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Updated: May 29, 2026

Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons
Published on: July 21, 2018
Large optical-frequency shift of molecular radiation via coherent coupling to an off-resonance plasmon
Roberto Macovez1, Marina Mariano, Sergio Di Finizio
1ICFO-Institut de Ciencies Fotoniques, Mediterranean Technology Park, Barcelona, Spain. roberto.macovez@upc.edu
Abstract:
We demonstrate coherent optical coupling between molecular and plasmon resonances that are well separated in energy. In the presence of metallic nanoparticles, the second harmonic spectrum of organic dyes no longer peaks at the absorption wavelength but is instead blueshifted by 25 nm towards the localized plasmon resonance. The phase of the light generated by the dyes displays a large modulation across the plasmon resonance and no change across the molecular one. The second harmonic signal contributed by the nanoparticles, which is peaked at the plasmon frequency when no molecules are present, similarly displays a shift towards the molecular resonance in their presence. A model based on the interplay of the nonlinear optical near fields is able to account for these observations.
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