Beyond the Quantum Picture: The Electrodynamic Origin of Chiral Nanoplasmonics

TL;DR

This paper demonstrates that a classical electrodynamic model can accurately explain the origin of plasmonic chirality in nanostructures, bridging the gap between quantum and classical descriptions.

Contribution

It introduces a fully atomistic classical electrodynamic model that reproduces experimental chiroptical spectra, supporting an electrodynamic origin of plasmonic chirality.

Findings

The model accurately reproduces experimental spectra across quantum and classical regimes.

Supports a unified electrodynamic explanation for plasmonic chirality.

Enables rational design of chiral nanostructures for specific applications.

Abstract

Chiral plasmonic nanostructures are rapidly emerging as ideal substrates for enantioselective sensing, chiral near-field engineering, and plasmon-assisted catalysis, owing to their exceptional sensitivity to structural handedness. However, the physical origin of plasmonic chirality, whether intrinsically quantum or primarily governed by collective electrodynamics, remains an open question, limiting the development of predictive theoretical methods for the design of novel chiral plasmonic architectures. Here, we show that a fully atomistic classical electrodynamic model, coupling intraband charge transport and interband polarization, quantitatively reproduces state-of-the-art \textit{ab initio} and experimental chiroptical spectra across the quantum-to-classical regime, from atomistically defined chiral Ag and Au nanostructures to DNA-origami-assembled Au nanorods containing up to $\sim 10^5$ atoms. Our results support a unified electrodynamic origin of plasmonic chirality, providing the missing foundation to connect local structural motifs to chiroptical response and local chiral near fields, and paving the way for the atomistically defined, rational design of chiral plasmonic nanostructures optimized for targeted applications.