Distance-Dependent Plasmon Resonant Coupling between a Gold Nanoparticle and Gold Film

Mock, Jack J.; Hill, Ryan T.; Degiron, Aloyse; Zauscher, Stefan; Chilkoti, Ashutosh; Smith, David R.

doi:10.1021/nl080872f

Cited by 499 publications

(600 citation statements)

References 44 publications

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“…1c) shows a doughnutshaped pattern, a typical feature where the electric fields in the gap are vertically excited with respect to the film surface [34]. In contrast, the doped NC-film cavity exhibits a dot-like scattering pattern (inset in Fig.…”

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confidence: 98%

“…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%

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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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confidence: 98%

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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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“…32 This format provides intrinsic control of the orientation of the observable dipolar excitation, as evident from the doughnut shape of the particle image. The reproducible dependence of the plasmon resonance frequency of single nanoparticles on the thickness of the spacer layer points to good *Address correspondence to anne.lazarides@duke.edu.…”

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confidence: 99%

Gold Nanoparticles on Polarizable Surfaces as Raman Scattering Antennas

et al. 2010

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Surface plasmons supported by metal nanoparticles are perturbed by coupling to a surface that is polarizable. Coupling results in enhancement of near fields and may increase the scattering efficiency of radiative modes. In this study, we investigate the Rayleigh and Raman scattering properties of gold nanoparticles functionalized with cyanine deposited on silicon and quartz wafers and on gold thin films. Dark-field scattering images display red shifting of the gold nanoparticle plasmon resonance and doughnut-shaped scattering patterns when particles are deposited on silicon or on a gold film. The imaged radiation patterns and individual particle spectra reveal that the polarizable substrates control both the orientation and brightness of the radiative modes. Comparison with simulation indicates that, in a particle−surface system with a fixed junction width, plasmon band shifts are controlled quantitatively by the permittivity of the wafer or the film. Surface-enhanced resonance Raman scattering (SERRS) spectra and images are collected from cyanine on particles on gold films. SERRS images of the particles on gold films are doughnut-shaped as are their Rayleigh images, indicating that the SERRS is controlled by the polarization of plasmons in the antenna nanostructures. Near-field enhancement and radiative efficiency of the antenna are sufficient to enable Raman scattering cyanines to function as gap field probes. Through collective interpretation of individual particle Rayleigh spectra and spectral simulations, the geometric basis for small observed variations in the wavelength and intensity of plasmon resonant scattering from individual antenna on the three surfaces is explained.

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“…This means that near-field coupling is highly sensitive to inter-particle distance normalized by the size of the particle (r/D) −3 . Hence, the first-order exponential decay Ruler equation has been used to fit the calculated near-field coupling data [17,24]:…”

Section: Near Field Coupling and Ruler Equationmentioning

confidence: 99%

Gap-Dependent Localized High Energy Multiple Dipolar Modes in Passive Silver-Coated Silica Nanoparticle Antennas

et al. 2017

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Abstract:The gap-induced plasmonic response of metallic nanoparticles drastically changes the near and far-field properties of nanoparticle antenna. Similar to a pair of metallic nanostructures, the two nanoparticles, with a dielectric core and silver shell in close proximity, exhibit multiple high energy plasmonic resonances at the short wavelength end of their optical spectrum. In this article, we have overwhelmingly investigated the disparity in the electric field of a core-shell dimer antenna when the gap between nanoparticles within the dimer becomes sub-nanometer in length. We used an electromagnetic planewave to excite the core-shell nanoparticles within the dimer. Frequency domain Finite Element Method (FEM) was employed for the numerical optical analysis of a dimer comprised of two silver-coated silica (SCS) nanoparticles in close proximity, using Computer Simulation Technology (CST) Microwave Studio. A modified Drude model has been used to predict the optical properties of the system with incorporating the size effects. The SCS dimer was numerically analyzed in the visible frequency band, and anomalies in near-field plasmonic coupling were investigated in detail. The inter-surface gap g between nanoparticles within the dimer varied in a range from 0.1 to 402 nm.

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Distance-Dependent Plasmon Resonant Coupling between a Gold Nanoparticle and Gold Film

Cited by 499 publications

References 44 publications

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

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

Gold Nanoparticles on Polarizable Surfaces as Raman Scattering Antennas

Gap-Dependent Localized High Energy Multiple Dipolar Modes in Passive Silver-Coated Silica Nanoparticle Antennas

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