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A generalized non-local optical response theory for plasmonic nanostructures

Nature Communications volume 5, Article number: 3809 (2014) | Download Citation

Abstract

Metallic nanostructures exhibit a multitude of optical resonances associated with localized surface plasmon excitations. Recent observations of plasmonic phenomena at the sub-nanometre to atomic scale have stimulated the development of various sophisticated theoretical approaches for their description. Here instead we present a comparatively simple semiclassical generalized non-local optical response theory that unifies quantum pressure convection effects and induced charge diffusion kinetics, with a concomitant complex-valued generalized non-local optical response parameter. Our theory explains surprisingly well both the frequency shifts and size-dependent damping in individual metallic nanoparticles as well as the observed broadening of the crossover regime from bonding-dipole plasmons to charge-transfer plasmons in metal nanoparticle dimers, thus unravelling a classical broadening mechanism that even dominates the widely anticipated short circuiting by quantum tunnelling. We anticipate that our theory can be successfully applied in plasmonics to a wide class of conducting media, including doped semiconductors and low-dimensional materials such as graphene.

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Acknowledgements

We acknowledge Giuseppe Toscano for use of his finite-element code and we thank Jørn Hvam, Antti-Pekka Jauho and Wei Yan for stimulating discussions. The Center for Nanostructured Graphene (CNG) is funded by the Danish National Research Foundation, Project DNRF58. The A P Møller and Chastine Mc-Kinney Møller Foundation is gratefully acknowledged for the contribution towards the establishment of the Center for Electron Nanoscopy. N.A.M. and M.W. acknowledge financial support by Danish Council for Independent Research—Natural Sciences, Project 1323-00087.

Author information

Affiliations

  1. Department of Photonics Engineering, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark

    • N. A. Mortensen
    • , S. Raza
    •  & M. Wubs
  2. Center for Nanostructured Graphene (CNG), Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark

    • N. A. Mortensen
    •  & M. Wubs
  3. Center for Electron Nanoscopy, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark

    • S. Raza
  4. Department of Physics and Nanotechnology, Aalborg University, DK-9220 Aalborg, Denmark

    • T. Søndergaard
  5. Department of Technology and Innovation, University of Southern Denmark, DK-5230 Odense, Denmark

    • S. I. Bozhevolnyi

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Contributions

N.A.M, S.I.B, T.S. and M.W. conceived the basic idea. N.A.M. derived the complex response model. S.R. performed all numerical simulations and the analytical analysis of spherical particles. Figures were prepared by N.A.M. and S.R. All authors interpreted and discussed the results and the writing of the manuscript was done in a joint effort.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to N. A. Mortensen.

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    Supplementary Information

    Supplementary Figures 1-2, Supplementary Table 1, Supplementary Notes 1-3 and Supplementary References

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https://doi.org/10.1038/ncomms4809

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