Surface Plasmon Resonance of Single Gold Nanodimers near the Conductive Contact Limit

Marhaba, Salem; Bachelier, Guillaume; Bonnet, Christophe; Broyer, M.; Cottancin, E.; Grillet, Nadia; Lermé, J.; Vialle, Jean; Pellarin, M.

doi:10.1021/jp810405y

Cited by 99 publications

(138 citation statements)

References 44 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: 76%

Atomic-Scale Confinement of Resonant Optical Fields

Kern¹,

Großmann²,

Tarakina³

et al. 2012

Nano Lett.

137

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: 76%

Atomic-Scale Confinement of Resonant Optical Fields

Kern¹,

Großmann²,

Tarakina³

et al. 2012

Nano Lett.

137

157

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“…Similarly, because of electron tunneling, the QP mode continuously evolves into a higher order charge transfer plasmon mode C2 before direct contact between the nanowires. Thus, already at positive S the nanowires are conductively connected showing characteristic charge transfer plasmon modes [48,[51][52][53]55,56]. For a dimer with a well established conductive contact at negative S, the C1 and C2 modes experience a blue shift with increasing overlap as also found in classical calculations [48,63].…”

Section: Coupled Nanowiressupporting

confidence: 63%

“…The nanoparticles thus appear conductively connected prior to direct contact, and the transition between the non-touching and conductive contact regimes is continuous. In particular, the charge transfer plasmon associated with interparticle charge transfer [51][52][53][54][55][56][57] progressively emerges in the optical response of the system, as has been fully confirmed in recent experiments [28,29]. These quantum effects can be reproduced with the Quantum Corrected Model (QCM) [33] that treats the junction between the nanoparticles as an effective medium mimicking quantum effects within the classical local Maxwell theory [28,29].…”

Section: Introductionmentioning

confidence: 66%

Quantum effects and nonlocality in strongly coupled plasmonic nanowire dimers

et al. 2013

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Abstract:Using a fully quantum mechanical approach we study the optical response of a strongly coupled metallic nanowire dimer for variable separation widths of the junction between the nanowires. The translational invariance of the system allows to apply the time-dependent density functional theory (TDDFT) for nanowires of diameters up to 10 nm which is the largest size considered so far in quantum modeling of plasmonic dimers. By performing a detailed analysis of the optical extinction, induced charge densities, and near fields, we reveal the major nonlocal quantum effects determining the plasmonic modes and field enhancement in the system. These effects consist mainly of electron tunneling between the nanowires at small junction widths and dynamical screening. The TDDFT results are compared with results from classical electromagnetic calculations based on the local Drude and non-local hydrodynamic descriptions of the nanowire permittivity, as well as with results from a recently developed quantum corrected model. The latter provides a way to include quantum mechanical effects such as electron tunneling in standard classical electromagnetic simulations. We show that the TDDFT results can be thus retrieved semi-quantitatively within a classical framework. We also discuss the shortcomings of classical non-local hydrodynamic approaches. Finally, the implications of the actual position of the screening charge density at the gap interfaces are discussed in connection with plasmon ruler applications at subnanometric distances. References and links 1. L. Kelly, E. Coronado, L. L. Zhao, and G. C. Schatz, "The optical properties of metal nanoparticles: the influence of size, shape and dielectric environment," J. Phys. Chem. B 107, 668-667 (2003 B 48, 18178-18188 (1993). 68. P. Apell, and D. R. Penn, "Optical properties of small metal spheres: surface effects," Phys. Rev. Lett. 50, 1316Lett. 50, -1319Lett. 50, (1983. 69. J.-H. Klein-Wiele, P. Simon, and H.-G. Rubahn, "Size-Dependent Plasmon lifetimes and electron-phonon coupling time constants for surface bound Na clusters," Phys. Rev. Lett. 80, 45-48 (1998 B 52, 14219-14234 (1995). 81. L. Serra, and A. Rubio, "Core polarization in the optical response of metal clusters: generalized time-dependent density-functional theory," Phys. Rev. Lett. 78, 1428Lett. 78, -1431Lett. 78, (1997. 82. E. Prodan, P. Nordlander, and N. J. Halas, "Electronic structure and optical properties of Gold nanoshells," Nano Lett. 3, 1411Lett. 3, -1415Lett. 3, (2003. 83. E. Prodan, P. Nordlander, and N. J. Halas, "Effects of dielectric screening on the optical properties of metallic nanoshells," Chem. Phys. Lett. 368, 94-101 (2003). 84. K.-D. Tsuei, E. W. Plummer, A. Liebsch, K. Kempa, and P. Bakshi, "Multipole plasmon modes at a metal surface," Phys. Rev. Lett. 64, 44-47 (1990). 85. A. J. Bennett, "Influence of the electron charge distribution on surface-plasmon dispersion," Phys. 80, 5105-5108 (1998). 88. S. Berciaud, L. Cognet, P. Tamarat, and B. Lounis, "Observation of intrinsic si...

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“…21,23,25,47,48,[50][51][52] The interaction strength between surface plasmons is significantly reduced though when D/r increases from 2.01 to 2.1, as investigated in detail both experimentally and through simulations for the smallest chain lengths of dimers and trimers. 32,[53][54][55] Due to this decrease in coupling, saturation of the redshifting for the lowest energy longitudinal chain mode is predicted to occur at chain lengths as short as 7 NPs and at shorter wavelengths as the interparticle gap increases.…”

Section: Introductionmentioning

confidence: 99%

Plasmonic polymers unraveled through single particle spectroscopy

et al. 2014

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Plasmonic polymers are quasi one-dimensional assemblies of nanoparticles whose optical responses are governed by near-field coupling of localized surface plasmons. Through single particle extinction spectroscopy correlated with electron microscopy, we reveal the effect of the composition of the repeat unit, the chain length, and extent of disorder on the energies, intensities, and line shapes of the collective resonances of individual plasmonic polymers constructed from three different sizes of gold nanoparticles. Our combined experiment and theoretical analysis focuses on the superradiant plasmon mode, which results from the most attractive interactions along the nanoparticle chain and yields the lowest energy resonance in the spectrum. This superradiant mode redshifts with increasing chain length until an infinite chain limit, where additional increases in chain length cause negligible change in the energy of the superradiant mode. We find that, among plasmonic polymers of equal width comprising nanoparticles with different sizes, the onset of the infinite chain limit and its associated energy are dictated by the number of repeat units and not the overall length, of the polymer. The intensities and linewidths of the superradiant mode relative to higher energy resonances, however, differ as the size and number of nanoparticles are varied in the plasmonic polymers studied here. These findings provide general guidelines for engineering the energies, intensities, and line shapes of the collective optical response of plasmonic polymers constructed from nanoparticles with sizes ranging from a few tens to one hundred nanometers.

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Surface Plasmon Resonance of Single Gold Nanodimers near the Conductive Contact Limit

Cited by 99 publications

References 44 publications

Atomic-Scale Confinement of Resonant Optical Fields

Atomic-Scale Confinement of Resonant Optical Fields

Quantum effects and nonlocality in strongly coupled plasmonic nanowire dimers

Plasmonic polymers unraveled through single particle spectroscopy

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