Athul S. Rema | Searcharxiv

arXiv2026

Engineering strong coupling with molecular coatings in optical nanocavities

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.

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arXiv2025

Ultrafast single-photon interference with a dipole qubit in a nanocavity

The stationary spectrum of individual dipole emitters in plasmonic nanocavities has been studied for a range of cavity geometries and dipole configurations. Less is known about the coherent dynamics of single photon creation in the nanocavity near field by an excited dipole. We address this gap by developing a Lorentzian kernel approximation that solves the time-dependent Schrödinger equation that describes the coupled dipole-photon dynamics in the single-excitation manifold. Our approach encodes the broadband nature of the nanocavity field through a non-Markovian memory kernel, derived from macroscopic QED theory. For a two-level dipole near a metallic nanosphere, we show that the single photon probability density in frequency space evolves in strong coupling from an initially localized source at the qubit frequency into a Rabi doublet over a timescale governed by the kernel spectrum. This dynamical crossover is accompanied by the formation of single-photon interference patterns in frequency and time, propagating coherently over a timescale limited by the shape of kernel spectrum to $\sim 100-150$ fs, which is accessible to ultrafast spectroscopy. We also show that the stationary spectrum of the coupled system can be manipulated by driving the nanocavity field using coherent pulses with variable spectral bandwidth. Using single-photon pulses narrower than the kernel spectrum, the Rabi splitting in a system that supports strong coupling can be effectively removed. The applicability of our results to other dipole-nanocavity configurations is discussed and a general strong coupling criterion for nanocavities is formulated.

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