Strong coupling of localized plasmons and molecular excitons in nanostructured silver films

NI Cade, T Ritman-Meer, D Richards - Physical Review B—Condensed Matter …, 2009 - APS
NI Cade, T Ritman-Meer, D Richards
Physical Review B—Condensed Matter and Materials Physics, 2009APS
We report on the resonant coupling between localized surface plasmon resonances
(LSPRs) in nanostructured Ag films and an adsorbed monolayer of Rhodamine 6 G dye.
Hybridization of the plasmons and molecular excitons creates new coupled polaritonic
modes, which have been tuned by varying the LSPR wavelength. The resulting polariton
dispersion curve shows an anticrossing behavior which is very well fit by a simple coupled-
oscillator Hamiltonian, giving a giant Rabi-splitting energy of∼ 400 meV. The strength of this …
We report on the resonant coupling between localized surface plasmon resonances (LSPRs) in nanostructured Ag films and an adsorbed monolayer of Rhodamine dye. Hybridization of the plasmons and molecular excitons creates new coupled polaritonic modes, which have been tuned by varying the LSPR wavelength. The resulting polariton dispersion curve shows an anticrossing behavior which is very well fit by a simple coupled-oscillator Hamiltonian, giving a giant Rabi-splitting energy of . The strength of this coupling is shown to be proportional to the square root of the molecular density. The Raman spectra of R6G on these films show an enhancement of many orders of magnitude due to surface enhanced scattering mechanisms; we find a maximum signal when a polariton mode lies in the middle of the Stokes shifted emission band.
American Physical Society
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