Circular Dichroism in Nanoparticle Helices as a Template for Assessing Quantum-Informed Models in Plasmonics

Christos Tserkezis*, A. T.Mina Yeşilyurt, Jer Shing Huang, N. Asger Mortensen

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

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Abstract

As characteristic lengths in plasmonics rapidly approach the sub-nanometer regime, quantum-informed models that can capture those aspects of the quantum nature of the electron gas that are not accessible by the standard approximations of classical electrodynamics, or even go beyond the free-electron description, become increasingly more important. Here we propose a template for comparing and validating the predictions of such models, through the circular dichroism signal of a metallic nanoparticle helix. For illustration purposes, we compare three widely used models, each dominant at different nanoparticle separations and governed by its own physical mechanism, namely, the hydrodynamic Drude model, the generalized nonlocal optical response theory, and the quantum-corrected model for tunneling. Our calculations show that, indeed, each case is characterized by a fundamentally distinctive response, always dissimilar to the predictions of the local optical response approximation of classical electrodynamics, dominated by a model-sensitive absorptive double-peak feature. In circular dichroism spectra, the striking differences between models manifest themselves as easily traceable sign changes rather than neighboring absorption peaks, thus overcoming experimental resolution limitations and enabling efficient evaluation of the relevance, validity, and range of applicability of quantum-informed theories for extreme-nanoscale plasmonics.

Original languageEnglish
JournalACS Photonics
Volume5
Issue number12
Pages (from-to)5017-5024
ISSN2330-4022
DOIs
Publication statusPublished - Nov 2018

Fingerprint

Quantum Theory
Circular Dichroism
helices
dichroism
templates
Electrons
Nanoparticles
nanoparticles
Hydrodynamics
Gases
Electrodynamics
Dichroism
electrodynamics
Electron gas
Quantum theory
predictions
approximation
quantum theory
free electrons
electron gas

Keywords

  • circular dichroism
  • electron tunneling
  • Landau damping
  • nonlocal screening
  • plasmonics nanoparticle helices
  • quantum-informed models

Cite this

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title = "Circular Dichroism in Nanoparticle Helices as a Template for Assessing Quantum-Informed Models in Plasmonics",
abstract = "As characteristic lengths in plasmonics rapidly approach the sub-nanometer regime, quantum-informed models that can capture those aspects of the quantum nature of the electron gas that are not accessible by the standard approximations of classical electrodynamics, or even go beyond the free-electron description, become increasingly more important. Here we propose a template for comparing and validating the predictions of such models, through the circular dichroism signal of a metallic nanoparticle helix. For illustration purposes, we compare three widely used models, each dominant at different nanoparticle separations and governed by its own physical mechanism, namely, the hydrodynamic Drude model, the generalized nonlocal optical response theory, and the quantum-corrected model for tunneling. Our calculations show that, indeed, each case is characterized by a fundamentally distinctive response, always dissimilar to the predictions of the local optical response approximation of classical electrodynamics, dominated by a model-sensitive absorptive double-peak feature. In circular dichroism spectra, the striking differences between models manifest themselves as easily traceable sign changes rather than neighboring absorption peaks, thus overcoming experimental resolution limitations and enabling efficient evaluation of the relevance, validity, and range of applicability of quantum-informed theories for extreme-nanoscale plasmonics.",
keywords = "circular dichroism, electron tunneling, Landau damping, nonlocal screening, plasmonics nanoparticle helices, quantum-informed models",
author = "Christos Tserkezis and Yeşilyurt, {A. T.Mina} and Huang, {Jer Shing} and Mortensen, {N. Asger}",
year = "2018",
month = "11",
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language = "English",
volume = "5",
pages = "5017--5024",
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publisher = "American Chemical Society",
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Circular Dichroism in Nanoparticle Helices as a Template for Assessing Quantum-Informed Models in Plasmonics. / Tserkezis, Christos; Yeşilyurt, A. T.Mina; Huang, Jer Shing; Mortensen, N. Asger.

In: ACS Photonics, Vol. 5, No. 12, 11.2018, p. 5017-5024.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Circular Dichroism in Nanoparticle Helices as a Template for Assessing Quantum-Informed Models in Plasmonics

AU - Tserkezis, Christos

AU - Yeşilyurt, A. T.Mina

AU - Huang, Jer Shing

AU - Mortensen, N. Asger

PY - 2018/11

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N2 - As characteristic lengths in plasmonics rapidly approach the sub-nanometer regime, quantum-informed models that can capture those aspects of the quantum nature of the electron gas that are not accessible by the standard approximations of classical electrodynamics, or even go beyond the free-electron description, become increasingly more important. Here we propose a template for comparing and validating the predictions of such models, through the circular dichroism signal of a metallic nanoparticle helix. For illustration purposes, we compare three widely used models, each dominant at different nanoparticle separations and governed by its own physical mechanism, namely, the hydrodynamic Drude model, the generalized nonlocal optical response theory, and the quantum-corrected model for tunneling. Our calculations show that, indeed, each case is characterized by a fundamentally distinctive response, always dissimilar to the predictions of the local optical response approximation of classical electrodynamics, dominated by a model-sensitive absorptive double-peak feature. In circular dichroism spectra, the striking differences between models manifest themselves as easily traceable sign changes rather than neighboring absorption peaks, thus overcoming experimental resolution limitations and enabling efficient evaluation of the relevance, validity, and range of applicability of quantum-informed theories for extreme-nanoscale plasmonics.

AB - As characteristic lengths in plasmonics rapidly approach the sub-nanometer regime, quantum-informed models that can capture those aspects of the quantum nature of the electron gas that are not accessible by the standard approximations of classical electrodynamics, or even go beyond the free-electron description, become increasingly more important. Here we propose a template for comparing and validating the predictions of such models, through the circular dichroism signal of a metallic nanoparticle helix. For illustration purposes, we compare three widely used models, each dominant at different nanoparticle separations and governed by its own physical mechanism, namely, the hydrodynamic Drude model, the generalized nonlocal optical response theory, and the quantum-corrected model for tunneling. Our calculations show that, indeed, each case is characterized by a fundamentally distinctive response, always dissimilar to the predictions of the local optical response approximation of classical electrodynamics, dominated by a model-sensitive absorptive double-peak feature. In circular dichroism spectra, the striking differences between models manifest themselves as easily traceable sign changes rather than neighboring absorption peaks, thus overcoming experimental resolution limitations and enabling efficient evaluation of the relevance, validity, and range of applicability of quantum-informed theories for extreme-nanoscale plasmonics.

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