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  Ab Initio Optimized Effective Potentials for Real Molecules in Optical Cavities: Photon Contributions to the Molecular Ground State

Flick, J., Schäfer, C., Ruggenthaler, M., Appel, H., & Rubio, A. (2018). Ab Initio Optimized Effective Potentials for Real Molecules in Optical Cavities: Photon Contributions to the Molecular Ground State. ACS Photonics, 5(3), 992-1005. doi:10.1021/acsphotonics.7b01279.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0001-A740-A Version Permalink: http://hdl.handle.net/21.11116/0000-0003-A4AD-1
Genre: Journal Article

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acsphotonics.7b01279.pdf (Publisher version), 4MB
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https://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html
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2018
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© American Chemical Society

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 Creators:
Flick, J.1, Author              
Schäfer, C.1, Author              
Ruggenthaler, M.1, Author              
Appel, H.1, Author              
Rubio, A.1, 2, Author              
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Center for Computational Quantum Physics (CCQ), The Flatiron Institute, New York, ou_persistent22              

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Free keywords: electronic structure; optimized effective potential; quantum-electrodynamical density-functional theory; strong light−matter coupling
 Abstract: We introduce a simple scheme to efficiently compute photon exchange-correlation contributions due to the coupling to transversal photons as formulated in the newly developed quantum-electrodynamical density-functional theory (QEDFT).(1−5) Our construction employs the optimized-effective potential (OEP) approach by means of the Sternheimer equation to avoid the explicit calculation of unoccupied states. We demonstrate the efficiency of the scheme by applying it to an exactly solvable GaAs quantum ring model system, a single azulene molecule, and chains of sodium dimers, all located in optical cavities and described in full real space. While the first example is a two-dimensional system and allows to benchmark the employed approximations, the latter two examples demonstrate that the correlated electron-photon interaction appreciably distorts the ground-state electronic structure of a real molecule. By using this scheme, we not only construct typical electronic observables, such as the electronic ground-state density, but also illustrate how photon observables, such as the photon number, and mixed electron-photon observables, for example, electron–photon correlation functions, become accessible in a density-functional theory (DFT) framework. This work constitutes the first three-dimensional ab initio calculation within the new QEDFT formalism and thus opens up a new computational route for the ab initio study of correlated electron–photon systems in quantum cavities.

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Language(s): eng - English
 Dates: 2017-10-302018-01-092018-03
 Publication Status: Published in print
 Pages: 14
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acsphotonics.7b01279
 Degree: -

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Project name : We would like to thank Claudiu Genes, Camilla Pellegrini, and Ilya V. Tokatly for insightful discussions and acknowledge financial support from the European Research Council (ERC-2015-AdG-694097), by the European Union’s H2020 program under GA No. 676580 (NOMAD), and the Austrian Science Fund (FWF P25739-N27).
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Title: ACS Photonics
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 5 (3) Sequence Number: - Start / End Page: 992 - 1005 Identifier: Other: 2330-4022
CoNE: /journals/resource/2330-4022