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Robustness of the far-field response of nonlocal plasmonic ensembles

Contrary to classical predictions, the optical response of few-nm plasmonic particles depends on particle size due to effects such as nonlocality and electron spill-out. Ensembles of such nanoparticles are therefore expected to exhibit a nonclassical inhomogeneous spectral broadening due to size dis...

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Autores principales: Tserkezis, Christos, Maack, Johan R., Liu, Zhaowei, Wubs, Martijn, Mortensen, N. Asger
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4916464/
https://www.ncbi.nlm.nih.gov/pubmed/27329703
http://dx.doi.org/10.1038/srep28441
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author Tserkezis, Christos
Maack, Johan R.
Liu, Zhaowei
Wubs, Martijn
Mortensen, N. Asger
author_facet Tserkezis, Christos
Maack, Johan R.
Liu, Zhaowei
Wubs, Martijn
Mortensen, N. Asger
author_sort Tserkezis, Christos
collection PubMed
description Contrary to classical predictions, the optical response of few-nm plasmonic particles depends on particle size due to effects such as nonlocality and electron spill-out. Ensembles of such nanoparticles are therefore expected to exhibit a nonclassical inhomogeneous spectral broadening due to size distribution. For a normal distribution of free-electron nanoparticles, and within the simple nonlocal hydrodynamic Drude model, both the nonlocal blueshift and the plasmon linewidth are shown to be considerably affected by ensemble averaging. Size-variance effects tend however to conceal nonlocality to a lesser extent when the homogeneous size-dependent broadening of individual nanoparticles is taken into account, either through a local size-dependent damping model or through the Generalized Nonlocal Optical Response theory. The role of ensemble averaging is further explored in realistic distributions of isolated or weakly-interacting noble-metal nanoparticles, as encountered in experiments, while an analytical expression to evaluate the importance of inhomogeneous broadening through measurable quantities is developed. Our findings are independent of the specific nonclassical theory used, thus providing important insight into a large range of experiments on nanoscale and quantum plasmonics.
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spelling pubmed-49164642016-06-27 Robustness of the far-field response of nonlocal plasmonic ensembles Tserkezis, Christos Maack, Johan R. Liu, Zhaowei Wubs, Martijn Mortensen, N. Asger Sci Rep Article Contrary to classical predictions, the optical response of few-nm plasmonic particles depends on particle size due to effects such as nonlocality and electron spill-out. Ensembles of such nanoparticles are therefore expected to exhibit a nonclassical inhomogeneous spectral broadening due to size distribution. For a normal distribution of free-electron nanoparticles, and within the simple nonlocal hydrodynamic Drude model, both the nonlocal blueshift and the plasmon linewidth are shown to be considerably affected by ensemble averaging. Size-variance effects tend however to conceal nonlocality to a lesser extent when the homogeneous size-dependent broadening of individual nanoparticles is taken into account, either through a local size-dependent damping model or through the Generalized Nonlocal Optical Response theory. The role of ensemble averaging is further explored in realistic distributions of isolated or weakly-interacting noble-metal nanoparticles, as encountered in experiments, while an analytical expression to evaluate the importance of inhomogeneous broadening through measurable quantities is developed. Our findings are independent of the specific nonclassical theory used, thus providing important insight into a large range of experiments on nanoscale and quantum plasmonics. Nature Publishing Group 2016-06-22 /pmc/articles/PMC4916464/ /pubmed/27329703 http://dx.doi.org/10.1038/srep28441 Text en Copyright © 2016, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Tserkezis, Christos
Maack, Johan R.
Liu, Zhaowei
Wubs, Martijn
Mortensen, N. Asger
Robustness of the far-field response of nonlocal plasmonic ensembles
title Robustness of the far-field response of nonlocal plasmonic ensembles
title_full Robustness of the far-field response of nonlocal plasmonic ensembles
title_fullStr Robustness of the far-field response of nonlocal plasmonic ensembles
title_full_unstemmed Robustness of the far-field response of nonlocal plasmonic ensembles
title_short Robustness of the far-field response of nonlocal plasmonic ensembles
title_sort robustness of the far-field response of nonlocal plasmonic ensembles
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4916464/
https://www.ncbi.nlm.nih.gov/pubmed/27329703
http://dx.doi.org/10.1038/srep28441
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