Absence of mutual polariton scatterings for strongly coupled surface plasmon polaritons and dye molecules with large Stokes shift

Abstract

The understanding and control of the dynamics of hybrid modes consisting of strongly coupled surface plasmon polaritons and molecular excitations of dye molecules is of great timely interest, as it allows one to tailor interactions between optical signals as needed for active all-optical devices. Here we utilize dye molecules with an especially large Stokes shift to demonstrate the absence of mutual scatterings among the strongly coupled hybrid modes. We employ a quantum mechanical three-level model and show that the hybrid modes decay via dephasing and internal relaxation of the molecules to a fluorescing state of the dye, which can be used as a measure for the decay. Our results provide essential information about the dynamics of the strongly coupled modes.