Fano resonance resulting from a tunable interaction between molecular vibrational modes and a double continuum of a plasmonic metamolecule.

Coupling between tunable broadband modes of an array of plasmonic metamolecules and a vibrational mode of carbonyl bond of poly(methyl methacrylate) is shown experimentally to produce a Fano resonance, which can be tuned in situ by varying the polarization of incident light. The interaction between the plasmon modes and the molecular resonance is investigated using both rigorous electromagnetic calculations and a quantum mechanical model describing the quantum interference between a discrete state and two continua. The predictions of the quantum mechanical model are in good agreement with the experimental data and provide an intuitive interpretation, at the quantum level, of the plasmon-molecule coupling.