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Inelastic Light Scattering by Multiple Vibrational Modes in Individual Gold Nanodimers

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    Inelastic Light Scattering by Multiple Vibrational Modes in Individual Gold Nanodimers
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    • Adrien Girard
      Adrien Girard
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
      More by Adrien Girard
    • Jean Lermé
      Jean Lermé
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
      More by Jean Lermé
    • Hélène Gehan
      Hélène Gehan
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
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    • Alain Mermet
      Alain Mermet
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
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    • Christophe Bonnet
      Christophe Bonnet
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
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    • Emmanuel Cottancin
      Emmanuel Cottancin
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
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      Orcidhttp://orcid.org/0000-0002-1185-770X
    • Aurélien Crut
      Aurélien Crut
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
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      Orcidhttp://orcid.org/0000-0003-2185-709X
    • Jérémie Margueritat*
      Jérémie Margueritat
      Institut Lumière Matière, Université de Lyon, Université Claude Bernard Lyon 1, UMR CNRS 5306, F-69622 Villeurbanne, France
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0003-2075-1875
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2019, 123, 23, 14834–14841
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.9b03090
    Published May 14, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    To be Raman-active (or, more generally, detectable using optical spectroscopy techniques), a vibrational mode of a nanosystem has to modulate its optical response. For small, isolated nanospheres, this is the case for only two categories of vibrational modes, namely, quadrupolar and radial ones. However, assembling nanospheres as dimers makes additional modes Raman-active, as previously demonstrated by the detection in the ultralow frequency range of a hybridized quasi-translation mode in previous measurements on single and ensembles of gold nanosphere dimers. In the present work, we use our recently developed single-particle Raman spectroscopy setup to compare inelastic light scattering by single isolated and dimerized gold nanospheres in an extended frequency range (0–40 GHz). The Raman spectra acquired on isolated nanoparticles present a single peak associated with their fundamental quadrupolar mode, consistently with previous ensemble measurements. In contrast, the spectra measured on dimers are richer and display a number of peaks increasing with decreasing interparticle distance, with all l = 2–8 Lamb modes detected in the quasi-contact case. These observations are rationalized using a recently developed classical model of inelastic light scattering by nanospheres. Importantly, our modeling approach takes into account the real electric field within the nanoparticles (computed using standard or generalized Mie theories) instead of relying on the frequently used Born and quasistatic approximations. This ingredient appears decisive for reaching a qualitative understanding of the measured spectra, explaining in particular the dominance of the l = 2 quadrupolar mode for isolated spheres and the increasing contribution of higher-order modes for increasing electromagnetic interactions in nanosphere dimers.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.9b03090.

    • Determination of the input parameters; analysis of the extinction cross sections; analysis of the low-frequency Raman spectra (LFRS) of the monomer, dimer A, and dimer B; dependence of the LFRS on the interparticle distance in dimers; comments about the dipole-induced-dipole mechanism; phenomenological modeling of the multiple scattering of the Stokes and anti-Stokes photons (PDF)

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    Cited By

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    This article is cited by 14 publications.

    1. Charles Vernier, Lucien Saviot, Yinan Fan, Alexa Courty, Hervé Portalès. Sensitivity of Localized Surface Plasmon Resonance and Acoustic Vibrations to Edge Rounding in Silver Nanocubes. ACS Nano 2023, 17 (20) , 20462-20472. https://doi.org/10.1021/acsnano.3c06990
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    3. Mariana M. Timm, Lucien Saviot, Aurélien Crut, Nicholas Blanchard, Lucian Roiban, Karine Masenelli-Varlot, Lucile Joly-Pottuz, Jérémie Margueritat. Study of Single Gold Nanocrystals by Inelastic Light Scattering Spectroscopy. The Journal of Physical Chemistry C 2022, 126 (7) , 3606-3613. https://doi.org/10.1021/acs.jpcc.2c00077
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    6. Hervé Portalès, Nicolas Goubet, Sandra Casale, Xiang Zhen Xu, Mostapha Ariane, Alain Mermet, Jérémie Margueritat, Lucien Saviot. Inelastic Light Scattering by Long Narrow Gold Nanocrystals: When Size, Shape, Crystallinity, and Assembly Matter. ACS Nano 2020, 14 (4) , 4395-4404. https://doi.org/10.1021/acsnano.9b09993
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    12. A. Noual, R. Akiki, G. Lévêque, Y. Pennec, B. Djafari-Rouhani. Enhanced phonon-plasmon interaction in film-coupled dimer nanoridges mediated by surface acoustic waves. Optics Express 2021, 29 (26) , 43104. https://doi.org/10.1364/OE.444430
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    14. Lucien Saviot. Free Vibrations of Anisotropic Nano-Objects with Rounded or Sharp Corners. Nanomaterials 2021, 11 (7) , 1838. https://doi.org/10.3390/nano11071838
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2019, 123, 23, 14834–14841
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.9b03090
    Published May 14, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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