Quenching of the Size Effects in Free and Matrix-Embedded Silver Clusters

Lermé, J.; Palpant, Bruno; Prével, B.; Pellarin, M.; Treilleux, M.; Vialle, Jean; Pérez, A.; Broyer, M.

doi:10.1103/physrevlett.80.5105

Cited by 129 publications

(122 citation statements)

References 17 publications

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“…While for metals that are well described by the jellium model, like for example sodium, the screening charges are located at approximately at 1Å outside the jellium edge (i.e. δ 1Å), for silver and gold, experimental data [32][33][34] seems to suggest that the effect of inner electrons is to push the reach of 5-s (free) electron peak density inside the jellium edge 21 . This would correspond in our model to an overlap of the free and bound electron surfaces (δ 0).…”

Section: Classical Modelmentioning

confidence: 99%

Third-harmonic generation in the presence of classical nonlocal effects in gap-plasmon nanostructures

2015

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Classical nonlocality in conducting nanostructures has been shown to dramatically alter the linear optical response, by placing a fundamental limit on the maximum field enhancement that can be achieved. This limit directly extends to all nonlinear processes, which depend on field amplitudes. A numerical study of third-harmonic generation in metal film-coupled nanowires reveals that for sub-nanometer vacuum gaps the nonlocality may boost the effective nonlinearity by five orders of magnitude as the field penetrates deeper inside the metal than that predicted assuming a purely local electronic response. We also study the impact of a nonlinear dielectric placed in the gap region. In this case the effect of nonlocality could be masked by the third harmonic signal generated by the spacer. By etching the dielectric underneath the nanowire however it is possible to muffle such contribution. Calculations are performed for both silver and gold nanowire.

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Section: Classical Modelmentioning

confidence: 99%

Third-harmonic generation in the presence of classical nonlocal effects in gap-plasmon nanostructures

2015

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“…core [21][22][23]. These effects lead to a reduction of the local values of n e and d , respectively, and thus of the screening of the electron-ion interaction.…”

Section: P H Y S I C a L R E V I E W L E T T E R S Week Ending 2 May mentioning

confidence: 99%

“…Using the bulk material results for the e-ph coupling rate [Eqs. (2) and (3)] and spatially averaging it over the nanoparticle volume using the known parameters for the spillout and d-electron localization effects [21][22][23], a large increase of the average scattering rates is computed in small clusters (Fig. 2).…”

Section: P H Y S I C a L R E V I E W L E T T E R S Week Ending 2 May mentioning

confidence: 99%

Electron-Phonon Scattering in Metal Clusters

et al. 2003

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“…For the free-electron Na surface, the screening charges are located at approximately 0.9 Å (3 Å ) outside the jellium edge (surface atomic layer), meaning that for a Na-Na junction, the effective junction width obtained from matching the measured DP frequency with local classical Drude calculations would be 1.8 Å (6 Å ) smaller than the actual separation between the jellium edges (surface atomic planes). For silver and gold, an analysis of the data on the blueshift of the dipole plasmon resonance in small clusters [9,27,34,44] using Eq. (1) places the effective screening charges inside the jellium edge at 0.8-1.5 Å .…”

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Robust Subnanometric Plasmon Ruler by Rescaling of the Nonlocal Optical Response

et al. 2013

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We present the optical response of two interacting metallic nanowires calculated for separation distances down to angstrom range. State-of-the-art local and nonlocal approaches are compared with full quantum time-dependent density functional theory calculations that give an exact account of nonlocal and tunneling effects. We find that the quantum results are equivalent to those from classical approaches when the nanoparticle separation is defined as the separation between centroids of the screening charges. This establishes a universal plasmon ruler for subnanometric distances. Such a ruler not only impacts the basis of many applications of plasmonics, but also provides a robust rule for subnanometric metrology. DOI: 10.1103/PhysRevLett.110.263901 PACS numbers: 42.25.Bs, 36.40.Gk, 73.20.Mf, 78.67.Bf The exact calculation of the optical response of a nanosystems is a challenging task. In metallic nanostructures the complex nonlocal interactions between conduction electrons modify the standard local classical response, typically characterized by the presence of surface plasmon resonances [1]. This effect is more pronounced in small particles and in strongly coupled systems where the nonlocal nature of electronic interactions is emphasized. To establish an exact and accurate model to describe the spectral features of plasmonic resonances in such systems is thus of paramount importance from both fundamental and practical points of view [2,3]. A variety of theoretical approaches that incorporate different levels of sophistication have been adopted to address the optical response, but certain lack of unification still persists. In particular, the community of surface physics has elaborated accurate nonlocal treatments to address the surface response of conduction electrons of metal surfaces and small metallic objects [1,[4][5][6][7][8][9], whereas the community of nano-optics has focused on developing practical local and nonlocal treatments where the emphasis is placed on the geometrical aspects of the metal boundaries rather than on the actual response of the electrons [2,3,[10][11][12][13][14][15][16]. This Letter bridges both fields, providing a unified and practical picture of the optical response in coupled metallic nanoparticles located at subnanometric proximity.We calculate the optical response of two interacting metallic nanowires in vacuum using a full quantum timedependent density functional theory (TDDFT) approach [17] as well as using macroscopic theory based on solution of classical Maxwell equations with local and nonlocal descriptions of the system. The comparison between quantum and classical results on coupled nanowires provides a perfect basis to unravel the limitations, tendencies, and physics of the optical response under different levels of approximation. By doing so, we are able to relate the results of the optical response from different approximations and predict the influence of nonlocality in the limit of subnanometric distances where nonlocal effects are pronounced. In elucidating the m...

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Quenching of the Size Effects in Free and Matrix-Embedded Silver Clusters

Cited by 129 publications

References 17 publications

Third-harmonic generation in the presence of classical nonlocal effects in gap-plasmon nanostructures

Third-harmonic generation in the presence of classical nonlocal effects in gap-plasmon nanostructures

Electron-Phonon Scattering in Metal Clusters

Robust Subnanometric Plasmon Ruler by Rescaling of the Nonlocal Optical Response

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