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The evidence of strong coupling between plasmons and molecular excitons forplasmonic nanoparticle (NP) dimers exhibiting ultra-sensitive surface enhancedresonant Raman scattering is the observation of anti-crossing in the coupledresonance. However, it is not easy to experimentally tune plasmon resonance ofsuch dimers for the observation. In this work, we theoretically investigate theanti-crossing properties of the dimers coated by the thin dye films withthicknesses greater than 0.1 nm and gap distances larger than 1.2 nm accordingto the principles of classical electromagnetism. The plasmon resonance spectraof these dimers are strongly affected by their coupling with the excitonresonance of dye molecules. A comparison of the film thickness dependences ofdimer spectral changes with those of silver ellipsoidal NPs indicates that thedipole plasmons localized in the dimer gap are coupled with molecular excitonsof the film much stronger than the dipole plasmons of ellipsoidal NPs.Furthermore, the anti-crossing of coupled resonances is investigated whiletuning plasmon resonance by changing the morphology and refractive index of thesurrounding medium. The spectral changes observed for ellipsoidal NPs clearlyexhibit anti-crossing properties; however, the anti-crossing behavior of dimersis more complex due to the strong coupling of dipoles and higher order plasmonswith multiple molecular excitons. We find that the anti-crossing for dimers isclearly confirmed by the refractive index dependence of coupled resonance.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Anti-crossing properties of strong coupling system of silver  nanoparticle dimers coated with thin dye molecular films analyzed by  classical electromagnetism