Quantum Emitters Near a Metal Nanoparticle: Strong Coupling and Quenching

Delga, A.; Feist, Johannes; Bravo‐Abad, Jorge; García‐Vidal, F. J.

doi:10.1103/physrevlett.112.253601

Cited by 294 publications

(334 citation statements)

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“…2(c,d)], which corresponds to the superposition of multiple highorder plasmonic modes, recently referred to as a 'pseudomode' [27,33]. However, the negligibleγ rad at λ pm shows the largeγ tot comes from emission coupled to the pseudo-mode decaying via non-radiative channels (γ tot =γ rad +γ nr ).…”

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confidence: 99%

Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

et al. 2017

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An emitter in the vicinity of a metal nanostructure is quenched by its decay through non-radiative channels, leading to the belief in a zone of inactivity for emitters placed within <10nm of a plasmonic nanostructure. Here we demonstrate that in tightly-coupled plasmonic resonators forming nanocavities "quenching is quenched" due to plasmon mixing. Unlike isolated nanoparticles, plasmonic nanocavities show mode hybridization which massively enhances emitter excitation and decay via radiative channels. This creates ideal conditions for realizing single-molecule strong-coupling with plasmons, evident in dynamic Rabi-oscillations and experimentally confirmed by laterally dependent emitter placement through DNA-origami.The lifetime of an excited atomic state is determined by the inherent properties of the atom and its environment, first theoretically suggested by Purcell [1] followed by experimental demonstration [2]. Subsequent experiments further verified this by placing atomic emitters within various optical-field-enhancing geometries [3][4][5]. Plasmonic structures have the ability to massively enhance electromagnetic fields, and therefore dramatically alter the excitation rate of an emitter [6]. However, it is well known that placing an emitter close to a plasmonic structure (< 10nm), quenches its fluorescence [7][8][9]. Analysis by Anger et al. [6] showed this is due to the coupling of the emitter to non-radiative higher-order plasmonic modes that dissipate its energy. This 'zone of inactivity' was previously believed to quench all quantum emitters. However, recent advancements have shown that an emitter's emission rate can be enhanced with plasmonic nano-antennas [10][11][12][13][14][15][16][17].Generally a single emitter placed into near-contact with an optical antenna gives larger fluorescence since the antenna efficiently converts far-field radiation into a localized field and vice versa [10,12,13,18]. This was recently demonstrated by Hoang et al. [17] who showed that a quantum dot in a 12nm nano-gap exhibits ultrafast spontaneous emission. What however remains unclear is if this enhanced emission is strong enough to allow for single emitter strong coupling.In this Letter, we demonstrate and explain why quenching is substantially suppressed in plasmonic nanocavities, to such a degree that facilitates lightmatter strong-coupling of single-molecules, even at roomtemperature, as we recently demonstrated experimentally [19]. This is due to: (i) the dramatic increase in the emitter excitation (similar to plasmonic antennas), and (ii) the changed nature of higher-order modes that acquire a radiative component, and therefore increase the quantum yield of the emitter. Modes in plasmonic nanocavities are not a simple superposition of modes from the isolated structures, but instead are hybridplasmonic states [20][21][22][23][24]. Hence, higher-order modes that are dark for an isolated spherical nanoparticle, radiate efficiently for tightly-coupled plasmonic structures [25], significantly reducing the non-radiative...

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Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

et al. 2017

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“…From the experimental side, in recent years, PEPs have been reported in emitter ensembles [10][11][12][13], in which excitonic nonlinearities are negligible [14][15][16]. Only very recently, thanks to advances in the fabrication and characterization of large Purcell enhancement nanocavities [17][18][19], far-field signatures of plasmonexciton strong coupling for single molecules have been reported experimentally [20].…”

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Transformation Optics Approach to Plasmon-Exciton Strong Coupling in Nanocavities

et al. 2016

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We investigate the conditions yielding plasmon-exciton strong coupling at the single emitter level in the gap between two metal nanoparticles. A quasi-analytical transformation optics approach is developed that makes possible a thorough exploration of this hybrid system incorporating the full richness of its plasmonic spectrum. This allows us to reveal that by placing the emitter away from the cavity center, its coupling to multipolar dark modes of both even and odd parity increases remarkably. This way, reversible dynamics in the population of the quantum emitter takes place in feasible implementations of this archetypal nanocavity.PACS numbers: 73.20. Mf, 42.50.Nn, 71.36.+c Plasmon-exciton-polaritons (PEPs) are hybrid lightmatter states that emerge from the electromagnetic (EM) interaction between surface plasmons (SPs) and nearby quantum emitters (QEs) [1,2]. Crucially, PEPs only exist when these two subsystems are strongly coupled, i.e., they exchange EM energy coherently in a time scale much shorter than their characteristic lifetimes. Recently, much attention has focused on PEPs, since they combine the exceptional light concentration ability of SPs with the extreme optical nonlinearity of QEs. These two attributes makes them promising platforms for the next generation of quantum nanophotonic components [3].A quantum electrodynamics description of plasmonic strong coupling of a single QE has been developed for a flat metal surface [4], and isolated [5,6] and distant nanoparticles [7][8][9], where SP hybridization is not fully exploited. From the experimental side, in recent years, PEPs have been reported in emitter ensembles [10][11][12][13], in which excitonic nonlinearities are negligible [14][15][16]. Only very recently, thanks to advances in the fabrication and characterization of large Purcell enhancement nanocavities [17][18][19], far-field signatures of plasmonexciton strong coupling for single molecules have been reported experimentally [20].In this Letter, we theoretically investigate the plasmonic coupling of a single emitter in a paradigmatic cavity: the nanometric gap between two metallic particles [13,19,20]. We consider spherical-shaped nanoparticles, and develop a transformation optics (TO) [21,22] approach that fully accounts for the rich EM spectrum that originates from SP hybridization across the gap. Our method, which is the first application of TO concepts to treat quantum optical phenomena, yields quasianalytical insight into the Wigner-Weisskopf problem [23] for these systems, and enables us to reveal the prescriptions that nanocavities must fulfil to support single QE PEPs. (1) level system (with transition frequency ω E and z-oriented arXiv:1605.09443v2 [cond-mat.mes-hall]

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“…A multiple-scattering method based on macroscopic quantum electrodynamics was used by Delga et al [6,7] to show similar results for a system of single spherical nanoparticle with adjacent fluorescent molecules.…”

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confidence: 70%

“…In the following, we compare the results of our model explained above to a multiple scattering model described in [6,12]. For details, we refer the reader to the supplement of [6], but we outline the main properties of the model here.…”

Section: The Scattering Approachmentioning

confidence: 99%

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Quantum emitter dipole–dipole interactions in nanoplasmonic systems

Nečada

Martikainen

Törmä

2017

Int. J. Mod. Phys. B

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We introduce a generalized Dicke-like model to describe two-level systems coupled with a single bosonic mode. In addition, the two-level systems mutually interact via direct dipole-dipole interaction. We apply the model to an ensemble of dye molecules coupled to a plasmonic excitation in a metallic nanoparticle and study how the dipole-dipole interaction and configurational randomness introduced to the system affect the energy spectra. Comparing the system eigenenergies obtained by our model with the light spectra from a multiple-scattering simulation, we suggest a way to identify dark modes in our model. Finally, we perform a parameter sweep in order to determine the scaling properties of the system and to classify the regions of the parameter space where the dipole-dipole interactions can have significant effects.

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Quantum Emitters Near a Metal Nanoparticle: Strong Coupling and Quenching

Cited by 294 publications

References 32 publications

Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

Transformation Optics Approach to Plasmon-Exciton Strong Coupling in Nanocavities

Quantum emitter dipole–dipole interactions in nanoplasmonic systems

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