Many-Body Exciton and Intervalley Correlations in Heavily Electron-Doped WSe2 Monolayers
Abstract
We shoe that in monolayer transition-metal dichalcogenide semiconductors, many-body correlations can manifest in optical spectra when electron-hole pairs (excitons) are photoexcited into a 2D Fermi sea of mobile carriers. At low carrier densities, the formation of charged excitons (X±) is well documented. However, in WSe2 monolayers, an additional absorption resonance, often called X-', emerges at high electron density. Its origin is not understood. Here, we investigate the X-' state via polarized absorption spectroscopy of gated WSe2 monolayers in magnetic fields to 60T. Field-induced filling and emptying of the lowest optically active Landau level in the K' valley causes repeated quenching of the corresponding optical absorption. Surprisingly, these quenchings are accompanied by absorption changes to higher Landau levels in both K' and K valleys, which are unoccupied. These results cannot be reconciled within a single-particle picture, and demonstrate the many-body nature and intervalley correlations of the X-' quasiparticle state.
- Authors:
-
[1];
[2];
[3];
[3]
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Huazhong Univ. of Science and Technology, Hubei (China)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Warsaw (Poland)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of Washington, Seattle, WA (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Norwegian Financial Mechanism; Polish National Agency for Academic Exchange
- OSTI Identifier:
- 1845263
- Report Number(s):
- LA-UR-21-31300
Journal ID: ISSN 1530-6984
- Grant/Contract Number:
- 89233218CNA000001; DMR-1644779; SC0018171; 2020/37/K/ST3/03656; PPN/PPO/2020/1/00030
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 22; Journal Issue: 1; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 2D materials; monolayer semiconductors; excitons; Landau levels; intervalley correlations; high magnetic fields
Citation Formats
Li, Jing, Goryca, Mateusz Marek, Choi, Junho, Xu, Xiaodong, and Crooker, Scott A. Many-Body Exciton and Intervalley Correlations in Heavily Electron-Doped WSe2 Monolayers. United States: N. p., 2021.
Web. doi:10.1021/acs.nanolett.1c04217.
Li, Jing, Goryca, Mateusz Marek, Choi, Junho, Xu, Xiaodong, & Crooker, Scott A. Many-Body Exciton and Intervalley Correlations in Heavily Electron-Doped WSe2 Monolayers. United States. https://doi.org/10.1021/acs.nanolett.1c04217
Li, Jing, Goryca, Mateusz Marek, Choi, Junho, Xu, Xiaodong, and Crooker, Scott A. Fri .
"Many-Body Exciton and Intervalley Correlations in Heavily Electron-Doped WSe2 Monolayers". United States. https://doi.org/10.1021/acs.nanolett.1c04217. https://www.osti.gov/servlets/purl/1845263.
@article{osti_1845263,
title = {Many-Body Exciton and Intervalley Correlations in Heavily Electron-Doped WSe2 Monolayers},
author = {Li, Jing and Goryca, Mateusz Marek and Choi, Junho and Xu, Xiaodong and Crooker, Scott A.},
abstractNote = {We shoe that in monolayer transition-metal dichalcogenide semiconductors, many-body correlations can manifest in optical spectra when electron-hole pairs (excitons) are photoexcited into a 2D Fermi sea of mobile carriers. At low carrier densities, the formation of charged excitons (X±) is well documented. However, in WSe2 monolayers, an additional absorption resonance, often called X-', emerges at high electron density. Its origin is not understood. Here, we investigate the X-' state via polarized absorption spectroscopy of gated WSe2 monolayers in magnetic fields to 60T. Field-induced filling and emptying of the lowest optically active Landau level in the K' valley causes repeated quenching of the corresponding optical absorption. Surprisingly, these quenchings are accompanied by absorption changes to higher Landau levels in both K' and K valleys, which are unoccupied. These results cannot be reconciled within a single-particle picture, and demonstrate the many-body nature and intervalley correlations of the X-' quasiparticle state.},
doi = {10.1021/acs.nanolett.1c04217},
journal = {Nano Letters},
number = 1,
volume = 22,
place = {United States},
year = {Fri Dec 17 00:00:00 EST 2021},
month = {Fri Dec 17 00:00:00 EST 2021}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Coupled Spin and Valley Physics in Monolayers of and Other Group-VI Dichalcogenides
journal, May 2012
- Xiao, Di; Liu, Gui-Bin; Feng, Wanxiang
- Physical Review Letters, Vol. 108, Issue 19
Magnetic control of the valley degree of freedom of massive Dirac fermions with application to transition metal dichalcogenides
journal, September 2013
- Cai, Tianyi; Yang, Shengyuan A.; Li, Xiao
- Physical Review B, Vol. 88, Issue 11
Charged excitons in monolayer : Experiment and theory
journal, August 2017
- Courtade, E.; Semina, M.; Manca, M.
- Physical Review B, Vol. 96, Issue 8
Excitonic Linewidth Approaching the Homogeneous Limit in -Based van der Waals Heterostructures
journal, May 2017
- Cadiz, F.; Courtade, E.; Robert, C.
- Physical Review X, Vol. 7, Issue 2
Many-body theory of the optical conductivity of excitons and trions in two-dimensional materials
journal, August 2020
- Rana, Farhan; Koksal, Okan; Manolatou, Christina
- Physical Review B, Vol. 102, Issue 8
Fermi polaron-polaritons in charge-tunable atomically thin semiconductors
journal, October 2016
- Sidler, Meinrad; Back, Patrick; Cotlet, Ovidiu
- Nature Physics, Vol. 13, Issue 3
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
Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014
- Xu, Xiaodong; Yao, Wang; Xiao, Di
- Nature Physics, Vol. 10, Issue 5
Charge-tuneable biexciton complexes in monolayer WSe2
journal, September 2018
- Barbone, Matteo; Montblanch, Alejandro R. -P.; Kara, Dhiren M.
- Nature Communications, Vol. 9, Issue 1
Valley- and spin-polarized Landau levels in monolayer WSe2
journal, October 2016
- Wang, Zefang; Shan, Jie; Mak, Kin Fai
- Nature Nanotechnology, Vol. 12, Issue 2
Exchange intervalley scattering and magnetic phase diagram of transition metal dichalcogenide monolayers
journal, July 2019
- Miserev, Dmitry; Klinovaja, Jelena; Loss, Daniel
- Physical Review B, Vol. 100, Issue 1
k · p theory for two-dimensional transition metal dichalcogenide semiconductors
journal, April 2015
- Kormányos, Andor; Burkard, Guido; Gmitra, Martin
- 2D Materials, Vol. 2, Issue 2
Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
journal, September 2016
- Plechinger, Gerd; Nagler, Philipp; Arora, Ashish
- Nature Communications, Vol. 7, Issue 1
Rich many-body phase diagram of electrons and holes in doped monolayer transition metal dichalcogenides
journal, September 2018
- Van der Donck, M.; Peeters, F. M.
- Physical Review B, Vol. 98, Issue 11
Spontaneous Valley Polarization of Interacting Carriers in a Monolayer Semiconductor
journal, October 2020
- Li, J.; Goryca, M.; Wilson, N. P.
- Physical Review Letters, Vol. 125, Issue 14
Marrying Excitons and Plasmons in Monolayer Transition-Metal Dichalcogenides
journal, November 2017
- Van Tuan, Dinh; Scharf, Benedikt; Žutić, Igor
- Physical Review X, Vol. 7, Issue 4
Spin-polarized electrons in monolayer MoS2
journal, March 2019
- Roch, Jonas Gaël; Froehlicher, Guillaume; Leisgang, Nadine
- Nature Nanotechnology, Vol. 14, Issue 5
Fast photothermal spatial light modulation for quantitative phase imaging at the nanoscale
journal, May 2021
- Robert, Hadrien M. L.; Holanová, Kristýna; Bujak, Łukasz
- Nature Communications, Vol. 12, Issue 1
Absorption spectrum of a weakly n -doped semiconductor quantum well
journal, May 2000
- Bronold, F. X.
- Physical Review B, Vol. 61, Issue 19
Rydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe2
journal, August 2021
- Kapuściński, Piotr; Delhomme, Alex; Vaclavkova, Diana
- Communications Physics, Vol. 4, Issue 1
Many-body theory of trion absorption features in two-dimensional semiconductors
journal, January 2017
- Efimkin, Dmitry K.; MacDonald, Allan H.
- Physical Review B, Vol. 95, Issue 3
Measurement of Conduction and Valence Bands -Factors in a Transition Metal Dichalcogenide Monolayer
journal, February 2021
- Robert, C.; Dery, H.; Ren, L.
- Physical Review Letters, Vol. 126, Issue 6
Spin- and valley-dependent magneto-optical properties of MoS
journal, September 2013
- Rose, Félix; Goerbig, M. O.; Piéchon, Frédéric
- Physical Review B, Vol. 88, Issue 12
Electron-exciton interactions in the exciton-polaron problem
journal, February 2021
- Efimkin, Dmitry K.; Laird, Emma K.; Levinsen, Jesper
- Physical Review B, Vol. 103, Issue 7
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
Correlation Energy and Spin Polarization in the 2D Electron Gas
journal, June 2002
- Attaccalite, Claudio; Moroni, Saverio; Gori-Giorgi, Paola
- Physical Review Letters, Vol. 88, Issue 25
Controlling exciton many-body states by the electric-field effect in monolayer
journal, April 2021
- Klein, J.; Hötger, A.; Florian, M.
- Physical Review Research, Vol. 3, Issue 2
Interaction-Induced Shubnikov–de Haas Oscillations in Optical Conductivity of Monolayer
journal, August 2019
- Smoleński, T.; Cotlet, O.; Popert, A.
- Physical Review Letters, Vol. 123, Issue 9
Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor
journal, February 2018
- Stier, A. V.; Wilson, N. P.; Velizhanin, K. A.
- Physical Review Letters, Vol. 120, Issue 5
Signatures of Wigner crystal of electrons in a monolayer semiconductor
journal, June 2021
- Smoleński, Tomasz; Dolgirev, Pavel E.; Kuhlenkamp, Clemens
- Nature, Vol. 595, Issue 7865
Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018
- Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
- Reviews of Modern Physics, Vol. 90, Issue 2
Optical properties of charged excitons in two-dimensional semiconductors
journal, July 2020
- Glazov, M. M.
- The Journal of Chemical Physics, Vol. 153, Issue 3
Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers
journal, July 2017
- Ajayi, Obafunso A.; Ardelean, Jenny V.; Shepard, Gabriella D.
- 2D Materials, Vol. 4, Issue 3
Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices
journal, March 2020
- Regan, Emma C.; Wang, Danqing; Jin, Chenhao
- Nature, Vol. 579, Issue 7799
Optical generation of excitonic valley coherence in monolayer WSe2
journal, August 2013
- Jones, Aaron M.; Yu, Hongyi; Ghimire, Nirmal J.
- Nature Nanotechnology, Vol. 8, Issue 9
Valley Zeeman Splitting and Valley Polarization of Neutral and Charged Excitons in Monolayer MoTe 2 at High Magnetic Fields
journal, May 2016
- Arora, Ashish; Schmidt, Robert; Schneider, Robert
- Nano Letters, Vol. 16, Issue 6
Exciton-Trion Polaritons in Doped Two-Dimensional Semiconductors
journal, March 2021
- Rana, Farhan; Koksal, Okan; Jung, Minwoo
- Physical Review Letters, Vol. 126, Issue 12
Correlated insulating states at fractional fillings of moiré superlattices
journal, November 2020
- Xu, Yang; Liu, Song; Rhodes, Daniel A.
- Nature, Vol. 587, Issue 7833
Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016
- Mak, Kin Fai; Shan, Jie
- Nature Photonics, Vol. 10, Issue 4
Valley-splitting and valley-dependent inter-Landau-level optical transitions in monolayer quantum Hall systems
journal, July 2014
- Chu, Rui-Lin; Li, Xiao; Wu, Sanfeng
- Physical Review B, Vol. 90, Issue 4
Optical Investigation of Monolayer and Bulk Tungsten Diselenide (WSe 2 ) in High Magnetic Fields
journal, June 2015
- Mitioglu, A. A.; Plochocka, P.; Granados del Aguila, Á.
- Nano Letters, Vol. 15, Issue 7
Excitons and Trions Modified by Interaction with a Two-Dimensional Electron Gas
journal, October 2001
- Suris, R. A.; Kochereshko, V. P.; Astakhov, G. V.
- physica status solidi (b), Vol. 227, Issue 2
Observation of Quantized Exciton Energies in Monolayer under a Strong Magnetic Field
journal, April 2020
- Wang, Tianmeng; Li, Zhipeng; Lu, Zhengguang
- Physical Review X, Vol. 10, Issue 2
Landau-Quantized Excitonic Absorption and Luminescence in a Monolayer Valley Semiconductor
journal, March 2020
- Liu, Erfu; van Baren, Jeremiah; Taniguchi, Takashi
- Physical Review Letters, Vol. 124, Issue 9
Crossover from trion-hole complex to exciton-polaron in -doped two-dimensional semiconductor quantum wells
journal, December 2018
- Chang, Yia-Chung; Shiau, Shiue-Yuan; Combescot, Monique
- Physical Review B, Vol. 98, Issue 23
Giant Paramagnetism-Induced Valley Polarization of Electrons in Charge-Tunable Monolayer
journal, June 2017
- Back, Patrick; Sidler, Meinrad; Cotlet, Ovidiu
- Physical Review Letters, Vol. 118, Issue 23
Valley relaxation of resident electrons and holes in a monolayer semiconductor: Dependence on carrier density and the role of substrate-induced disorder
journal, April 2021
- Li, Jing; Goryca, M.; Yumigeta, K.
- Physical Review Materials, Vol. 5, Issue 4
Valleytronics in 2D materials
journal, August 2016
- Schaibley, John R.; Yu, Hongyi; Clark, Genevieve
- Nature Reviews Materials, Vol. 1, Issue 11
Probing the Spin-Polarized Electronic Band Structure in Monolayer Transition Metal Dichalcogenides by Optical Spectroscopy
journal, January 2017
- Wang, Zefang; Zhao, Liang; Mak, Kin Fai
- Nano Letters, Vol. 17, Issue 2
Singlet and triplet trions in WS 2 monolayer encapsulated in hexagonal boron nitride
journal, June 2018
- Vaclavkova, D.; Wyzula, J.; Nogajewski, K.
- Nanotechnology, Vol. 29, Issue 32