Optical properties of coupled metal-semiconductor and metal-molecule nanocrystal complexes: the role of multipole effects

TL;DR

This paper provides a theoretical analysis of exciton-plasmon interactions in hybrid nanocrystals, emphasizing the importance of multipole effects for understanding their optical spectra and interference phenomena.

Contribution

It presents an exact solution beyond the dipole approximation, highlighting the crucial role of multipole interactions in strongly coupled nano-systems.

Findings

Multipole effects significantly influence absorption spectra.

Interference enhances exciton resonance visibility at small distances.

Destructive interference can be observed at room temperature.

Abstract

We investigate theoretically the effects of interaction between an optical dipole (semiconductor quantum dot or molecule) and metal nanoparticles. The calculated absorption spectra of hybrid structures demonstrate strong effects of interference coming from the exciton-plasmon coupling. In particular, the absorption spectra acquire characteristic asymmetric lineshapes and strong anti-resonances. We present here an exact solution of the problem beyond the dipole approximation and find that the multipole treatment of the interaction is crucial for the understanding of strongly-interacting exciton-plasmon nano-systems. Interestingly, the visibility of the exciton resonance becomes greatly enhanced for small inter-particle distances due to the interference phenomenon, multipole effects, and electromagnetic enhancement. We find that the destructive interference is particularly strong. Using our exact theory, we show that the interference effects can be observed experimentally even in the exciting systems at room temperature.