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  Cavity Control of Excitons in Two-Dimensional Materials

Latini, S., Ronca, E., de Giovannini, U., Hübener, H., & Rubio, A. (2019). Cavity Control of Excitons in Two-Dimensional Materials. Nano Letters, 19(6), 3473-3479. doi:10.1021/acs.nanolett.9b00183.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0002-5598-3 Version Permalink: http://hdl.handle.net/21.11116/0000-0005-42C0-7
Genre: Journal Article

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acs.nanolett.9b00183.pdf (Publisher version), 3MB
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This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
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nl9b00183_si_001.pdf (Supplementary material), 2MB
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extensive computational details, convergence tests with respect to the number of excitonic states, number of photons and number of cavity modes included in the calculation, details about the Mott-Wannier methodology, and a comparison between the matter and photon spectral functions
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https://arxiv.org/abs/1810.02672 (Preprint)
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 Creators:
Latini, S.1, 2, 3, Author              
Ronca, E.1, 2, 3, Author              
de Giovannini, U.1, 2, 3, 4, Author              
Hübener, H.1, 2, 3, Author              
Rubio, A.1, 2, 3, 5, Author              
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Center for Free-Electron Laser Science, ou_persistent22              
3Department of Physics, University of Hamburg, ou_persistent22              
4Dipartimento di Fisica e Chimica, Universitá degli Studi di Palermo, ou_persistent22              
5Center for Computational Quantum Physics (CCQ), The Flatiron Institute, ou_persistent22              

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Free keywords: Exciton−polaritons, quantum cavity, QED, transition metal dichalcogenides, Bethe-Salpeter equation, first-principles
 Abstract: We propose a robust and efficient way of controlling the optical spectra of two-dimensional materials and van der Waals heterostructures by quantum cavity embedding. The cavity light-matter coupling leads to the formation of exciton–polaritons, a superposition of photons and excitons. Our first-principles study demonstrates a reordering and mixing of bright and dark excitons spectral features and in the case of a type II van-der-Waals heterostructure an inversion of intra- and interlayer excitonic resonances. We further show that the cavity light-matter coupling strongly depends on the dielectric environment and can be controlled by encapsulating the active two-dimensional (2D) crystal in another dielectric material. Our theoretical calculations are based on a newly developed nonperturbative many-body framework to solve the coupled electron–photon Schrödinger equation in a quantum-electrodynamical extension of the Bethe-Salpeter approach. This approach enables the ab initio simulations of exciton–polariton states and their dispersion from weak to strong cavity light-matter coupling regimes. Our method is then extended to treat van der Waals heterostructures and encapsulated 2D materials using a simplified Mott-Wannier description of the excitons that can be applied to very large systems beyond reach for fully ab initio approaches.

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Language(s): eng - English
 Dates: 2019-04-302019-01-152019-05-022019-06-12
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: arXiv: 1810.02672
DOI: 10.1021/acs.nanolett.9b00183
 Degree: -

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Project name : We are grateful for helpful discussions with Ch. Schäfer, M. Sentef, and M. Ruggenthaler. S.L. acknowledges support from the Alexander von Humboldt foundation. We further acknowledge financial support from the European Research Council (ERC-2015-AdG-694097). The Flatiron Institute is a division of the Simons Foundation.
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Title: Nano Letters
  Abbreviation : Nano Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 19 (6) Sequence Number: - Start / End Page: 3473 - 3479 Identifier: ISSN: 1530-6984
CoNE: https://pure.mpg.de/cone/journals/resource/110978984570403