In this review we look at the concepts and state-of-the-art concerning the strong coupling of surface plasmon-polariton modes to states associated with quantum emitters such as excitons in J-aggregates, dye molecules and quantum dots. We explore the phenomenon of strong coupling with reference to a number of examples involving electromagnetic fields and matter. We then provide a concise description of the relevant background physics of surface plasmon polaritons. An extensive overview of the historical background and a detailed discussion of more recent relevant experimental advances concerning strong coupling between surface plasmon polaritons and quantum emitters is then presented. Three conceptual frameworks are then discussed and compared in depth: classical, semi-classical and fully quantum mechanical; these theoretical frameworks will have relevance to strong coupling beyond that involving surface plasmon polaritons. We conclude our review with a perspective on the future of this rapidly emerging field, one we are sure will grow to encompass more intriguing physics and will develop in scope to be of relevance to other areas of science.

https://iopscience.iop.org/article/10.1088/0034-4885/78/1/013901/pdf

Strong coupling between surface plasmon polaritons and emitters: a review

Metals support surface plasmons at optical wavelengths and have the ability to localize light to subwavelength regions. The field enhancements that occur in these regions set the ultimate limitations on a wide range of nonlinear and quantum optical phenomena. We found that the dominant limiting factor is not the resistive loss of the metal, but rather the intrinsic nonlocality of its dielectric response. A semiclassical model of the electronic response of a metal places strict bounds on the ultimate field enhancement. To demonstrate the accuracy of this model, we studied optical scattering from gold nanoparticles spaced a few angstroms from a gold film. The bounds derived from the models and experiments impose limitations on all nanophotonic systems.

https://science.sciencemag.org/content/sci/337/6098/1072.full.pdf

Probing the Ultimate Limits of Plasmonic Enhancement

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Electrodynamics Of Continuous Media

Understanding how light interacts with matter at the nanometre scale is a fundamental issue in optoelectronics and nanophotonics. In particular, many applications (such as bio-sensing, cancer therapy and all-optical signal processing) rely on surface-bound optical excitations in metallic nanoparticles. However, so far no experimental technique has been capable of imaging localized optical excitations with sufficient resolution to reveal their dramatic spatial variation over one single nanoparticle. Here, we present a novel method applied on silver nanotriangles, achieving such resolution by recording maps of plasmons in the near-infrared/visible/ultraviolet domain using electron beams instead of photons. This method relies on the detection of plasmons as resonance peaks in the energy-loss spectra of subnanometre electron beams rastered on nanoparticles of well-defined geometrical parameters. This represents a significant improvement in the spatial resolution with which plasmonic modes can be imaged, and provides a powerful tool in the development of nanometre-level optics.

Mapping surface plasmons on a single metallic nanoparticle

Metallic structures with nanogap features have proven highly effective as building blocks for plasmonic systems, as they can provide a wide tuning range of operating frequencies and large near-field enhancements. Recent work has shown that quantum mechanical effects such as electron tunnelling and nonlocal screening become important as the gap distances approach the subnanometre length-scale. Such quantum effects challenge the classical picture of nanogap plasmons and have stimulated a number of theoretical and experimental studies. This review outlines the findings of many groups into quantum mechanical effects in nanogap plasmons, and discusses outstanding challenges and future directions.

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Quantum mechanical effects in plasmonic structures with subnanometre gaps.

Surface plasmons on metals can concentrate light into subnanometric volumes and on these near atomic length scales the electronic response at the metal interface is smeared out over a Thomas-Fermi screening length. This nonlocality is a barrier to a good understanding of atomic scale response to light and complicates the practical matter of computing the fields. In this Letter, we present a local analogue model and show that spatial nonlocality can be represented by replacing the nonlocal metal with a composite material, comprising a thin dielectric layer on top of a local metal. This method not only makes possible the quantitative analysis of nonlocal effects in complex plasmonic phenomena with unprecedented simplicity and physical insight, but also offers great practical advantages in their numerical treatment.

Surface plasmons and nonlocality: a simple model.

We develop an insightful transformation-optics approach to investigate the impact that nonlocality has on the optical properties of plasmonic nanostructures. The light-harvesting performance of a dimer of touching nanowires is studied by using the hydrodynamical Drude model, which reveals nonlocal resonances not predicted by previous local calculations. Our method clarifies the interplay between radiative and nonlocal effects in this nanoparticle configuration, which enables us to elucidate the optimum size that maximizes its absorption and field enhancement capabilities.

/pdf/transformation-optics-description-of-nonlocal-effects-in-3htvrvuv53.pdf

Transformation-optics description of nonlocal effects in plasmonic nanostructures

The nanofocusing performance of plasmonic tips is studied analytically and numerically. The effects of electron-electron interactions in the dielectric response of the metal are taken into account through the implementation of a nonlocal, spatially dispersive, hydrodynamic permittivity. We demonstrate that spatial dispersion only slightly modifies the device parameters which maximize its field enhancement capabilities. The interplay between nonlocality, tip bluntness, and surface roughness is explored. We show that, although spatial dispersion reduces the field enhancement taking place at the structure apex, it also diminishes the impact that geometric imperfections have on its performance.

Nonlocal effects in the nanofocusing performance of plasmonic tips.

Nanopore sensors embedded within thin dielectric membranes have been gaining significant interest due to their single molecule sensitivity and compatibility of detecting a large range of analytes, from DNA and proteins, to small molecules and particles. Building on this concept we utilize a metallic Au solid-state membrane to translocate and rapidly detect single Au nanoparticles (NPs) functionalized with 589 dye molecules using surface-enhanced resonance Raman spectroscopy (SERRS). We show that, due to the plasmonic coupling between the Au metallic nanopore surface and the NP, signal intensities are enhanced when probing analyte molecules bound to the NP surface. Although not single molecule, this nanopore sensing scheme benefits from the ability of SERRS to provide rich vibrational information on the analyte, improving on current nanopore-based electrical and optical detection techniques. We show that the full vibrational spectrum of the analyte can be detected with ultrahigh spectral sensitivity and a ...

Rapid ultrasensitive single particle surface-enhanced Raman spectroscopy using metallic nanopores.

We investigate the emergence of nonlocal effects in plasmonic nanostructures through electron-energy loss spectroscopy. To theoretically describe the spatial dispersion in the metal permittivity, we develop a full three-dimensional nonlocal hydrodynamic solution of Maxwell’s equations in frequency domain that implements the electron beam as a line current source. We use our numerical approach to perform an exhaustive analysis of the impact of nonlocality in the plasmonic response of single triangular prisms and connected bowtie dimers. Our results demonstrate the complexity of the interplay between nonlocal and geometric effects taking place in these structures. We show the different sensitivities to both effects of the various plasmonic modes supported by these systems. Finally, we present an experimental electron-energy loss study on gold nanoprisms connected by bridges as narrow as 1.6 nm. The comparison with our theoretical predictions enables us to reveal in a phenomenological fashion the enhancement...

Aeneas Wiener

Papers

Surface plasmons and nonlocality: a simple model.

Transformation-optics description of nonlocal effects in plasmonic nanostructures

Nonlocal effects in the nanofocusing performance of plasmonic tips.

Rapid ultrasensitive single particle surface-enhanced Raman spectroscopy using metallic nanopores.

Electron-Energy Loss Study of Nonlocal Effects in Connected Plasmonic Nanoprisms