Engineering strong coupling with molecular coatings in optical nanocavities

Fuente: arXiv
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Autores principales: Rema, Athul S., López, Adrián E. Rubio, Herrera, Felipe
Formato: Preprint
Publicado: 2026
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author Rema, Athul S.
López, Adrián E. Rubio
Herrera, Felipe
author_facet Rema, Athul S.
López, Adrián E. Rubio
Herrera, Felipe
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2603_17269
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Engineering strong coupling with molecular coatings in optical nanocavities
Rema, Athul S.
López, Adrián E. Rubio
Herrera, Felipe
Quantum Physics
Mesoscale and Nanoscale Physics
Chemical Physics
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.
title Engineering strong coupling with molecular coatings in optical nanocavities
topic Quantum Physics
Mesoscale and Nanoscale Physics
Chemical Physics
url https://arxiv.org/abs/2603.17269