Abstract

We demonstrate strong coupling between molecular excited states and surface plasmon modes of a slit array in a thin metal film. The coupling manifests itself as an anticrossing behavior of the two newly formed polaritons. As the coupling strength grows, a new mode emerges, which is attributed to long-range molecular interactions mediated by the plasmonic field. The new, molecular-like mode repels the polariton states, and leads to an opening of energy gaps both below and above the asymptotic free molecule energy.

Highlights

  • We use a self-consistent model and numerically solve the Maxwell-Liouvillevon Neumann equations, where coupling between molecular excitations and metallic surface plasmon polariton (SPP) modes is explicitly taken into account

  • We simulate the SPP-molecular interaction in this strong coupling regime for experimentally realizable parameters and explore its dependence on the dipole strength, the molecular density, and the distance of the molecular layer from the surface

  • We illustrate the conditions under which such new spectral features are expected, and unravel the signatures of the strong coupling regime in the new context of nano-plasmonics

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Summary

Introduction

We study the interaction between plasmonic modes excited within an array of slits in a thin silver film and a layer of molecules deposited in proximity to the surface. We use a self-consistent model and numerically solve the Maxwell-Liouvillevon Neumann equations, where coupling between molecular excitations and metallic surface plasmon polariton (SPP) modes is explicitly taken into account.

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