Strong coupling of surface plasmon resonances to molecules on a gold grating

The intense electromagnetic fields generated by a surface plasmon resonance can strongly couple to molecules in the vicinity of the surface, causing significant line shifts. By measuring the angle dependent transmission spectrum through gold gratings with Rhodamine-6G molecules deposited on them, the coupling of the surface plasmon resonance to the molecular levels at different frequencies was determined. The strong coupling within the absorption and fluorescence bands of the molecules leads to anti-crossing of the states of the coupled system evidenced by the transmission minima. In particular, simultaneous existence of two distinct resonances at different wavevectors for a given wavelength over the absorption and fluorescence bands is observed. The multiplicity of the molecular levels and the coupling fields involved in the process is captured in a three-level Lambda-system model coherently driven by the enhanced surface plasmon fields. The enhanced surface plasmon fields and the resonant absorption/fluorescent fields form the two arms of the Lambda-system with approriate detuning.