High-index spherical dielectric nanoparticles are explored as templates for tailoring the fluorescence of nearby electric point-dipole-like emitters. The role of emitter orientation and position around the nanosphere on the modification of both its excitation and its emission rate is studied rigorously through derivation of appropriate analytic solutions. It is shown that dielectric nanoparticles, which support a richness of optical modes of electric or magnetic character and thus a variety of mechanisms for near-field enhancement, provide moderate fluorescence enhancement factors—as compared, e.g., to their plasmonic counterparts—which survive, however, for a wide range of emitter positions and orientations. Understanding the physical mechanisms governing this behaviour, which offers a promising route towards efficient control of the emission properties of randomly arranged emitters, is widely facilitated by the existence of analytic expressions such as the ones derived here. Further enhancement can be achieved by designing nanoparticle-aggregate antennas, or by combining dielectric and plasmonic components.
The tremendous growth of the field of plasmonics in the past twenty years owes much to the pre-existence of solid theoretical foundations. Rather than calling for the introduction of radically new theory and computational techniques, plasmonics required, to a large extent, application of some of the most fundamental laws in physics, namely Maxwell’s equations, albeit adjusted to the nanoscale. The success of this description, which was triggered by the rapid advances in nanofabrication, makes a striking example of new effects and novel applications emerging by applying known physics to a different context. Nevertheless, the prosperous recipe of treating nanostructures within the framework of classical electrodynamics and with use of macroscopic, bulk material response functions (known as the local-response approximation, LRA) has its own limitations, and inevitably fails once the relevant length scales approach the few- to sub-nm regime, dominated by characteristic length scales such as the electron mean free path and the Fermi wavelength. Here we provide a review of the main non-classical effects that emerge when crossing the border between the macroscopic and atomistic worlds. We study the physical mechanisms involved, highlight experimental manifestations thereof and focus on the theoretical efforts developed in the quest for models that implement atomistic descriptions into otherwise classical-electrodynamic calculations for mesoscopic plasmonic nanostructures.
We use time-dependent density functional theory (TDDFT) within the jellium model to study the impact of quantum-mechanical effects on the self-interaction Green’s function that governs the electromagnetic interaction between quantum emitters and plasmonic metallic nanoantennas. A semiclassical model based on the Feibelman parameters, which incorporates quantum surface-response corrections into an otherwise classical description, confirms surface-enabled Landau damping and the spill out of the induced charges as the dominant quantum mechanisms strongly affecting the nanoantenna–emitter interaction. These quantum effects produce a redshift and broadening of plasmonic resonances not present in classical theories that consider a local dielectric response of the metals. We show that the Feibelman approach correctly reproduces the nonlocal surface response obtained by full quantum TDDFT calculations for most nanoantenna–emitter configurations. However, when the emitter is located in very close proximity to the nanoantenna surface, we show that the standard Feibelman approach fails, requiring an implementation that explicitly accounts for the nonlocality of the surface response in the direction parallel to the surface. Our study thus provides a fundamental description of the electromagnetic coupling between plasmonic nanoantennas and quantum emitters at the nanoscale.
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