Photon echo in exciton-plasmon nanomaterials: A time-dependent signature of strong coupling.

We investigate the dynamics of the photon echo exhibited by exciton-plasmon systems under strong coupling conditions. Using a self-consistent model based on coupled Maxwell-Bloch equations, we investigate the femtosecond time dynamics of ensembles of interacting molecules optically coupled to surface plasmon supporting materials. It is shown that observed photon echoes under a two pulse pump-probe sequence are highly dependent on various material parameters such as molecular concentration and periodicity. Simulations of photon echoes in exciton-plasmon materials reveal a unique signature of the strong exciton-plasmon coupling, namely, a double-peak structure in spectra of recorded echo signals. This phenomenon is shown to be related to hybrid states (upper and lower polaritons) in exciton-plasmon systems under strong coupling conditions. It is also demonstrated that the double-peak echo is highly sensitive to mild deviations of the coupling from resonant conditions making it a great tool for ultrafast probes.