular dichroism spectra, the striking differences between models manifest themselves as easily traceable sign changes rather than neighboring absorption peaks, thus overcoming experimental resolution limitations and enabling efficient evaluation of the relevance, validity, and range of applicability of quantum-informed theories for extreme-nanoscale plasmonics.