Strong multipolar transition enhancement with graphene nanoislands

TL;DR

This paper develops a model to compute multipolar transition rates of quantum emitters near nanostructures, revealing significant enhancement of quadrupolar transitions near graphene nanoislands, challenging traditional dipole-only approximations.

Contribution

It introduces a general Green's function-based model for multipolar transitions, surpassing the point-dipole approximation in complex nanostructured environments.

Findings

Quadrupolar transition rates can surpass dipolar ones by 100 times near graphene nanoislands.

The model captures breakdown of selection rules at the nanoscale.

Enhanced multipolar transitions enable new light-matter interaction regimes.

Abstract

During the past half century, a major approximation was natural in the field of light-matter interaction: the point-dipole model. It was assumed that the wavelength is much larger than the size of the emitting atom or molecule, so that the emitter can be described as a single or a collection of elementary dipoles. As it is legitimate for visible light, the approximation does no longer hold near plasmonic nanostructures, where the effective wavelength can drop below 10 nm. In that case deviations arise from the approximate model. First, the emitter spatial extent influences the far-field spectrum. Second, high-order transitions beyond the dipolar ones are not forbidden anymore. Going beyond the approximation requires intensive numerical efforts to compute the photonic response over the spatial extent of the emitter, since the complete Green's function is required. Here, we develop a general model that computes the multipolar transition rates of a quantum emitter in a photonic environment, by computing the Green's function through an eigenpermittivity modal expansion. We apply the method on graphene nanoislands, and we demonstrate a local breakdown of the selection rules, with quadrupolar transition rates becoming 100 times larger than dipolar ones.