Cavity Control of Excitons in Two-Dimensional Materials

Latini, S.; Ronca, E.; de Giovannini, U.; Hübener, H.; Rubio, A.

doi:10.1021/acs.nanolett.9b00183

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Cavity Control of Excitons in Two-Dimensional Materials

MPG-Autoren

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Latini, S.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Department of Physics, University of Hamburg;

/persons/resource/persons226551

Ronca, E.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Department of Physics, University of Hamburg;

/persons/resource/persons221949

de Giovannini, U.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Department of Physics, University of Hamburg;
Dipartimento di Fisica e Chimica, Universitá degli Studi di Palermo;

/persons/resource/persons221951

Hübener, H.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Department of Physics, University of Hamburg;

/persons/resource/persons22028

Rubio, A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Department of Physics, University of Hamburg;
Center for Computational Quantum Physics (CCQ), The Flatiron Institute;

Externe Ressourcen

https://arxiv.org/abs/1810.02672
(Preprint)

https://dx.doi.org/10.1021/acs.nanolett.9b00183
(Verlagsversion)

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Zitation

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.

Zitierlink: https://hdl.handle.net/21.11116/0000-0002-5598-3

Zusammenfassung

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.