How nonlocal damping reduces plasmon-enhanced fluorescence in ultranarrow gaps

The nonclassical modification of plasmon-assisted fluorescence enhancement is theoretically explored by placing two-level dipole emitters at the narrow gaps encountered in canonical plasmonic architectures, namely, dimers and trimers of different metallic nanoparticles. Through detailed simulations, in comparison with appropriate analytical modeling, it is shown that within classical electrodynamics and for the reduced separations explored here, fluorescence enhancement factors of the order of 10(5) can be achieved, with a divergent behavior as the particle touching regime is approached. This remarkable prediction is mainly governed by the dramatic increase in excitation rate triggered by the corresponding field enhancement inside the gaps. Nevertheless, once nonclassical corrections are included, the amplification factors decrease by up to two orders of magnitude, and a saturation regime for narrower gaps is reached. These nonclassical limitations are demonstrated by simulations based on the generalized nonlocal optical response theory, which accounts in an efficient way not only for nonlocal screening but also for the enhanced Landau damping near the metal surface. A simple strategy to introduce nonlocal corrections to the analytic solutions is also proposed. It is therefore shown that the nonlocal optical response of the metal imposes more realistic, finite upper bounds to the enhancement feasible with ultrasmall plasmonic cavities, thus providing a theoretical description closer to state-of-the-art experiments.