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Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling
Strong light–matter coupling provides a promising path for the control of quantum matter where the latter is routinely described from first principles. However, combining the quantized nature of light with this ab initio tool set is challenging and merely developing as the coupled light–matter Hilbe...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2021
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8521676/ https://www.ncbi.nlm.nih.gov/pubmed/34625493 http://dx.doi.org/10.1073/pnas.2110464118 |
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author | Schäfer, Christian Buchholz, Florian Penz, Markus Ruggenthaler, Michael Rubio, Angel |
author_facet | Schäfer, Christian Buchholz, Florian Penz, Markus Ruggenthaler, Michael Rubio, Angel |
author_sort | Schäfer, Christian |
collection | PubMed |
description | Strong light–matter coupling provides a promising path for the control of quantum matter where the latter is routinely described from first principles. However, combining the quantized nature of light with this ab initio tool set is challenging and merely developing as the coupled light–matter Hilbert space is conceptually different and computational cost quickly becomes overwhelming. In this work, we provide a nonperturbative photon-free formulation of quantum electrodynamics (QED) in the long-wavelength limit, which is formulated solely on the matter Hilbert space and can serve as an accurate starting point for such ab initio methods. The present formulation is an extension of quantum mechanics that recovers the exact results of QED for the zero- and infinite-coupling limit and the infinite-frequency as well as the homogeneous limit, and we can constructively increase its accuracy. We show how this formulation can be used to devise approximations for quantum-electrodynamical density-functional theory (QEDFT), which in turn also allows us to extend the ansatz to the full minimal-coupling problem and to nonadiabatic situations. Finally, we provide a simple local density–type functional that takes the strong coupling to the transverse photon degrees of freedom into account and includes the correct frequency and polarization dependence. This QEDFT functional accounts for the quantized nature of light while remaining computationally simple enough to allow its application to a large range of systems. All approximations allow the seamless application to periodic systems. |
format | Online Article Text |
id | pubmed-8521676 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | National Academy of Sciences |
record_format | MEDLINE/PubMed |
spelling | pubmed-85216762021-10-27 Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling Schäfer, Christian Buchholz, Florian Penz, Markus Ruggenthaler, Michael Rubio, Angel Proc Natl Acad Sci U S A Physical Sciences Strong light–matter coupling provides a promising path for the control of quantum matter where the latter is routinely described from first principles. However, combining the quantized nature of light with this ab initio tool set is challenging and merely developing as the coupled light–matter Hilbert space is conceptually different and computational cost quickly becomes overwhelming. In this work, we provide a nonperturbative photon-free formulation of quantum electrodynamics (QED) in the long-wavelength limit, which is formulated solely on the matter Hilbert space and can serve as an accurate starting point for such ab initio methods. The present formulation is an extension of quantum mechanics that recovers the exact results of QED for the zero- and infinite-coupling limit and the infinite-frequency as well as the homogeneous limit, and we can constructively increase its accuracy. We show how this formulation can be used to devise approximations for quantum-electrodynamical density-functional theory (QEDFT), which in turn also allows us to extend the ansatz to the full minimal-coupling problem and to nonadiabatic situations. Finally, we provide a simple local density–type functional that takes the strong coupling to the transverse photon degrees of freedom into account and includes the correct frequency and polarization dependence. This QEDFT functional accounts for the quantized nature of light while remaining computationally simple enough to allow its application to a large range of systems. All approximations allow the seamless application to periodic systems. National Academy of Sciences 2021-10-12 2021-10-08 /pmc/articles/PMC8521676/ /pubmed/34625493 http://dx.doi.org/10.1073/pnas.2110464118 Text en Copyright © 2021 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This open access article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) . |
spellingShingle | Physical Sciences Schäfer, Christian Buchholz, Florian Penz, Markus Ruggenthaler, Michael Rubio, Angel Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling |
title | Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling |
title_full | Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling |
title_fullStr | Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling |
title_full_unstemmed | Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling |
title_short | Making ab initio QED functional(s): Nonperturbative and photon-free effective frameworks for strong light–matter coupling |
title_sort | making ab initio qed functional(s): nonperturbative and photon-free effective frameworks for strong light–matter coupling |
topic | Physical Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8521676/ https://www.ncbi.nlm.nih.gov/pubmed/34625493 http://dx.doi.org/10.1073/pnas.2110464118 |
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