Strong Coupling between Self-Assembled Molecules and Surface Plasmon Polaritons

We experimentally demonstrate strong coupling between self-assembled PTCDI-C7 organic molecules and the electromagnetic mode generated by surface plasmon polaritons (SPPs). The system consists of a dense self-assembly of ordered molecules evaporated directly on a thin gold film, which stack perpendicularly to the metal surface to form H-aggregates, without a host matrix. Experimental wavevector-resolved reflectance spectra show the formation of hybrid states that display a clear anticrossing, attesting the strong coupling regime with a Rabi splitting energy of Omega(R) similar or equal to 102 meV at room temperature. We demonstrate that the strength of the observed strong coupling regime derives from the high degree of organization of the dense layers of self-assembled molecules at the nanoscale that results in the concentration of the oscillator strength in a charge-transfer Frenkel exciton, with a dipole moment parallel to the direction of the maximum electric field. We compare our results to numerical simulations of a transfer matrix model and reach good qualitative agreement with the experimental findings. In our nanophotonic system, the use of self assembled molecules opens interesting prospects in the context of strong coupling regimes with molecular systems.