Effects of Symmetry Breaking and Conductive Contact on the Plasmon Coupling in Gold Nanorod Dimers

Slaughter, Liane Siu; Wu, Yanpeng; Willingham, Britain A.; Nordlander, Peter; Link, Stephan

doi:10.1021/nn1011144

Cited by 228 publications

(313 citation statements)

References 47 publications

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“…In contrast to previous work [20][21][22] we demonstrate full control over symmetric and anti-symmetric optical modes by means of white-light scattering experiments. We experimentally demonstrate the presence of atomic-scale light confinement in these structures by observing an extreme > 800 meV hybridization splitting of corresponding symmetric and antisymmetric dimer modes.…”

contrasting

confidence: 74%

Atomic-Scale Confinement of Resonant Optical Fields

Kern¹,

Großmann²,

Tarakina³

et al. 2012

Nano Lett.

139

157

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2The interaction of light and matter, i.e. absorption and emission of photons, can be considerably enhanced in the presence of strongly localized and therefore highly intense optical near fields 1 .Plasmonic antennas consisting of pairs of closely spaced metal nano particles have gained much attention in this context since they provide the possibility to strongly concentrate optical fields into the gap between the two metal particles [2][3][4] . Pairs of closely spaced metal nanoparticles supporting plasmonic gap resonances consequently find broad applications, e.g. in single-emitter surfaceenhanced spectroscopy 5,6 , quantum optics 7 , extreme nonlinear optics 8-10 , optical trapping 11 , metamaterials 12, 13 and molecular opto-electronics 14 .The success of metal-insulator-metal structures is based on two fundamental properties of their anti-symmetric electromagnetic gap modes. (i) As a direct consequence of the boundary conditions, the dominating field components normal to the metal-dielectric interfaces are sizable only inside the dielectric gap. This means that for anti-symmetric gap modes the achievable field confinement is not limited by the skin depth of the metal, but is solely determined by the actual size of the gap. (ii) Since the free electrons of the metal respond resonantly to an external optical frequency field, enormous surface charge accumulations, accompanied by ultra-intense optical near fields, will occur. In addition, with decreasing gap width, stronger attractive coulomb forces 4 across the gap lead to further surface-charge accumulation and a concomitantly increased near-field intensity enhancement. We therefore conclude that an experimental realization of atomic-scale concentration of electromagnetic fields at visible frequencies is possible but it requires atomic-scale shape control of the field-confining structure, i.e. the gap, as well as a careful assignment and selection of suitable optical modes.Here we achieve atomic-scale confinement of electromagnetic fields at visible frequencies by combining for the first time both atomic-scale shape control of the field confining structure 15 as well as a careful selection and assignment of suitable optical modes [16][17][18] . We study single-crystalline nanorods which self-assemble into side-by-side aligned dimers with gap widths below 0.5 nm. Sideby-side aligned nanorod dimers possess various distinguishable symmetric and anti-symmetric 3 modes in the visible range 19 . In contrast to previous work 20-22 we demonstrate full control over symmetric and anti-symmetric optical modes by means of white-light scattering experiments. We experimentally demonstrate the presence of atomic-scale light confinement in these structures by observing an extreme > 800 meV hybridization splitting of corresponding symmetric and antisymmetric dimer modes. Our results open new perspectives for atomically-resolved spectroscopic imaging, deeply nonlinear optics and attosecond physics, cavity optomechanics and ultra-sensing as well as quantum optics.To obtain nano...

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contrasting

confidence: 74%

Atomic-Scale Confinement of Resonant Optical Fields

Kern¹,

Großmann²,

Tarakina³

et al. 2012

Nano Lett.

139

157

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“…35 Aggregates of nanorods usually produce broad non-Lorentzian spectra, often with more than one longitudinal peak or with a plasmon resonance well shifted from the expected resonance position of a single nanorod. 36,37 Figure 3d shows a fluorescence time trace recorded on the single gold nanorod highlighted in Figure 3c excited with a circularly polarized 633 nm laser. The fluorescence time trace shows bursts that are due to the enhanced fluorescence from the CV molecules passing close to the tips, through the near-field volume of the nanorod.…”

Section: Articlementioning

confidence: 99%

Resonant Plasmonic Enhancement of Single-Molecule Fluorescence by Individual Gold Nanorods

et al. 2014

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Enhancing the fluorescence of a weak emitter is important to further extend the reach of single-molecule fluorescence imaging to many unexplored systems. Here we study fluorescence enhancement by isolated gold nanorods and explore the role of the surface plasmon resonance (SPR) on the observed enhancements. Gold nanorods can be cheaply synthesized in large volumes, yet we find similar fluorescence enhancements as literature reports on lithographically fabricated nanoparticle assemblies. The fluorescence of a weak emitter, crystal violet, can be enhanced more than 1000-fold by a single nanorod with its SPR at 629 nm excited at 633 nm. This strong enhancement results from both an excitation rate enhancement of ∼130 and an effective emission enhancement of ∼9. The fluorescence enhancement, however, decreases sharply when the SPR wavelength moves away from the excitation laser wavelength or when the SPR has only a partial overlap with the emission spectrum of the fluorophore. The reported measurements of fluorescence enhancement by 11 nanorods with varying SPR wavelengths are consistent with numerical simulations.

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“…[19][20][21] Some effects of symmetry breaking have been investigated experimentally in colloidal nanoparticle heterodimers consisting of different sized nanorods and nanospheres. [22][23][24] As an extension of the highly successful dimer gap antenna concept, asymmetric dimers may be of interest for a variety of applications, such as sum-frequency generation, multi-frequency sensors, and Raman scattering. [25][26][27] Here, we present a combined experimental and theoretical study to address the optical response of individual asymmetric dimers both in the linear and nonlinear regime.…”

mentioning

confidence: 99%

Interference, Coupling, and Nonlinear Control of High-Order Modes in Single Asymmetric Nanoantennas

Abb

Wang²,

Albella

et al. 2012

ACS Nano

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We investigate theoretically and experimentally the structure of plasmonic modes in individual asymmetric dimer antennas. Plasmonic near-field coupling of high-order modes results in hybridization of bright and dark modes of the individual nanorods leading to an anticrossing of the coupled resonances. For two bright modes, hybridization results in a capacitive redshift and superradiant broadening. We show that the properties of asymmetric dimers can be used for nonlinear control of spectral modes and demonstrate such a nonlinear effect by measuring the modulation of a hybrid asymmetric dimer -ITO antenna. With use of full electrodynamical calculations we find that the properties of the near-field nonlinear responses are distinctly different from the far field, which opens up new routes for nonlinear control of plasmonic nanosystems.

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Effects of Symmetry Breaking and Conductive Contact on the Plasmon Coupling in Gold Nanorod Dimers

Cited by 228 publications

References 47 publications

Atomic-Scale Confinement of Resonant Optical Fields

Atomic-Scale Confinement of Resonant Optical Fields

Resonant Plasmonic Enhancement of Single-Molecule Fluorescence by Individual Gold Nanorods

Interference, Coupling, and Nonlinear Control of High-Order Modes in Single Asymmetric Nanoantennas

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