Dynamics of Strong Coupling between J-Aggregates and Surface Plasmon Polaritons in Subwavelength Hole Arrays

A prototypical hybrid system formed by strong coupled gold hole arrays and J-aggregate molecules is investigated by using both steady-state spectroscopic method and ultrafast pump-probe approach. In particular, the plasmonic response of the device has been tuned by modifying its periodicity thus to achieve the strongest possible coupling regime. It is found that in the transient absorption spectra, under upper band excitation, the bleaching signal from uncoupled J-aggregate molecules completely disappears. Instead, two distinctive period dependent bleaching bands are formed, clearly fingerprint of the hybrid exciton-plasmon state. The dynamics of these bands is also directly analyzed. A remarkable long lifetime is found especially for the upper band, corresponding to the presence of a trap state in its transient absorption spectra under resonance excitation. Such unique feature should provide a new approach to control quantum-mechanical states under coherent coupling.