Probing the Ultimate Limits of Plasmonic Enhancement

Ciracì, Cristian; Hill, Ryan T.; Mock, Jack J.; Urzhumov, Yaroslav; Fernández‐Domínguez, Antonio I.; Maier, Stefan A.; Pendry, J. B.; Chilkoti, Ashutosh; Smith, David R.

doi:10.1126/science.1224823

Cited by 1,044 publications

(1,180 citation statements)

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“…This conclusion is supported by experiments by Scholl et al 28 on silver nanoparticles, where the bonding dipole plasmon was replaced by a charge-transfer plasmon below 0.27 nm. Other experiments on film-coupled nanoparticles 29 found the energy of hybridized modes to be blue shifted relative to the classical result at separations less than 1 nm, a similar blue shifting is anticipated for nanowire dimers within a hydrodynamic description. 30 However, until now, the influence of quantum effects on the spatial shape of the hybridized modes has not been explored.…”

Section: Introductionmentioning

confidence: 66%

Visualizing hybridized quantum plasmons in coupled nanowires: From classical to tunneling regime

et al. 2013

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We present full quantum mechanical calculations of the hybridized plasmon modes of two nanowires at small separation, providing real space visualization of the modes in the transition from the classical to the quantum tunneling regime. The plasmon modes are obtained as certain eigenfunctions of the dynamical dielectric function which is computed using time dependent density functional theory (TDDFT). For freestanding wires, the energy of both surface and bulk plasmon modes deviate from the classical result for low wire radii and high momentum transfer due to effects of electron spill-out, non-local response, and coupling to single-particle transitions. For the wire dimer the shape of the hybridized plasmon modes are continuously altered with decreasing separation, and below 6 Å the energy dispersion of the modes deviate from classical results due to the onset of weak tunneling. Below 2-3 Å separation this mode is replaced by a charge-transfer plasmon which blue shifts with decreasing separation in agreement with experiment, and marks the onset of the strong tunneling regime.

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Section: Introductionmentioning

confidence: 66%

Visualizing hybridized quantum plasmons in coupled nanowires: From classical to tunneling regime

et al. 2013

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“…Nonetheless, for the typical noble metals used in plasmonic experiments, the centroid of the charge is indeed displaced towards the interior of the particles due to the inuence of the bound d-electrons, and the hydrodynamic approach can then be applied for practical purposes. 47 In the following, we describe briey how we introduce the hydrodynamical approach into both the classical local and QCM theoretical frameworks. First, we discuss how the nonlocality is implemented into the optical response.…”

Section: Faraday Discussion Papermentioning

confidence: 99%

“…2,[64][65][66][67][68][69][70][71][72][73] The nonlocal hydrodynamical (NLHD) description has attracted considerable interest because of its numerical efficiency for arbitrarily-shaped objects 47,[74][75][76][77][78][79][80][81][82][83][84] and the possibility to obtain semi-analytical Example of the implementation of QCM in metallic gaps. In (a), a spatially inhomogeneous effective medium whose properties depend continuously on the separation distance is introduced in the gap between two metallic spheres.…”

Section: Introductionmentioning

confidence: 99%

A classical treatment of optical tunneling in plasmonic gaps: extending the quantum corrected model to practical situations

et al. 2015

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(2015). A classical treatment of optical tunneling in plasmonic gaps: extending the quantum corrected model to practical situations. Faraday Discussions, 178, The optical response of plasmonic nanogaps is challenging to address when the separation between the two nanoparticles forming the gap is reduced to a few nanometers or even subnanometer distances. We have compared results of the plasmon response within different levels of approximation, and identified a classical local regime, a nonlocal regime and a quantum regime of interaction. For separations of a fewÅngstroms, in the quantum regime, optical tunneling can occur, strongly modifying the optics of the nanogap. We have considered a classical effective model, so called Quantum Corrected Model (QCM), that has been introduced to correctly describe the main features of optical transport in plasmonic nanogaps. The basics of this model are explained in detail, and its implementation is extended to include nonlocal effects and address practical situations involving different materials and temperatures of operation.

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“…single Au nanocube-film (NC-film) resonators ( Figure 1a) that can squeeze EM fields into an extremely narrow gap (a few nanometers wide, typically less than 100 / λ ) between nanoparticles and a metallic substrate [33][34][35][36][37]. The exceptionally small V significantly enhances the density of optical states, even enabling single molecules strong coupling in the cavity [38].…”

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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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Probing the Ultimate Limits of Plasmonic Enhancement

Cited by 1,044 publications

References 23 publications

Visualizing hybridized quantum plasmons in coupled nanowires: From classical to tunneling regime

Visualizing hybridized quantum plasmons in coupled nanowires: From classical to tunneling regime

A classical treatment of optical tunneling in plasmonic gaps: extending the quantum corrected model to practical situations

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

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