Nonlocal Response of Metallic Nanospheres Probed by Light, Electrons, and Atoms

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Inspired by recent measurements on individual metallic nanospheres that cannot be explained with traditional classical electrodynamics, we theoretically investigate the effects of nonlocal response by metallic nanospheres in three distinct settings: atomic spontaneous emission, electron energy loss spectroscopy, and light scattering. These constitute two near-field and one far-field measurements, with zero-, one-, and two-dimensional excitation sources, respectively. We search for the clearest signatures of hydrodynamic pressure waves in nanospheres. We employ a linearized hydrodynamic model, and Mie–Lorenz theory is applied for each case. Nonlocal response shows its mark in all three configurations, but for the two near-field measurements, we predict especially pronounced nonlocal effects that are not exhibited in far-field measurements. Associated with every multipole order is not only a single blueshifted surface plasmon but also an infinite series of bulk plasmons that have no counterpart in a local-response approximation. We show that these increasingly blueshifted multipole plasmons become spectrally more prominent at shorter probe-to-surface separations and for decreasing nanosphere radii. For selected metals, we predict hydrodynamic multipolar plasmons to be measurable on single nanospheres.
Original languageEnglish
JournalA C S Nano
Volume8
Issue number2
Pages (from-to)1745-1758
ISSN1936-0851
DOIs
Publication statusPublished - 2014

Keywords

  • Nonlocal response
  • Nanoplasmonics
  • EELS
  • Extinction
  • LDOS
  • Spontaneous emission
  • Multipole plasmons

Cite this

@article{a37dce3577ee4905a84aaf5c22f86129,
title = "Nonlocal Response of Metallic Nanospheres Probed by Light, Electrons, and Atoms",
abstract = "Inspired by recent measurements on individual metallic nanospheres that cannot be explained with traditional classical electrodynamics, we theoretically investigate the effects of nonlocal response by metallic nanospheres in three distinct settings: atomic spontaneous emission, electron energy loss spectroscopy, and light scattering. These constitute two near-field and one far-field measurements, with zero-, one-, and two-dimensional excitation sources, respectively. We search for the clearest signatures of hydrodynamic pressure waves in nanospheres. We employ a linearized hydrodynamic model, and Mie–Lorenz theory is applied for each case. Nonlocal response shows its mark in all three configurations, but for the two near-field measurements, we predict especially pronounced nonlocal effects that are not exhibited in far-field measurements. Associated with every multipole order is not only a single blueshifted surface plasmon but also an infinite series of bulk plasmons that have no counterpart in a local-response approximation. We show that these increasingly blueshifted multipole plasmons become spectrally more prominent at shorter probe-to-surface separations and for decreasing nanosphere radii. For selected metals, we predict hydrodynamic multipolar plasmons to be measurable on single nanospheres.",
keywords = "Nonlocal response, Nanoplasmonics, EELS, Extinction, LDOS, Spontaneous emission, Multipole plasmons",
author = "Thomas Christensen and Wei Yan and S{\o}ren Raza and Antti-Pekka Jauho and Mortensen, {N. Asger} and Martijn Wubs",
year = "2014",
doi = "10.1021/nn406153k",
language = "English",
volume = "8",
pages = "1745--1758",
journal = "A C S Nano",
issn = "1936-0851",
publisher = "American Chemical Society",
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}

Nonlocal Response of Metallic Nanospheres Probed by Light, Electrons, and Atoms. / Christensen, Thomas; Yan, Wei; Raza, Søren; Jauho, Antti-Pekka; Mortensen, N. Asger; Wubs, Martijn.

In: A C S Nano, Vol. 8, No. 2, 2014, p. 1745-1758.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Nonlocal Response of Metallic Nanospheres Probed by Light, Electrons, and Atoms

AU - Christensen, Thomas

AU - Yan, Wei

AU - Raza, Søren

AU - Jauho, Antti-Pekka

AU - Mortensen, N. Asger

AU - Wubs, Martijn

PY - 2014

Y1 - 2014

N2 - Inspired by recent measurements on individual metallic nanospheres that cannot be explained with traditional classical electrodynamics, we theoretically investigate the effects of nonlocal response by metallic nanospheres in three distinct settings: atomic spontaneous emission, electron energy loss spectroscopy, and light scattering. These constitute two near-field and one far-field measurements, with zero-, one-, and two-dimensional excitation sources, respectively. We search for the clearest signatures of hydrodynamic pressure waves in nanospheres. We employ a linearized hydrodynamic model, and Mie–Lorenz theory is applied for each case. Nonlocal response shows its mark in all three configurations, but for the two near-field measurements, we predict especially pronounced nonlocal effects that are not exhibited in far-field measurements. Associated with every multipole order is not only a single blueshifted surface plasmon but also an infinite series of bulk plasmons that have no counterpart in a local-response approximation. We show that these increasingly blueshifted multipole plasmons become spectrally more prominent at shorter probe-to-surface separations and for decreasing nanosphere radii. For selected metals, we predict hydrodynamic multipolar plasmons to be measurable on single nanospheres.

AB - Inspired by recent measurements on individual metallic nanospheres that cannot be explained with traditional classical electrodynamics, we theoretically investigate the effects of nonlocal response by metallic nanospheres in three distinct settings: atomic spontaneous emission, electron energy loss spectroscopy, and light scattering. These constitute two near-field and one far-field measurements, with zero-, one-, and two-dimensional excitation sources, respectively. We search for the clearest signatures of hydrodynamic pressure waves in nanospheres. We employ a linearized hydrodynamic model, and Mie–Lorenz theory is applied for each case. Nonlocal response shows its mark in all three configurations, but for the two near-field measurements, we predict especially pronounced nonlocal effects that are not exhibited in far-field measurements. Associated with every multipole order is not only a single blueshifted surface plasmon but also an infinite series of bulk plasmons that have no counterpart in a local-response approximation. We show that these increasingly blueshifted multipole plasmons become spectrally more prominent at shorter probe-to-surface separations and for decreasing nanosphere radii. For selected metals, we predict hydrodynamic multipolar plasmons to be measurable on single nanospheres.

KW - Nonlocal response

KW - Nanoplasmonics

KW - EELS

KW - Extinction

KW - LDOS

KW - Spontaneous emission

KW - Multipole plasmons

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