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Title: Magnetic control of valley pseudospin in monolayer WSe2

Abstract

Local energy extrema of the bands in momentum space, or valleys, can endow electrons in solids with pseudo-spin in addition to real spin1-5. In transition metal dichalcogenides this valley pseudo-spin, like real spin, is associated with a magnetic moment1,6 which underlies the valley-dependent circular dichroism6 that allows optical generation of valley polarization7-9, intervalley quantum coherence10, and the valley Hall effect11. However, magnetic manipulation of valley pseudospin via this magnetic moment12-13, analogous to what is possible with real spin, has not been shown before. Here we report observation of the valley Zeeman splitting and magnetic tuning of polarization and coherence of the excitonic valley pseudospin, by performing polarization-resolved magneto-photoluminescence on monolayer WSe2. Our measurements reveal both the atomic orbital and lattice contributions to the valley orbital magnetic moment; demonstrate the deviation of the band edges in the valleys from an exact massive Dirac fermion model; and reveal a striking difference between the magnetic responses of neutral and charged valley excitons which is explained by renormalization of the excitonic spectrum due to strong exchange interactions.

Authors:
 [1];  [2];  [1];  [3];  [4];  [4];  [3];  [1];  [2];  [1]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Univ. of Hong Kong, Hong Kong (China)
  3. Univ. of Texas-Dallas, Richardson, TX (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1265429
Grant/Contract Number:  
AC05-00OR22725; SC0008145; SC0002197; HKU705513P; HKU9/CRF/13G; AoE/P-04/08
Resource Type:
Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Volume: 11; Journal Issue: 2; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Aivazian, G., Gong, Zhirui, Jones, Aaron M., Chu, Rui-Lin, Yan, J., Mandrus, D. G., Zhang, Chuanwei, Cobden, David, Yao, Wang, and Xu, X. Magnetic control of valley pseudospin in monolayer WSe2. United States: N. p., 2015. Web. doi:10.1038/nphys3201.
Aivazian, G., Gong, Zhirui, Jones, Aaron M., Chu, Rui-Lin, Yan, J., Mandrus, D. G., Zhang, Chuanwei, Cobden, David, Yao, Wang, & Xu, X. Magnetic control of valley pseudospin in monolayer WSe2. United States. https://doi.org/10.1038/nphys3201
Aivazian, G., Gong, Zhirui, Jones, Aaron M., Chu, Rui-Lin, Yan, J., Mandrus, D. G., Zhang, Chuanwei, Cobden, David, Yao, Wang, and Xu, X. Mon . "Magnetic control of valley pseudospin in monolayer WSe2". United States. https://doi.org/10.1038/nphys3201. https://www.osti.gov/servlets/purl/1265429.
@article{osti_1265429,
title = {Magnetic control of valley pseudospin in monolayer WSe2},
author = {Aivazian, G. and Gong, Zhirui and Jones, Aaron M. and Chu, Rui-Lin and Yan, J. and Mandrus, D. G. and Zhang, Chuanwei and Cobden, David and Yao, Wang and Xu, X.},
abstractNote = {Local energy extrema of the bands in momentum space, or valleys, can endow electrons in solids with pseudo-spin in addition to real spin1-5. In transition metal dichalcogenides this valley pseudo-spin, like real spin, is associated with a magnetic moment1,6 which underlies the valley-dependent circular dichroism6 that allows optical generation of valley polarization7-9, intervalley quantum coherence10, and the valley Hall effect11. However, magnetic manipulation of valley pseudospin via this magnetic moment12-13, analogous to what is possible with real spin, has not been shown before. Here we report observation of the valley Zeeman splitting and magnetic tuning of polarization and coherence of the excitonic valley pseudospin, by performing polarization-resolved magneto-photoluminescence on monolayer WSe2. Our measurements reveal both the atomic orbital and lattice contributions to the valley orbital magnetic moment; demonstrate the deviation of the band edges in the valleys from an exact massive Dirac fermion model; and reveal a striking difference between the magnetic responses of neutral and charged valley excitons which is explained by renormalization of the excitonic spectrum due to strong exchange interactions.},
doi = {10.1038/nphys3201},
journal = {Nature Physics},
number = 2,
volume = 11,
place = {United States},
year = {Mon Jan 26 00:00:00 EST 2015},
month = {Mon Jan 26 00:00:00 EST 2015}
}

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Identifying defect-related quantum emitters in monolayer WSe2
journal, February 2020


Discrete quantum dot like emitters in monolayer MoSe 2 : Spatial mapping, magneto-optics, and charge tuning
journal, April 2016

  • Branny, Artur; Wang, Gang; Kumar, Santosh
  • Applied Physics Letters, Vol. 108, Issue 14
  • DOI: 10.1063/1.4945268

Strain engineering of valley polarized currents in topological crystalline insulators
journal, May 2019

  • Kanjouri, F.; Piri Pishekloo, S.; Khani, H.
  • Journal of Physics: Condensed Matter, Vol. 31, Issue 30
  • DOI: 10.1088/1361-648x/ab1113

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


Universal low-temperature Ohmic contacts for quantum transport in transition metal dichalcogenides
journal, April 2016


Twisting dirac fermions: circular dichroism in bilayer graphene
journal, July 2017


Vibration detection schemes based on absorbance tuning in monolayer molybdenum disulfide mechanical resonators
journal, October 2018


Zeeman spectroscopy of excitons and hybridization of electronic states in few-layer WSe 2 , MoSe 2 and MoTe 2
journal, November 2018


Valley-contrasting physics in all-dielectric photonic crystals: Orbital angular momentum and topological propagation
journal, July 2017


Imaging of pure spin-valley diffusion current in WS 2 -WSe 2 heterostructures
journal, May 2018


Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer WS2
text, January 2018

  • Nagler, Philipp; Ballottin, Mariana V.; Mitioglu, Anatolie A.
  • Universität Regensburg
  • DOI: 10.5283/epub.39849

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

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


Valley coherent exciton-polaritons in a monolayer semiconductor
journal, November 2018


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


Entanglement of single-photons and chiral phonons in atomically thin WSe2
journal, December 2018


Spin-orbital effects in metal-dichalcogenide semiconducting monolayers
journal, April 2016

  • Reyes-Retana, J. A.; Cervantes-Sodi, F.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep24093

Spin polarization and tunable valley degeneracy in a MoS 2 monolayer via proximity coupling to a Cr 2 O 3 substrate
journal, January 2019


Diffusion dynamics of valley excitons by transient grating spectroscopy in monolayer WSe 2
journal, September 2019

  • Wang, Jing; Guo, Yang; Huang, Yuan
  • Applied Physics Letters, Vol. 115, Issue 13
  • DOI: 10.1063/1.5116263

Intrinsic valley polarization of magnetic VSe 2 monolayers
journal, May 2017

  • Liu, Jian; Hou, Wen-Jie; Cheng, Cai
  • Journal of Physics: Condensed Matter, Vol. 29, Issue 25
  • DOI: 10.1088/1361-648x/aa6e6e

Influence of the substrate material on the optical properties of tungsten diselenide monolayers
journal, March 2017

  • Lippert, Sina; Schneider, Lorenz Maximilian; Renaud, Dylan
  • 2D Materials, Vol. 4, Issue 2
  • DOI: 10.1088/2053-1583/aa5b21

Electronic structure-dependent magneto-optical Raman effect in atomically thin WS 2
journal, June 2018


Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe 2 , WSe 2 and WS 2 Monolayers
journal, October 2018


Controlling valley splitting and polarization of dark- and bi-excitons in monolayer WS 2 by a tilted magnetic field
journal, July 2019


Magneto-optical Kerr effect in spin split two-dimensional massive Dirac materials
journal, January 2020


Valley excitons in two-dimensional semiconductors
journal, December 2014

  • Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong
  • National Science Review, Vol. 2, Issue 1
  • DOI: 10.1093/nsr/nwu078

Spin-degenerate regimes for single quantum dots in transition metal dichalcogenide monolayers
journal, June 2017


Spatial variations of valley splitting in monolayer transition metal dichalcogenide
journal, November 2019


Light Sources and Photodetectors Enabled by 2D Semiconductors
journal, May 2018


Valleytronics in transition metal dichalcogenides materials
journal, August 2019


Valley magnetoelectricity in single-layer MoS2
journal, July 2017

  • Lee, Jieun; Wang, Zefang; Xie, Hongchao
  • Nature Materials, Vol. 16, Issue 9
  • DOI: 10.1038/nmat4931

Excitonic luminescence upconversion in a two-dimensional semiconductor
journal, December 2015

  • Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.
  • Nature Physics, Vol. 12, Issue 4
  • DOI: 10.1038/nphys3604

An ab initio study of sensing applications of MoB 2 monolayer: a potential gas sensor
journal, January 2019

  • Bano, Amreen; Krishna, Jyoti; Pandey, Devendra K.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 8
  • DOI: 10.1039/c8cp07038e

Spin- and valley-polarized transport in a monolayer of MoS 2
journal, August 2016


Valley-selective directional emission from a transition-metal dichalcogenide monolayer mediated by a plasmonic nanoantenna
journal, January 2018

  • Chen, Haitao; Liu, Mingkai; Xu, Lei
  • Beilstein Journal of Nanotechnology, Vol. 9
  • DOI: 10.3762/bjnano.9.71

Environmental engineering of transition metal dichalcogenide optoelectronics
journal, June 2018

  • LaMountain, Trevor; Lenferink, Erik J.; Chen, Yen-Jung
  • Frontiers of Physics, Vol. 13, Issue 4
  • DOI: 10.1007/s11467-018-0795-x

Low-dimensional ScO 2 with tunable electronic and magnetic properties: first-principles studies
journal, November 2015


Robust effective Zeeman energy in monolayer MoS 2 quantum dots
journal, July 2016


Exciton polaritons in transition-metal dichalcogenides and their direct excitation via energy transfer
journal, August 2015


Magneto-optics in transition metal diselenide monolayers
text, January 2015


Concepts of Ferrovalley Material and Anomalous Valley Hall Effect
text, January 2016


Directional Interlayer Spin-Valley Transfer in Two-Dimensional Heterostructures
text, January 2016


Twisting Dirac fermions: Circular dichroism in bilayer graphene
text, January 2017


Enhanced interlayer neutral excitons and trions in trilayer van der Waals heterostructures
text, January 2017


Ambipolar Landau levels and strong band-selective carrier interactions in monolayer WSe$_2$
text, January 2017


Symmetry-forbidden intervalley scattering by atomic defects in monolayer transition-metal dichalcogenides
text, January 2017


Spin-orbit coupling induced valley Hall effects in transition-metal dichalcogenides
text, January 2017


Valley coherent exciton-polaritons in a monolayer semiconductor
text, January 2018


Entanglement of single-photons and chiral phonons in atomically thin WSe$_2$
text, January 2018


Magneto-spectroscopy of exciton Rydberg states in a CVD grown WSe2 monolayer
text, January 2019


Identifying defect-related quantum emitters in monolayer WSe$_2$
text, January 2020


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

  • Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
  • Universität Regensburg
  • DOI: 10.5283/epub.40518

High Quality Factor Mechanical Resonators Based on WSe 2 Monolayers
journal, August 2016


Valley Polarization by Spin Injection in a Light-Emitting van der Waals Heterojunction
journal, August 2016


Microsecond dark-exciton valley polarization memory in two-dimensional heterostructures
journal, February 2018


Evidence for line width and carrier screening effects on excitonic valley relaxation in 2D semiconductors
journal, July 2018


Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2
journal, June 2019


Enhancing and controlling valley magnetic response in MoS2/WS2 heterostructures by all-optical route
journal, September 2019


Gate controlled valley polarizer in bilayer graphene
journal, March 2020


Giant Valley Coherence at Room Temperature in 3R WS 2 with Broken Inversion Symmetry
journal, October 2019


Valley-selective directional emission from a transition-metal dichalcogenide monolayer mediated by a plasmonic nanoantenna
journal, January 2018

  • Chen, Haitao; Liu, Mingkai; Xu, Lei
  • Beilstein Journal of Nanotechnology, Vol. 9
  • DOI: 10.3762/bjnano.9.71

Valley coherent exciton-polaritons in a monolayer semiconductor
text, January 2018


Giant Valley Splitting in Monolayer WS2 by Magnetic Proximity Effect
text, January 2019


Valley Phonons and Exciton Complexes in a Monolayer Semiconductor
text, January 2020


Giant magnetic splitting inducing near-unity valley polarization in van der Waals heterostructures
text, January 2017

  • Nagler, Philipp; Ballottin, Mariana V.; Mitioglu, Anatolie A.
  • Universität Regensburg
  • DOI: 10.5283/epub.36370