Engineering strong coupling with molecular coatings in optical nanocavities

Quantum Physics [Submitted on 18 Mar 2026] Engineering strong coupling with molecular coatings in optical nanocavities Athul S. Rema, Adrián E. Rubio López, Felipe Herrera 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. Comments: 15 pages, 6 figures, 4 appendices Subjects: Quantum Physics (quant-ph); Mesoscale and Nanoscale Physics (cond-mat.mes-hall); Chemical Physics (physics.chem-ph) Cite as: arXiv:2603.17269 [quant-ph]   (or arXiv:2603.17269v1 [quant-ph] for this version)   https://doi.org/10.48550/arXiv.2603.17269 Focus to learn more Submission history From: Athul S Rema [view email] [v1] Wed, 18 Mar 2026 01:49:58 UTC (1,829 KB) Access Paper: HTML (experimental) view license Current browse context: quant-ph < prev   |   next > new | recent | 2026-03 Change to browse by: cond-mat cond-mat.mes-hall physics physics.chem-ph References & Citations INSPIRE HEP NASA ADS Google Scholar Semantic Scholar Export BibTeX Citation Bookmark Bibliographic Tools Bibliographic and Citation Tools Bibliographic Explorer Toggle Bibliographic Explorer (What is the Explorer?) Connected Papers Toggle Connected Papers (What is Connected Papers?) Litmaps Toggle Litmaps (What is Litmaps?) scite.ai Toggle scite Smart Citations (What are Smart Citations?) Code, Data, Media Demos Related Papers About arXivLabs Which authors of this paper are endorsers? | Disable MathJax (What is MathJax?)