A general theoretical and experimental framework for nanoscale electromagnetism

© 2019, The Author(s), under exclusive licence to Springer Nature Limited. The macroscopic electromagnetic boundary conditions, which have been established for over a century1, are essential for the understanding of photonics at macroscopic length scales. Even state-of-the-art nanoplasmonic studies2...

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Main Authors: Yang, Yi, Zhu, Di, Yan, Wei, Agarwal, Akshay, Zheng, Mengjie, Joannopoulos, John D, Lalanne, Philippe, Christensen, Thomas, Berggren, Karl K, Soljačić, Marin
Format: Article
Language:English
Published: Springer Science and Business Media LLC 2021
Online Access:https://hdl.handle.net/1721.1/132450
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author Yang, Yi
Zhu, Di
Yan, Wei
Agarwal, Akshay
Zheng, Mengjie
Joannopoulos, John D
Lalanne, Philippe
Christensen, Thomas
Berggren, Karl K
Soljačić, Marin
author_facet Yang, Yi
Zhu, Di
Yan, Wei
Agarwal, Akshay
Zheng, Mengjie
Joannopoulos, John D
Lalanne, Philippe
Christensen, Thomas
Berggren, Karl K
Soljačić, Marin
author_sort Yang, Yi
collection MIT
description © 2019, The Author(s), under exclusive licence to Springer Nature Limited. The macroscopic electromagnetic boundary conditions, which have been established for over a century1, are essential for the understanding of photonics at macroscopic length scales. Even state-of-the-art nanoplasmonic studies2–4, exemplars of extremely interface-localized fields, rely on their validity. This classical description, however, neglects the intrinsic electronic length scales (of the order of ångström) associated with interfaces, leading to considerable discrepancies between classical predictions and experimental observations in systems with deeply nanoscale feature sizes, which are typically evident below about 10 to 20 nanometres5–10. The onset of these discrepancies has a mesoscopic character: it lies between the granular microscopic (electronic-scale) and continuous macroscopic (wavelength-scale) domains. Existing top-down phenomenological approaches deal only with individual aspects of these omissions, such as nonlocality11–13 and local-response spill-out14,15. Alternatively, bottom-up first-principles approaches—for example, time-dependent density functional theory16,17—are severely constrained by computational demands and thus become impractical for multiscale problems. Consequently, a general and unified framework for nanoscale electromagnetism remains absent. Here we introduce and experimentally demonstrate such a framework—amenable to both analytics and numerics, and applicable to multiscale problems—that reintroduces the electronic length scale via surface-response functions known as Feibelman d parameters18,19. We establish an experimental procedure to measure these complex dispersive surface-response functions, using quasi-normal-mode perturbation theory and observations of pronounced nonclassical effects. We observe nonclassical spectral shifts in excess of 30 per cent and the breakdown of Kreibig-like broadening in a quintessential multiscale architecture: film-coupled nanoresonators, with feature sizes comparable to both the wavelength and the electronic length scale. Our results provide a general framework for modelling and understanding nanoscale (that is, all relevant length scales above about 1 nanometre) electromagnetic phenomena.
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spelling mit-1721.1/1324502021-09-21T03:36:56Z A general theoretical and experimental framework for nanoscale electromagnetism Yang, Yi Zhu, Di Yan, Wei Agarwal, Akshay Zheng, Mengjie Joannopoulos, John D Lalanne, Philippe Christensen, Thomas Berggren, Karl K Soljačić, Marin © 2019, The Author(s), under exclusive licence to Springer Nature Limited. The macroscopic electromagnetic boundary conditions, which have been established for over a century1, are essential for the understanding of photonics at macroscopic length scales. Even state-of-the-art nanoplasmonic studies2–4, exemplars of extremely interface-localized fields, rely on their validity. This classical description, however, neglects the intrinsic electronic length scales (of the order of ångström) associated with interfaces, leading to considerable discrepancies between classical predictions and experimental observations in systems with deeply nanoscale feature sizes, which are typically evident below about 10 to 20 nanometres5–10. The onset of these discrepancies has a mesoscopic character: it lies between the granular microscopic (electronic-scale) and continuous macroscopic (wavelength-scale) domains. Existing top-down phenomenological approaches deal only with individual aspects of these omissions, such as nonlocality11–13 and local-response spill-out14,15. Alternatively, bottom-up first-principles approaches—for example, time-dependent density functional theory16,17—are severely constrained by computational demands and thus become impractical for multiscale problems. Consequently, a general and unified framework for nanoscale electromagnetism remains absent. Here we introduce and experimentally demonstrate such a framework—amenable to both analytics and numerics, and applicable to multiscale problems—that reintroduces the electronic length scale via surface-response functions known as Feibelman d parameters18,19. We establish an experimental procedure to measure these complex dispersive surface-response functions, using quasi-normal-mode perturbation theory and observations of pronounced nonclassical effects. We observe nonclassical spectral shifts in excess of 30 per cent and the breakdown of Kreibig-like broadening in a quintessential multiscale architecture: film-coupled nanoresonators, with feature sizes comparable to both the wavelength and the electronic length scale. Our results provide a general framework for modelling and understanding nanoscale (that is, all relevant length scales above about 1 nanometre) electromagnetic phenomena. 2021-09-20T18:22:28Z 2021-09-20T18:22:28Z 2020-10-30T17:27:38Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/132450 en 10.1038/S41586-019-1803-1 Nature Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf Springer Science and Business Media LLC arXiv
spellingShingle Yang, Yi
Zhu, Di
Yan, Wei
Agarwal, Akshay
Zheng, Mengjie
Joannopoulos, John D
Lalanne, Philippe
Christensen, Thomas
Berggren, Karl K
Soljačić, Marin
A general theoretical and experimental framework for nanoscale electromagnetism
title A general theoretical and experimental framework for nanoscale electromagnetism
title_full A general theoretical and experimental framework for nanoscale electromagnetism
title_fullStr A general theoretical and experimental framework for nanoscale electromagnetism
title_full_unstemmed A general theoretical and experimental framework for nanoscale electromagnetism
title_short A general theoretical and experimental framework for nanoscale electromagnetism
title_sort general theoretical and experimental framework for nanoscale electromagnetism
url https://hdl.handle.net/1721.1/132450
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