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Title: Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor

Abstract

In this paper, we report 65 T magnetoabsorption spectroscopy of exciton Rydberg states in the archetypal monolayer semiconductor WSe 2 . The strongly field-dependent and distinct energy shifts of the 2 s , 3 s , and 4 s excited neutral excitons permits their unambiguous identification and allows for quantitative comparison with leading theoretical models. Both the sizes (via low-field diamagnetic shifts) and the energies of the n s exciton states agree remarkably well with detailed numerical simulations using the nonhydrogenic screened Keldysh potential for 2D semiconductors. Finally and moreover, at the highest magnetic fields, the nearly linear diamagnetic shifts of the weakly bound 3 s and 4 s excitons provide a direct experimental measure of the exciton’s reduced mass m r = 0.20 ± 0.01 m 0 .

Authors:
 [1];  [2];  [3];  [4];  [2];  [1]
  1. National High Magnetic Field Lab. (MagLab), Los Alamos, NM (United States)
  2. Univ. of Washington, Seattle, WA (United States). Dept. of Physics
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Rice Univ., Houston, TX (United States). Dept. of Electrical and Computer Engineering. Dept. of Physics and Astronomy. Dept. of Materials Science and NanoEngineering
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Washington, Seattle, WA (United States); National High Magnetic Field Lab. (MagLab), Los Alamos, NM (United States); Rice Univ., Houston, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1475347
Alternate Identifier(s):
OSTI ID: 1419092
Report Number(s):
LA-UR-17-27395
Journal ID: ISSN 0031-9007
Grant/Contract Number:  
AC52-06NA25396; SC0018171; DMR-1157490; FA9550-14-1-0268
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 5; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; diamagnetism; excitons; magneto-optical spectra; Zeeman effect; 2-dimensional systems; transition-metal dichalcogenide

Citation Formats

Stier, A. V., Wilson, N. P., Velizhanin, K. A., Kono, J., Xu, X., and Crooker, S. A. Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.057405.
Stier, A. V., Wilson, N. P., Velizhanin, K. A., Kono, J., Xu, X., & Crooker, S. A. Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor. United States. doi:10.1103/PhysRevLett.120.057405.
Stier, A. V., Wilson, N. P., Velizhanin, K. A., Kono, J., Xu, X., and Crooker, S. A. Thu . "Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor". United States. doi:10.1103/PhysRevLett.120.057405. https://www.osti.gov/servlets/purl/1475347.
@article{osti_1475347,
title = {Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor},
author = {Stier, A. V. and Wilson, N. P. and Velizhanin, K. A. and Kono, J. and Xu, X. and Crooker, S. A.},
abstractNote = {In this paper, we report 65 T magnetoabsorption spectroscopy of exciton Rydberg states in the archetypal monolayer semiconductor WSe2. The strongly field-dependent and distinct energy shifts of the 2s, 3s, and 4s excited neutral excitons permits their unambiguous identification and allows for quantitative comparison with leading theoretical models. Both the sizes (via low-field diamagnetic shifts) and the energies of the ns exciton states agree remarkably well with detailed numerical simulations using the nonhydrogenic screened Keldysh potential for 2D semiconductors. Finally and moreover, at the highest magnetic fields, the nearly linear diamagnetic shifts of the weakly bound 3s and 4s excitons provide a direct experimental measure of the exciton’s reduced mass mr=0.20±0.01m0.},
doi = {10.1103/PhysRevLett.120.057405},
journal = {Physical Review Letters},
number = 5,
volume = 120,
place = {United States},
year = {2018},
month = {2}
}

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Works referenced in this record:

Exciton spectra in thin crystals: the diamagnetic effect
journal, June 1967


Coupled Spin and Valley Physics in Monolayers of MoS 2 and Other Group-VI Dichalcogenides
journal, May 2012


Charged excitons in monolayer WSe 2 : Experiment and theory
journal, August 2017


Giant Enhancement of the Optical Second-Harmonic Emission of WSe 2 Monolayers by Laser Excitation at Exciton Resonances
journal, March 2015


Hydrogenic energy levels in two dimensions at arbitrary magnetic fields
journal, June 1986


Normal Modes in Hexagonal Boron Nitride
journal, June 1966


Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014


Unconventional Quantum Hall Effect and Tunable Spin Hall Effect in Dirac Materials: Application to an Isolated MoS 2 Trilayer
journal, February 2013


Interlayer electron–phonon coupling in WSe2/hBN heterostructures
journal, October 2016

  • Jin, Chenhao; Kim, Jonghwan; Suh, Joonki
  • Nature Physics, Vol. 13, Issue 2
  • DOI: 10.1038/nphys3928

Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

  • Xu, Xiaodong; Yao, Wang; Xiao, Di
  • Nature Physics, Vol. 10, Issue 5
  • DOI: 10.1038/nphys2942

Observation of Excitonic Rydberg States in Monolayer MoS 2 and WS 2 by Photoluminescence Excitation Spectroscopy
journal, April 2015

  • Hill, Heather M.; Rigosi, Albert F.; Roquelet, Cyrielle
  • Nano Letters, Vol. 15, Issue 5
  • DOI: 10.1021/nl504868p

Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment
journal, November 2015


Dielectric screening in two-dimensional insulators: Implications for excitonic and impurity states in graphane
journal, August 2011


Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016


Exciton Binding Energy of Monolayer WS2
journal, March 2015

  • Zhu, Bairen; Chen, Xi; Cui, Xiaodong
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep09218

Valley- and spin-polarized Landau levels in monolayer WSe2
journal, October 2016


Binding energies of trions and biexcitons in two-dimensional semiconductors from diffusion quantum Monte Carlo calculations
journal, February 2017


Interband Optical Transitions in Extremely Anisotropic Semiconductors. II. Coexistence of Exciton and the Landau Levels
journal, January 1967

  • Akimoto, Okikazu; Hasegawa, Hiroshi
  • Journal of the Physical Society of Japan, Vol. 22, Issue 1
  • DOI: 10.1143/JPSJ.22.181

Valley-splitting and valley-dependent inter-Landau-level optical transitions in monolayer MoS 2 quantum Hall systems
journal, July 2014


Exciton band structure of monolayer MoS 2
journal, February 2015


Optical Investigation of Monolayer and Bulk Tungsten Diselenide (WSe 2 ) in High Magnetic Fields
journal, June 2015


Optically bright p -excitons indicating strong Coulomb coupling in transition-metal dichalcogenides
journal, August 2015


Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

  • Ye, Ziliang; Cao, Ting; O’Brien, Kevin
  • Nature, Vol. 513, Issue 7517
  • DOI: 10.1038/nature13734

Neutral and charged inter-valley biexcitons in monolayer MoSe2
journal, June 2017

  • Hao, Kai; Specht, Judith F.; Nagler, Philipp
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15552

Two-dimensional excitons in magnetic fields
journal, April 1989

  • Edelstein, Warren; Spector, Harold N.; Marasas, Richard
  • Physical Review B, Vol. 39, Issue 11
  • DOI: 10.1103/PhysRevB.39.7697

Magneto-optics in transition metal diselenide monolayers
journal, June 2015


Exciton diamagnetic shift in semiconductor nanostructures
journal, April 1998


Coulomb engineering of the bandgap and excitons in two-dimensional materials
journal, May 2017

  • Raja, Archana; Chaves, Andrey; Yu, Jaeeun
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15251

Spin- and valley-dependent magneto-optical properties of MoS 2
journal, September 2013


Excitons in van der Waals heterostructures: The important role of dielectric screening
journal, December 2015


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

  • Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10643

Electrical control of neutral and charged excitons in a monolayer semiconductor
journal, February 2013

  • Ross, Jason S.; Wu, Sanfeng; Yu, Hongyi
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2498

Observation of biexcitons in monolayer WSe2
journal, May 2015

  • You, Yumeng; Zhang, Xiao-Xiao; Berkelbach, Timothy C.
  • Nature Physics, Vol. 11, Issue 6
  • DOI: 10.1038/nphys3324

Valley Zeeman effect in elementary optical excitations of monolayer WSe2
journal, January 2015

  • Srivastava, Ajit; Sidler, Meinrad; Allain, Adrien V.
  • Nature Physics, Vol. 11, Issue 2
  • DOI: 10.1038/nphys3203

Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

  • Cao, Ting; Wang, Gang; Han, Wenpeng
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1882

Excitons in 2H-WSe 2 and 3R-WS 2
journal, June 1976


Unusual Exciton–Phonon Interactions at van der Waals Engineered Interfaces
journal, January 2017


Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2
journal, August 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


Theory of neutral and charged excitons in monolayer transition metal dichalcogenides
journal, July 2013

  • Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichman, David R.
  • Physical Review B, Vol. 88, Issue 4
  • DOI: 10.1103/PhysRevB.88.045318

Berry Phase Modification to the Energy Spectrum of Excitons
journal, October 2015


Signatures of Bloch-Band Geometry on Excitons: Nonhydrogenic Spectra in Transition-Metal Dichalcogenides
journal, October 2015


Enabling valley selective exciton scattering in monolayer WSe2 through upconversion
journal, April 2017

  • Manca, M.; Glazov, M. M.; Robert, C.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14927

Probing the Influence of Dielectric Environment on Excitons in Monolayer WSe 2 : Insight from High Magnetic Fields
journal, October 2016


    Works referencing / citing this record:

    Intrinsic lifetime of higher excitonic states in tungsten diselenide monolayers
    journal, January 2019

    • Brem, Samuel; Zipfel, Jonas; Selig, Malte
    • Nanoscale, Vol. 11, Issue 25
    • DOI: 10.1039/c9nr04211c

    Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WS e 2
    journal, October 2019


    Intrinsic lifetime of higher excitonic states in tungsten diselenide monolayers
    journal, January 2019

    • Brem, Samuel; Zipfel, Jonas; Selig, Malte
    • Nanoscale, Vol. 11, Issue 25
    • DOI: 10.1039/c9nr04211c

    Common nonlinear features and spin-orbit coupling effects in the Zeeman splitting of novel wurtzite materials
    journal, May 2019


    Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WS e 2
    journal, October 2019


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


    Biexcitons in monolayer transition metal dichalcogenides tuned by magnetic fields
    journal, September 2018


    Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures
    journal, May 2019


    Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
    journal, September 2019


    Valley phonons and exciton complexes in a monolayer semiconductor
    journal, January 2020


    Dielectric disorder in two-dimensional materials
    journal, August 2019


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


    Visualizing electrostatic gating effects in two-dimensional heterostructures
    journal, July 2019


    Exciton diffusion in WSe 2 monolayers embedded in a van der Waals heterostructure
    journal, April 2018

    • Cadiz, F.; Robert, C.; Courtade, E.
    • Applied Physics Letters, Vol. 112, Issue 15
    • DOI: 10.1063/1.5026478

    Magneto-spectroscopy of exciton Rydberg states in a CVD grown WSe 2 monolayer
    journal, June 2019

    • Delhomme, A.; Butseraen, G.; Zheng, B.
    • Applied Physics Letters, Vol. 114, Issue 23
    • DOI: 10.1063/1.5095573

    Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum
    journal, March 2019

    • Scharf, Benedikt; Van Tuan, Dinh; Žutić, Igor
    • Journal of Physics: Condensed Matter, Vol. 31, Issue 20
    • DOI: 10.1088/1361-648x/ab071f

    Singlet and triplet trions in WS 2 monolayer encapsulated in hexagonal boron nitride
    journal, June 2018


    Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers
    journal, May 2018


    Dielectric impact on exciton binding energy and quasiparticle bandgap in monolayer WS 2 and WSe 2
    journal, March 2019


    Probing the exciton k-space dynamics in monolayer tungsten diselenides
    journal, March 2019


    High optical quality of MoS 2 monolayers grown by chemical vapor deposition
    journal, November 2019


    Theory of coherent pump–probe spectroscopy in monolayer transition metal dichalcogenides
    journal, December 2019


    Intervalley polaron in atomically thin transition metal dichalcogenides
    journal, July 2019


    Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response
    journal, July 2019


    k · p theory for phosphorene: Effective g -factors, Landau levels, and excitons
    journal, September 2019


    Multiphonon Raman scattering mediated by the exciton states in monolayer transition metal chalcogenides
    journal, September 2019


    Strain-tunable orbital, spin-orbit, and optical properties of monolayer transition-metal dichalcogenides
    journal, November 2019


    Comment on “Excitons, trions, and biexcitons in transition-metal dichalcogenides: Magnetic-field dependence”
    journal, March 2020


    Strain tuning of excitons in monolayer WSe 2
    journal, September 2018


    Coulomb interaction in monolayer transition-metal dichalcogenides
    journal, September 2018


    Dependence of band structure and exciton properties of encapsulated WSe 2 monolayers on the hBN-layer thickness
    journal, December 2018


    Monolayer transition metal dichalcogenides in strong magnetic fields: Validating the Wannier model using a microscopic calculation
    journal, January 2019


    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


    Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
    journal, August 2019


    Interaction-Induced Shubnikov–de Haas Oscillations in Optical Conductivity of Monolayer MoSe 2
    journal, August 2019


    Energy Spectrum of Two-Dimensional Excitons in a Nonuniform Dielectric Medium
    journal, September 2019


    Excited-State Trions in Monolayer WS 2
    journal, October 2019


    Controlling Excitons in an Atomically Thin Membrane with a Mirror
    journal, January 2020


    Exciton States in Monolayer MoSe 2 and MoTe 2 Probed by Upconversion Spectroscopy
    journal, September 2018