Effective single mode methodology for strongly coupled multimode molecular-plasmon nanosystems

TL;DR

This paper introduces a new theoretical method to accurately model the complex interactions between molecules and multiple plasmonic modes in nanocavities, enabling better understanding and control of hybrid molecular-plasmonic states.

Contribution

A novel, computationally feasible theoretical approach for modeling strong coupling of molecules with multiple plasmonic modes in nanostructures.

Findings

Successfully accounts for multimode effects in molecule-plasmon interactions

Provides insights into the nature of multi-plasmonic mode coupling

Enhances the design of nanoplasmonic systems for sensing and spectroscopy

Abstract

Strong coupling between molecules and quantized fields has emerged as an effective methodology to engineer molecular properties. New hybrid states are formed when molecules interact with quantized fields. Since the properties of these states can be modulated by fine-tuning the field features, an exciting and new side of chemistry can be explored. In particular, significant modifications of the molecular properties can be achieved in plasmonic nanocavities, where the field quantization volume is reduced to sub-nanometric volumes. Intriguing applications of nanoplasmonics include the possibility of coupling the plasmons with a single molecule, instrumental for sensing, high-resolution spectroscopy, and single-molecule imaging. In this work, we focus on phenomena where the simultaneous effects of multiple plasmonic modes are critical. We propose a theoretical methodology to account for many plasmonic modes simultaneously while retaining computational feasibility. Our approach is conceptually simple and allows us to accurately account for the multimode effects and rationalize the nature of the interaction between multiple plasmonic excitations and molecules.