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The paper investigates strong coupling between quantum emitters and silver nanoparticles by coating the nanoparticles with a thin layer of molecular J-aggregates. This coating restructures the local electromagnetic vacuum at dipole-mode frequencies, enabling Rabi oscillations for quantum emitters that would otherwise only undergo exponential population decay. Using macroscopic quantum electrodynamics theory with a Lorentzian pseudo-mode approximation, the study demonstrates that weak-to-strong coupling crossovers can be induced with 2 nm J-aggregate shells for quantum dot emitters near 20 nm silver nanospheres.
Molecular coatings can restructure the electromagnetic vacuum around nanoparticles, enabling strong coupling and Rabi oscillations where they were previously impossible.
Quantum emitters near the surface of silver nanoparticles undergo Rabi oscillations in electronic population dynamics due to strong coupling with near-field multipole modes that are not radiative. Low-frequency nanoparticle dipole modes are radiative but do not couple strong enough to quantum emitters. These features limit the observation of strong coupling. Using macroscopic quantum electrodynamics theory within a Lorentzian pseudo-mode approximation for the non-Markovian interaction kernel, we demonstrate that by coating spherical silver nanoparticles with a thin molecular J-aggregate layer, the resulting core-shell plexciton resonance restructures the local electromagnetic vacuum at dipole-mode frequencies to enable Rabi oscillations for quantum emitters that otherwise would only undergo exponential population decay. Specifically, we show for quantum dot emitters in the near field of silver nanospheres of 20 nm radius, that weak-to-strong coupling crossovers can be induced using 2 nm J-aggregate shells. Our work demonstrates the potential of molecular aggregates to enable deep sub-wavelength structuring of the vacuum field for the observation of coherent quantum dynamics in optical nanocavities.
