We introduce a theory to analyze the behavior of light emitters in nanostructured environments rigorously. Based on spectral theory, the approach opens the possibility to quantify precisely how an emitter decays to resonant states of the structure and how it couples to a background, also in the presence of general dispersive media. Quantification on this level is essential for designing and analyzing topical nanophotonic setups, e.g., in quantum technology applications. We use a numerical implementation of the theory for computing modal and background decay rates of a single-photon emitter in a diamond nanoresonator.
Optical resonators are widely used in modern photonics. Their spectral response and temporal dynamics are fundamentally driven by their natural resonances, the so-called quasinormal modes (QNMs), with complex frequencies.For optical resonators made of dispersive materials, the QNM computation requires solving a nonlinear eigenvalue problem. This rises a difficulty that is only scarcely documented in the literature. We review our recent efforts for implementing efficient and accurate QNM-solvers for computing and normalizing the QNMs of micro-and nanoresonators made of highly-dispersive materials. We benchmark several methods for three geometries, a twodimensional plasmonic crystal, a two-dimensional metal grating, and a three-dimensional nanopatch antenna on a metal substrate, in the perspective to elaborate standards for the computation of resonance modes.
Circular dichroism (CD) has long been used to trace chiral molecular states and changes of protein configurations. In recent years, chiral plasmonic nanostructures have shown potential for applications ranging from pathogen sensing to novel optical materials. The plasmonic coupling of the individual elements of such metallic structures is a crucial prerequisite to obtain sizeable CD signals. We here identify and implement various coupling entities—chiral and achiral—to demonstrate chiral transfer over distances close to 100 nm. The coupling is realized by an achiral nanosphere situated between a pair of gold nanorods that are arranged far apart but in a chiral fashion using DNA origami. The transmitter particle causes a strong enhancement of the CD response, the emergence of an additional chiral feature at the resonance frequency of the nanosphere, and a redshift of the longitudinal plasmonic resonance frequency of the nanorods. Matching numerical simulations elucidate the intricate chiral optical fields in complex architectures.
Strong coupling of plasmonic excitations and dipolar emitters, such as organic molecules, have been studied extensively in the last years. The questions whether strong coupling can be achieved with a single molecule only and how this is unambiguously proven are still under debate. A critical issue of plasmonic in contrast to photonic systems is additional excitonic line broadening, which is often neglected when modeling such systems. This has led to too optimistic design predictions or incorrect interpretation of ambiguous experimental data, for example in models relying on Maxwell solvers without self-consistent incorporation of line broadening effects. In this paper, we present a heuristic modeling approach for strongly coupled systems based on plasmonic nanoparticles and dipolar emitters that accounts for such broadening and elucidates on recent experiments with single emitters. We explicitly focus on a clear and intuitive classical description that utilizes well-established methods, easy to use within typical Maxwell solvers. The heuristic model (i) provides experimentally relevant numbers like arXiv:1904.04584v1 [physics.optics] 9 Apr 2019 emitter densities and spectra (ii) allows to discriminate systems, which can reach the strong coupling regime from those, which can not (iii) allows to identify optimization routes and (iv) nicely matches with experimental findings. In particular, we employ an approach related to quasi normal modes and extinction simulations where the excitonic system is represented by a frequency dependent permittivity. As examples, we investigate two configurations with many, but also single emitters, which have been studied in recent experiments. Keywordssurface plasmons, nanoantenna, strong coupling, Purcell effect, quantum optics Strong coupling (SC) of single emitters and photonic cavities 1 has been theoretically
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