Collective resonance in helical superstructures of gold nanorods

TL;DR

This paper presents a comprehensive theoretical analysis of collective plasmonic resonances in helical gold nanorod superstructures, revealing polarization-dependent hybridized modes and a universal selection rule for their excitation.

Contribution

It introduces a full theoretical framework for understanding collective resonances in helical nanorod assemblies, including a new selection rule based on symmetry considerations.

Findings

Hybridized resonances depend on light polarization (LCP or RCP).

Multiple hybridized modes evolve into a single collective resonance.

Only one resonance mode is excited for a given circular polarization.

Abstract

Chiroptical responses of helical superstructures are determined by collective behaviors of the individual building blocks. In this paper, we present a full theoretical description of the collective resonance in superstructures. We use the gold nanorods as individual building blocks and arrange them helically along an axis in an end-to-end fashion. Numerical simulations on single-unit cells reveal that the plasmonic coupling between the nanorods produces hybridized resonances, whose intensity is strongly dependent on the excitation light with left- or right-handed circular polarizations (LCP or RCP). A node-mode criterion is proposed on the basis of the microscopic mechanism, which successfully explains the difference between LCP and RCP. We further demonstrate, by repeating the unit cell from 1 to infinity along the helical axis, the multiple hybridized resonances gradually evolve and merge into a single collective resonance, whose energy is also dependent on LCP and RCP. An analytical description is provided for the collective resonance of the helical superstructure on the basis of the coupled dipole approximation method. Our theory shows that n collective resonance modes are present in the helical superstructure with the unit cell consisting of $n$ nanorods. Strikingly, only one resonance can be excited by the incident light with certain circular polarization. We propose a universal selection rule for such selective excitation of the collective resonances by analyzing the symmetry of the helical superstructures. The new insights provided in this work may shed light on future designs and fabrications of helical superstructures using plasmonic building blocks.