Aluminum Nanoantenna Complexes for Strong Coupling between Excitons and Localized Surface Plasmons

Eizner, Elad; Avayu, Ori; Ditcovski, Ran; Ellenbogen, Tal

doi:10.1021/acs.nanolett.5b02584

Cited by 112 publications

(123 citation statements)

References 59 publications

(91 reference statements)

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“…However, the subwavelength field enhancements generated by resonant metallic nanostructures can significantly boost the light-matter coupling. Indeed, strong plasmon-exciton coupling has already been observed [11,13,[22][23][24][25][26][27], but earlier attempts toward achieving plasmon-exciton-polariton (PEP) lasing remained unsuccessful due to the inefficient relaxation mechanism of PEPs and the saturation of strong coupling at large pumping fluences [23]. Here, we demonstrate PEP lasing from an optically pumped array of silver nanoparticles coated by a thin layer of organic molecules at room temperature, occurring at a low threshold [8].…”

Section: Introductionmentioning

confidence: 77%

Plasmon-exciton-polariton lasing

Ramezani¹,

Halpin²,

Fernández‐Domínguez³

et al. 2016

Optica

237

256

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Metallic nanostructures provide a toolkit for the generation of coherent light below the diffraction limit. Plasmonicbased lasing relies on the population inversion of emitters (such as organic fluorophores) along with feedback provided by plasmonic resonances. In this regime, known as weak light-matter coupling, the radiative characteristics of the system can be described by the Purcell effect. Strong light-matter coupling between the molecular excitons and electromagnetic field generated by the plasmonic structures leads to the formation of hybrid quasi-particles known as plasmon-exciton-polaritons (PEPs). Due to the bosonic character of these quasi-particles, exciton-polariton condensation can lead to laser-like emission at much lower threshold powers than in conventional photon lasers. Here, we observe PEP lasing through a dark plasmonic mode in an array of metallic nanoparticles with a low threshold in an optically pumped organic system. Interestingly, the threshold power of the lasing is reduced by increasing the degree of light-matter coupling in spite of the degradation of the quantum efficiency of the active material, highlighting the ultrafast dynamic responsible for the lasing, i.e., stimulated scattering. These results demonstrate a unique roomtemperature platform for exploring the physics of exciton-polaritons in an open-cavity architecture and pave the road toward the integration of this on-chip lasing device with the current photonics and active metamaterial planar technologies.

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Section: Introductionmentioning

confidence: 77%

Plasmon-exciton-polariton lasing

Ramezani¹,

Halpin²,

Fernández‐Domínguez³

et al. 2016

Optica

237

256

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“…Specifically, plasmonic cavities are specially designed metallic nanostructures, in which collective oscillation of conduction electrons, known as localized surface plasmons, can be excited upon illumination. The interaction between plasmonic resonances and nearby atomic or molecular excitons gives rise to so called plexcitonic coupling [16].For convenience of measurements, previous experiments exploring plexcitonic coupling were primarily based on ensemble metallic nanostructures, including arrays of nanovoids [17,18] or nanoparticles (NPs) [19][20][21][22][23] and nanocrystals in solution [16,[24][25][26]. Recently several groups have 3 moved to a much smaller scale, investigating strong interaction of molecular excitons with individual plasmonic resonators, such as metallic nanospheres [27,28], nanorods [29][30][31], nanoprisms [15] and nanodisk dimers [13].…”

mentioning

confidence: 99%

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Chen

Qin

et al. 2017

Nano Lett.

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Plasmonic cavities can be used to control the atom-photon coupling process at the nanoscale, since they provide ultrahigh density of optical states in an exceptionally small mode volume. Here we demonstrate strong coupling between molecular excitons and plasmonic resonances (so-called plexcitonic coupling) in a film-coupled nanocube cavity, which can induce profound and significant spectral and spatial modifications to the plasmonic gap modes. Within the spectral span of a single gap mode in the nanotube-film cavity with a 3-nm wide gap, the introduction of narrow-band J-aggregate dye molecules not only enables an anti-crossing behavior in the spectral response, but also splits the single spatial mode into two distinct modes that are easily identified by their far-field scattering profiles. Simulation results confirm the experimental findings and the sensitivity of the plexcitonic coupling is explored using digital control of the gap spacing. Our work opens up a new perspective to study the strong coupling process, greatly extending the functionality of nanophotonic systems, with the potential to be applied in cavity quantum electrodynamic systems. † These authors contributed equally to this work 2 Strong light-matter interactions build upon fast energy exchange [1] between excitonic quantum emitters and electromagnetic (EM) modes in a cavity, which leads to cavity-exciton mode hybridization, manifesting as a split in the cavity spectral response, known as vacuum Rabi splitting.Understanding these phenomena is very important for cavity quantum electrodynamics applications [2,3]; for example, quantum computing requires repeated manipulation of excitonic states with photons before atomic or molecular excitons lose their coherence. On the other hand, once strongly coupled to a resonant cavity, electronic states of molecules can be greatly reshaped [4] from those in free space, enabling a variety of extraordinary effects, such as modification of molecular thermodynamics [5] and chemical landscape [6], mediation of energy transfer between multiple molecules [7] and even alternation of photosynthetic processes in bacteria [8].Strong coupling (SC) requires a high atomic cooperativity (, where g is the coupling strength, γ and κ are the spectral width of the excitonic transition of emitters and EM modes respectively. To achieve high C, traditional investigations [9][10][11][12] have used cavities with high Q performance (quality factor κ ω / = Q , where ω is the oscillation frequency of the cavity).Another solution is to reduce the cavity mode volume V, sincewhere N is the number of excitons contributing to the coupling process. In this context, plasmonic cavities have been proposed to investigate strong coupling, because these cavities can concentrate light energy within deep subwavelength volumes, and thus are capable of providing high cooperativity by compensating their moderate Q values with ultra-small V [13][14][15]. Specifically, plasmonic cavities are specially designed metallic nanostructures, in w...

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“…4(a,b), the response strongly depends on the orientation of the source, which therefore constitutes a knob to tune in and out of the individual mode resonances or address both modes simultaneously. Please note that the nanometric accuracy in the quantum-emitter positioning required for our scheme is feasible with several current experimental techniques [16,40,41].…”

Section: Appendix A: Simulation Of Spectramentioning

confidence: 99%

Entangled light from bimodal optical nanoantennas

et al. 2017

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We suggest a hybrid plasmonic device made of a bimodal metallic nanoantenna coupled to an incoherently pumped quantum emitter. This device emits light into the two modes entangled in the number of photons. The process is a prime example for losses turning from a nuisance into something beneficial, since, even though counterintuitively, the entanglement is enabled by strong incoherent processes, i.e. dominant scattering and absorption rates of the nanoantenna. This renders the nanoantenna an active source of nonclassicality. Both, the high emission rate and the degree of entanglement of the emitted light are insensitive with respect to imperfections in the nanoantenna length, rendering the scheme feasible for an implementation.

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Aluminum Nanoantenna Complexes for Strong Coupling between Excitons and Localized Surface Plasmons

Cited by 112 publications

References 59 publications

Plasmon-exciton-polariton lasing

Plasmon-exciton-polariton lasing

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Entangled light from bimodal optical nanoantennas

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