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

Journal Article · · Physical Review. B, Condensed Matter and Materials Physics
 [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)

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI ID:
1213377
Report Number(s):
BNL--108047-2015-JA; KC0403020
Journal Information:
Physical Review. B, Condensed Matter and Materials Physics, Journal Name: Physical Review. B, Condensed Matter and Materials Physics Journal Issue: 8 Vol. 92; ISSN 1098-0121
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Chirality and Correlations in Graphene journal June 2007
The electronic properties of graphene journal January 2009
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Theory of Two-Photon Spectroscopy in Solids journal June 1968
Two-photon absorption in quantum-well structures near half the direct band gap journal July 1989
Electron-hole excitations and optical spectra from first principles journal August 2000
Optical matrix elements in tight-binding calculations journal May 2001
Theory of neutral and charged excitons in monolayer transition metal dichalcogenides journal July 2013
Monolayer MoS 2 : Trigonal warping, the Γ valley, and spin-orbit coupling effects journal July 2013
Three-band tight-binding model for monolayers of group-VIB transition metal dichalcogenides journal August 2013
Effective lattice Hamiltonian for monolayer MoS 2 : Tailoring electronic structure with perpendicular electric and magnetic fields journal August 2013
Analytical approach to excitonic properties of MoS 2 journal March 2014
Effect of Coulomb interactions on optical properties of monolayer transition-metal dichalcogenides journal October 2014
Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: MoS 2 , Mo S e 2 , WS 2 , and WS e 2 journal November 2014
Exciton band structure of monolayer MoS 2 journal February 2015
Anisotropic exciton Stark shift in black phosphorus journal April 2015
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Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States journal November 2013
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Cited By (40)

Dynamics of Free and Localized Excitons in Two‐Dimensional Transition Metal Dichalcogenides journal February 2019
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
Brightening the dark excitons journal June 2017
Many-body simulation of two-dimensional electronic spectroscopy of excitons and trions in monolayer transition metal dichalcogenides journal July 2019
Valley-dependent exciton fine structure and Autler–Townes doublets from Berry phases in monolayer MoSe2 journal August 2019
Dielectric disorder in two-dimensional materials journal August 2019
Light–valley interactions in 2D semiconductors journal July 2018
Nonlinear excitonic spin Hall effect in monolayer transition metal dichalcogenides journal October 2019
Triple sum frequency pump-probe spectroscopy of transition metal dichalcogenides journal December 2019
Binding energies and spatial structures of small carrier complexes in monolayer transition-metal dichalcogenides via diffusion Monte Carlo journal October 2015
Optical absorption by Dirac excitons in single-layer transition-metal dichalcogenides journal July 2016
Excitonic Stark effect in MoS 2 monolayers journal December 2016
Intrinsic exciton-state mixing and nonlinear optical properties in transition metal dichalcogenide monolayers journal January 2017
Environmentally sensitive theory of electronic and optical transitions in atomically thin semiconductors journal January 2018
Mapping of the dark exciton landscape in transition metal dichalcogenides journal July 2018
Two-photon absorption in two-dimensional materials: The case of hexagonal boron nitride journal October 2018
Probing many-body interactions in monolayer transition-metal dichalcogenides journal February 2019
Magnetophotoluminescence of exciton Rydberg states in monolayer WS e 2 journal May 2019
Signatures of Bloch-Band Geometry on Excitons: Nonhydrogenic Spectra in Transition-Metal Dichalcogenides journal October 2015
Berry Phase Modification to the Energy Spectrum of Excitons journal October 2015
Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons journal September 2017
Unifying Optical Selection Rules for Excitons in Two Dimensions: Band Topology and Winding Numbers journal February 2018
Model Prediction of Self-Rotating Excitons in Two-Dimensional Transition-Metal Dichalcogenides journal May 2018
Dark excitons in transition metal dichalcogenides journal January 2018
Colloquium : Excitons in atomically thin transition metal dichalcogenides journal April 2018
Berry phase modification to the energy spectrum of excitons text January 2015
Berry phase modification to the energy spectrum of excitons text January 2018
Layer-modulated two-photon absorption in MoS 2 : probing the shift of the excitonic dark state and band-edge journal January 2019
Binding energies and spatial structures of small carrier complexes in monolayer transition metal dichalcogenides via diffusion Monte Carlo text January 2015
Exciton Diamagnetic Shifts and Valley Zeeman Effects in Monolayer WS$_2$ and MoS$_2$ to 65 Tesla text January 2015
Probing Many-Body Interactions in Monolayer Transition-Metal Dichalcogenides text January 2016
Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons text January 2017
Model Prediction of Self-Rotating Excitons in Two-Dimensional Transition-Metal Dichalcogenides text January 2017
Dark excitons in transition metal dichalcogenides text January 2017
Environmentally-Sensitive Theory of Electronic and Optical Transitions in Atomically-Thin Semiconductors text January 2017
Nonlinear excitonic spin Hall effect in monolayer transition metal dichalcogenides preprint January 2018
Mapping of the dark exciton landscape in transition metal dichalcogenides text January 2018
Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons text January 2017
Colloquium : Excitons in atomically thin transition metal dichalcogenides text January 2018