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Title: 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:
 [1];  [2];  [3]
  1. Princeton Univ., Princeton, NJ (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. 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}
}

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Cited by: 62 works
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Works referenced in this record:

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Works referencing / citing this record:

Dielectric disorder in two-dimensional materials
journal, August 2019


Dark excitons in transition metal dichalcogenides
text, January 2017


Model Prediction of Self-Rotating Excitons in Two-Dimensional Transition-Metal Dichalcogenides
journal, May 2018


Berry phase modification to the energy spectrum of excitons
text, January 2015


Light–valley interactions in 2D semiconductors
journal, July 2018


Dark excitons in transition metal dichalcogenides
journal, January 2018


Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons
text, January 2017


Dynamics of Free and Localized Excitons in Two‐Dimensional Transition Metal Dichalcogenides
journal, February 2019


Magnetophotoluminescence of exciton Rydberg states in monolayer WS e 2
journal, May 2019


Layer-modulated two-photon absorption in MoS 2 : probing the shift of the excitonic dark state and band-edge
journal, January 2019


Valley-dependent exciton fine structure and Autler–Townes doublets from Berry phases in monolayer MoSe2
journal, August 2019


Berry phase modification to the energy spectrum of excitons
text, January 2018


Triple sum frequency pump-probe spectroscopy of transition metal dichalcogenides
journal, December 2019


Mapping of the dark exciton landscape in transition metal dichalcogenides
journal, July 2018


Colloquium : Excitons in atomically thin transition metal dichalcogenides
text, January 2018


Nonlinear excitonic spin Hall effect in monolayer transition metal dichalcogenides
journal, October 2019


Binding energies and spatial structures of small carrier complexes in monolayer transition-metal dichalcogenides via diffusion Monte Carlo
journal, October 2015


Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla
journal, February 2016


1s-intraexcitonic dynamics in monolayer MoS2 probed by ultrafast mid-infrared spectroscopy
journal, February 2016


Mapping of the dark exciton landscape in transition metal dichalcogenides
text, January 2018


Two-photon absorption in two-dimensional materials: The case of hexagonal boron nitride
journal, October 2018


Brightening the dark excitons
journal, June 2017