Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures

P Vasa, R Pomraenke, G Cirmi, E De Re, W Wang, S Schwieger, D Leipold, E Runge, G Cerullo, C Lienau
ACS Nano 2010 December 28, 4 (12): 7559-65
We demonstrate an ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure. Femtosecond excitation drastically alters the optical properties of a model system formed by coating a gold nanoslit array with a thin J-aggregated dye layer. Controlled and reversible transient switching from strong (Ω(R) ≃ 55 meV) to weak (Ω(R) ≈ 0) coupling on a sub-ps time scale is directly evidenced by mapping the nonequilibrium dispersion relations of the coupled excitations. Such a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plasmonic circuits.

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