Abstract

Abstract Tunable plasmon-exciton coupling is demonstrated at room temperature in hybrid systems consisting of Ag@Au hollow nanoshells (HNSs) and J-aggregates. The strong coupling depends on the exciton binding energy and the localized surface plasmon resonance strength, which can be tuned by changing the thickness of the Ag@Au HNS. An evident anticrossing dispersion curve in the coupled energy diagram of the hybrid system was observed based on the absorption spectra obtained at room temperature. In this paper, strong coupling was observed twice (first at lower wavelength and then also at a higher wavelength) via a single preparation process of the Ag@Au HNS system. The first Rabi splitting energy (ħΩ) is 225 meV. Then, the extinction spectra of the bare Ag@Au HNS and the Ag@Au HNS-J-aggregate hybrid system were reproduced by numerical simulations using the finite-difference time domain method, which were in good agreement with the experimental observations. We attributed the strong coupling of the new shell hybrid system to the reduced local surface plasmon (LSP) mode volume of the Ag@Au HNS. This volume is about 1021.6 nm3. The features of the Ag@Au HNS nanostructure with a small LSP mode volume enabled strong light-matter interactions to be achieved in single open plasmonic nanocavities. These findings may pave the way toward nanophotonic devices operating at room temperature.

Highlights

  • Studies on strong light-matter interactions are interesting

  • The strong coupling depends on the exciton binding energy and the localized surface plasmon resonance strength, which can be tuned by changing the thickness of the Ag@Au hollow nanoshells (HNSs)

  • The extinction spectra of the bare Ag@Au HNS and the Ag@Au HNS-J-aggregate hybrid system were reproduced by numerical simulations using the finite-difference time domain method, which were in good agreement with the experimental observations

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Summary

Introduction

Studies on strong light-matter interactions are interesting. Strong light-matter interactions, which are a focal issue for nanotechnology and modern nanophotonic devices, can be described by cavity quantum electrodynamics (cQED) [1, 2]. cQED lays the foundation for the studies on fundamental quantum science such as quantum information processing [3, 4], quantum networks [5], single-atom lasers [6, 7], and modern nanophotonic devices [8]. The interaction of surface plasmons with quantum emitters is the basis of most of the above light-matter interactions phenomena These interactions can be classified into two principal regimes [3, 9,10,11,12,13]: the weak and strong coupling (SC) regimes. Sun et al.: Strong coupling of Ag@Au hollow nanoshell/J-aggregate to the complexity involved in the design of ­cavity-based systems These harsh conditions can be solved by using noble metal nanoparticles because plasmonic modes can be confined into volumes far below the diffraction limit [21, 22]. We realize light-matter interaction in the SC regime between plasmons confined within Ag@ Au hollow nanoshells (HNS) and molecular excitons in J-aggregates in the solution phase. The effective local surface plasmon (LSP) mode volume of a Ag@Au HNS is estimated to be much smaller than that of a solid Ag or Au sphere with a similar radius

Strong coupling of plasmons and excitons based on experiments
The first strong coupling
The second strong coupling
Strong coupling of plasmons and excitons via FDTD simulations
A nticrossing behavior of plexcitonic states
Electric field distributions
Conclusions
Sample preparation
Characterization

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