Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides
Abstract
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.
- Authors:
-
- Princeton Univ., Princeton, NJ (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1213377
- Alternate Identifier(s):
- OSTI ID: 1209848
- Report Number(s):
- BNL-108047-2015-JA
Journal ID: ISSN 1098-0121; R&D Project: 16068; KC0403020
- Grant/Contract Number:
- SC00112704; SC0012704
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Physical Review. B, Condensed Matter and Materials Physics
- Additional Journal Information:
- Journal Volume: 92; Journal Issue: 8; Journal ID: ISSN 1098-0121
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Berkelbach, Timothy C., Hybertsen, Mark S., and Reichmann, David R. Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides. United States: N. p., 2015.
Web. doi:10.1103/PhysRevB.92.085413.
Berkelbach, Timothy C., Hybertsen, Mark S., & Reichmann, David R. Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides. United States. https://doi.org/10.1103/PhysRevB.92.085413
Berkelbach, Timothy C., Hybertsen, Mark S., and Reichmann, David R. 2015.
"Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides". United States. https://doi.org/10.1103/PhysRevB.92.085413. https://www.osti.gov/servlets/purl/1213377.
@article{osti_1213377,
title = {Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides},
author = {Berkelbach, Timothy C. and Hybertsen, Mark S. and Reichmann, David R.},
abstractNote = {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.},
doi = {10.1103/PhysRevB.92.085413},
url = {https://www.osti.gov/biblio/1213377},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 8,
volume = 92,
place = {United States},
year = {Mon Aug 10 00:00:00 EDT 2015},
month = {Mon Aug 10 00:00:00 EDT 2015}
}
Web of Science
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