Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides

Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichmann, David R.

doi:10.1103/PhysRevB.92.085413

Title: Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides

Journal Article · Mon Aug 10 00:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PhysRevB.92.085413· OSTI ID:1213377

Berkelbach, Timothy C. ^[1]; Hybertsen, Mark S. ^[2]; Reichmann, David R. ^[3]

Princeton Univ., Princeton, NJ (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Columbia Univ., New York, NY (United States)

We discuss the linear and two-photon spectroscopic selection rules for spin-singlet excitons in monolayer transition-metal dichalcogenides. Our microscopic formalism combines a fully k-dependent few-orbital band structure with a many-body Bethe-Salpeter equation treatment of the electron-hole interaction, using a model dielectric function. We show analytically and numerically that the single-particle, valley-dependent selection rules are preserved in the presence of excitonic effects. Furthermore, we definitively demonstrate that the bright (one-photon allowed) excitons have s-type azimuthal symmetry and that dark p-type excitons can be probed via two-photon spectroscopy. Thus, the screened Coulomb interaction in these materials substantially deviates from the 1/ε₀r form; this breaks the “accidental” angular momentum degeneracy in the exciton spectrum, such that the 2p exciton has a lower energy than the 2s exciton by at least 50 meV. We compare our calculated two-photon absorption spectra to recent experimental measurements.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704; SC0012704

OSTI ID:: 1213377

Alternate ID(s):: OSTI ID: 1209848

Report Number(s):: BNL-108047-2015-JA; R&D Project: 16068; KC0403020

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Vol. 92, Issue 8; ISSN 1098-0121

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 62 works

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