Coupling between electromagnetic cavity fields and fluorescent molecules or quantum emitters can be strongly enhanced by reducing the cavity mode volume. Plasmonic structures allow light confinement down to volumes that are only a few cubic nanometers. At such length scales, nonlocal and quantum tunneling effects are expected to influence the emitter interaction with the surface plasmon modes, which unavoidably requires going beyond classical models to accurately describe the electron response at the metal surface. In this context, the quantum hydrodynamic theory (QHT) has emerged as an efficient tool to probe nonlocal and quantum effects in metallic nanostructures. Here, we apply state-of-the-art QHT to investigate the quantum effects on strong coupling of a dipole emitter placed at nanometer distances from metallic particles. A comparison with conventional local response approximation (LRA) and Thomas-Fermi hydrodynamic theory results shows the importance of quantum effects on the plasmon-emitter coupling. The QHT predicts qualitative deviation from LRA in the weak coupling regime that leads to quantitative differences in the strong coupling regime. In nano-gap systems, the inclusion of quantum broadening leads to the existence of an optimal gap size for Rabi splitting that minimizes the requirements on the emitter oscillator strength.
Plasmonic response of the metallic structure characterized by sub-nanometer dielectric gaps can be strongly affected by nonlocal or quantum effects. In this paper, we investigate these effects in spherical Na and Au nanomatryoshka structures with sub-nanometer core-shell separation. We use the state-of-the-art quantum hydrodynamic theory (QHT) to study both near-field and far-field optical properties of these systems: results are compared with the classical local response approximation (LRA), Thomas-Fermi hydrodynamic theory (TF-HT), and the reference time-dependent density functional theory (TD-DFT). We find that the results obtained using the QHT method are in a very good agreement with TD-DFT calculations, whereas other LRA and TF-HT significantly overestimate the field-enhancements. Thus, the QHT approach efficiently and accurately describes microscopic details of multiscale plasmonic systems whose sizes are computationally out-of-reach for a TD-DFT approach; here, we report results for Na and Au nanomatryoshka with a diameter of 60 nm.
Nonlocal and quantum effects play an important role in accurately modeling the optical response of nanometer-sized metallic nanoparticles. These effects cannot be described by conventional classical theories, as they neglect essential microscopic details. Quantum hydrodynamic theory (QHT) has emerged as an excellent tool to correctly predict the nonlocal and quantum effects by taking into account the spatial dependence of the charge density. In this article, we used a QHT to investigate the impact of nonlocality and electron spill-out on the plasmonic behavior of spherical Na and Au nanoshells. We adopted a self-consistent way to compute the equilibrium charge density. The results predicted by QHT were compared with those obtained with the local response approximation (LRA) and the Thomas–Fermi hydrodynamic theory (TFHT). We found that nonlocal effects have a strong impact on both the near- and far-field optical properties of nanoshells, in particular, for the antibonding resonant mode. We also investigated the optical response of these systems for different thicknesses of the shell, both for Na and Au metals.
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