Intercell moiré exciton complexes in electron lattices
Abstract
Excitons, Coulomb bound electron-hole pairs, play a fundamental role in both optical excitation and correlated phenomena in solids1. When an exciton interacts with other quasi-particles, few- and many-body excited states, such as trions2-4, exciton Fermi-polarons5, Mahan excitons6, and other exotic excitonic phases7-9 will appear. Here, we report a new interaction between exciton and charges enabled by unusual quantum confinement in 2D moiré superlattices, which results in novel exciton many-body ground states composed of moiré excitons and correlated electron lattices. Unique to H-stacked (or 60o-twisted) WS2/WSe2 heterobilayer, we found that the interlayer atomic registry and moiré structural reconstruction lead to distinct spatial distribution for the frontier conduction and valence bands in WS2 and WSe2, respectively. This gives rise to interlayer moiré excitons (IMEs) with a novel 3D structure, i.e., the hole in one layer is surrounded by its partner electron’s wavefunction spread among three adjacent moiré traps in another layer. Thus, this new type of IME can possess large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the electric quadrupole enables the binding of IME to the charges in neighboring moiré cells, forming an intercell charged exciton complex distinct from trions2-4. The exciton complex is unveiled bymore »
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- Univ. of Washington, Seattle, WA (United States)
- National Institute for Materials Science (NIMS), Tsukuba (Japan)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Univ. of Hong Kong (Hong Kong); HKU-UCAS Joint Institute of Theoretical and Computational Physics (Hong Kong)
- Univ. of Washington, Seattle, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Army Research Office (ARO)
- OSTI Identifier:
- 1986201
- Alternate Identifier(s):
- OSTI ID: 2283190
- Report Number(s):
- PNNL-SA-170857
Journal ID: ISSN 1476-1122
- Grant/Contract Number:
- AC05-00OR22725; SC0018171; SC0019443; SC0012509; DMR-1719797; DGE-1762114; W911NF-18-1-0431; AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 22; Journal Issue: 5; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; electronic properties and materials; two-dimensional materials
Citation Formats
Wang, Xi, Zhang, Xiaowei, Zhu, Jiayi, Park, Heonjoon, Wang, Yingqi, Wang, Chong, Holtzmann, William G., Taniguchi, Takashi, Watanabe, Kenji, Yan, Jiaqiang, Gamelin, Daniel R., Yao, Wang, Xiao, Di, Cao, Ting, and Xu, Xiaodong. Intercell moiré exciton complexes in electron lattices. United States: N. p., 2023.
Web. doi:10.1038/s41563-023-01496-2.
Wang, Xi, Zhang, Xiaowei, Zhu, Jiayi, Park, Heonjoon, Wang, Yingqi, Wang, Chong, Holtzmann, William G., Taniguchi, Takashi, Watanabe, Kenji, Yan, Jiaqiang, Gamelin, Daniel R., Yao, Wang, Xiao, Di, Cao, Ting, & Xu, Xiaodong. Intercell moiré exciton complexes in electron lattices. United States. https://doi.org/10.1038/s41563-023-01496-2
Wang, Xi, Zhang, Xiaowei, Zhu, Jiayi, Park, Heonjoon, Wang, Yingqi, Wang, Chong, Holtzmann, William G., Taniguchi, Takashi, Watanabe, Kenji, Yan, Jiaqiang, Gamelin, Daniel R., Yao, Wang, Xiao, Di, Cao, Ting, and Xu, Xiaodong. Thu .
"Intercell moiré exciton complexes in electron lattices". United States. https://doi.org/10.1038/s41563-023-01496-2. https://www.osti.gov/servlets/purl/1986201.
@article{osti_1986201,
title = {Intercell moiré exciton complexes in electron lattices},
author = {Wang, Xi and Zhang, Xiaowei and Zhu, Jiayi and Park, Heonjoon and Wang, Yingqi and Wang, Chong and Holtzmann, William G. and Taniguchi, Takashi and Watanabe, Kenji and Yan, Jiaqiang and Gamelin, Daniel R. and Yao, Wang and Xiao, Di and Cao, Ting and Xu, Xiaodong},
abstractNote = {Excitons, Coulomb bound electron-hole pairs, play a fundamental role in both optical excitation and correlated phenomena in solids1. When an exciton interacts with other quasi-particles, few- and many-body excited states, such as trions2-4, exciton Fermi-polarons5, Mahan excitons6, and other exotic excitonic phases7-9 will appear. Here, we report a new interaction between exciton and charges enabled by unusual quantum confinement in 2D moiré superlattices, which results in novel exciton many-body ground states composed of moiré excitons and correlated electron lattices. Unique to H-stacked (or 60o-twisted) WS2/WSe2 heterobilayer, we found that the interlayer atomic registry and moiré structural reconstruction lead to distinct spatial distribution for the frontier conduction and valence bands in WS2 and WSe2, respectively. This gives rise to interlayer moiré excitons (IMEs) with a novel 3D structure, i.e., the hole in one layer is surrounded by its partner electron’s wavefunction spread among three adjacent moiré traps in another layer. Thus, this new type of IME can possess large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the electric quadrupole enables the binding of IME to the charges in neighboring moiré cells, forming an intercell charged exciton complex distinct from trions2-4. The exciton complex is unveiled by the IME photoluminescence energy jumps when the electron lattices form at both fractional and integer fillings of moiré minibands, with replica like spectral features between successive integer moiré fillings. Our work provides the framework in understanding and engineering novel exciton many-body states in moiré superlattices with correlated charge orders.},
doi = {10.1038/s41563-023-01496-2},
journal = {Nature Materials},
number = 5,
volume = 22,
place = {United States},
year = {Thu Mar 09 00:00:00 EST 2023},
month = {Thu Mar 09 00:00:00 EST 2023}
}
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Works referenced in this record:
Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices
journal, November 2017
- Yu, Hongyi; Liu, Gui-Bin; Tang, Jianju
- Science Advances, Vol. 3, Issue 11
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers
journal, May 2018
- Yu, Hongyi; Liu, Gui-Bin; Yao, Wang
- 2D Materials, Vol. 5, 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
Hubbard Model Physics in Transition Metal Dichalcogenide Moiré Bands
journal, July 2018
- Wu, Fengcheng; Lovorn, Timothy; Tutuc, Emanuel
- Physical Review Letters, Vol. 121, Issue 2
Electronic structures, charge transfer, and charge order in twisted transition metal dichalcogenide bilayers
journal, April 2021
- Zhang, Yang; Liu, Tongtong; Fu, Liang
- Physical Review B, Vol. 103, Issue 15
Moiré Intralayer Excitons in a MoSe 2 /MoS 2 Heterostructure
journal, November 2018
- Zhang, Nan; Surrente, Alessandro; Baranowski, Michał
- Nano Letters, Vol. 18, Issue 12
Fermi polaron-polaritons in charge-tunable atomically thin semiconductors
journal, October 2016
- Sidler, Meinrad; Back, Patrick; Cotlet, Ovidiu
- Nature Physics, Vol. 13, Issue 3
Directional interlayer spin-valley transfer in two-dimensional heterostructures
journal, December 2016
- Schaibley, John R.; Rivera, Pasqual; Yu, Hongyi
- Nature Communications, Vol. 7, Issue 1
Imaging moiré flat bands in three-dimensional reconstructed WSe2/WS2 superlattices
journal, February 2021
- Li, Hongyuan; Li, Shaowei; Naik, Mit H.
- Nature Materials, Vol. 20, Issue 7
Magic in twisted transition metal dichalcogenide bilayers
journal, November 2021
- Devakul, Trithep; Crépel, Valentin; Zhang, Yang
- Nature Communications, Vol. 12, Issue 1
Correlated insulating states at fractional fillings of the WS2/WSe2 moiré lattice
journal, February 2021
- Huang, Xiong; Wang, Tianmeng; Miao, Shengnan
- Nature Physics
Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers
journal, February 2019
- Seyler, Kyle L.; Rivera, Pasqual; Yu, Hongyi
- Nature, Vol. 567, Issue 7746
Highly energy-tunable quantum light from moiré-trapped excitons
journal, September 2020
- Baek, H.; Brotons-Gisbert, M.; Koong, Z. X.
- Science Advances, Vol. 6, Issue 37
The SIESTA method for ab initio order- N materials simulation
journal, March 2002
- Soler, José M.; Artacho, Emilio; Gale, Julian D.
- Journal of Physics: Condensed Matter, Vol. 14, Issue 11
Correlated insulating states at fractional fillings of moiré superlattices
journal, November 2020
- Xu, Yang; Liu, Song; Rhodes, Daniel A.
- Nature, Vol. 587, Issue 7833
Simulation of Hubbard model physics in WSe2/WS2 moiré superlattices
journal, March 2020
- Tang, Yanhao; Li, Lizhong; Li, Tingxin
- Nature, Vol. 579, Issue 7799
Quantum anomalous Hall effect from intertwined moiré bands
journal, December 2021
- Li, Tingxin; Jiang, Shengwei; Shen, Bowen
- Nature, Vol. 600, Issue 7890
Moiré heterostructures as a condensed-matter quantum simulator
journal, February 2021
- Kennes, Dante M.; Claassen, Martin; Xian, Lede
- Nature Physics, Vol. 17, Issue 2
Observation of moiré excitons in WSe2/WS2 heterostructure superlattices
journal, February 2019
- Jin, Chenhao; Regan, Emma C.; Yan, Aiming
- Nature, Vol. 567, Issue 7746
Evidence for moiré excitons in van der Waals heterostructures
journal, February 2019
- Tran, Kha; Moody, Galan; Wu, Fengcheng
- Nature, Vol. 567, Issue 7746
Bilayer Wigner crystals in a transition metal dichalcogenide heterostructure
journal, June 2021
- Zhou, You; Sung, Jiho; Brutschea, Elise
- Nature, Vol. 595, Issue 7865
Quantum phase diagram of a Moiré-Hubbard model
journal, November 2020
- Pan, Haining; Wu, Fengcheng; Das Sarma, Sankar
- Physical Review B, Vol. 102, Issue 20
Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moiré superlattice
journal, June 2021
- Miao, Shengnan; Wang, Tianmeng; Huang, Xiong
- Nature Communications, Vol. 12, Issue 1
Excitonic and Valley-Polarization Signatures of Fractional Correlated Electronic Phases in a Moiré Superlattice
journal, July 2021
- Liu, Erfu; Taniguchi, Takashi; Watanabe, Kenji
- Physical Review Letters, Vol. 127, Issue 3
Spin liquid phase of the Heisenberg model on the triangular lattice
journal, July 2015
- Zhu, Zhenyue; White, Steven R.
- Physical Review B, Vol. 92, Issue 4
Optimized norm-conserving Vanderbilt pseudopotentials
journal, August 2013
- Hamann, D. R.
- Physical Review B, Vol. 88, Issue 8
Dipolar excitonic insulator in a moiré lattice
journal, March 2022
- Gu, Jie; Ma, Liguo; Liu, Song
- Nature Physics, Vol. 18, Issue 4
Hartree-Fock study of the moiré Hubbard model for twisted bilayer transition metal dichalcogenides
journal, August 2021
- Zang, Jiawei; Wang, Jie; Cano, Jennifer
- Physical Review B, Vol. 104, Issue 7
Signatures of moiré trions in WSe2/MoSe2 heterobilayers
journal, June 2021
- Liu, Erfu; Barré, Elyse; van Baren, Jeremiah
- Nature, Vol. 594, Issue 7861
Quantum criticality in twisted transition metal dichalcogenides
journal, September 2021
- Ghiotto, Augusto; Shih, En-Min; Pereira, Giancarlo S. S. G.
- Nature, Vol. 597, Issue 7876
Many-body correlations and excitonic effects in semiconductor spectroscopy
journal, January 2006
- Kira, M.; Koch, S. W.
- Progress in Quantum Electronics, Vol. 30, Issue 5
Anomalous Light Cones and Valley Optical Selection Rules of Interlayer Excitons in Twisted Heterobilayers
journal, October 2015
- Yu, Hongyi; Wang, Yong; Tong, Qingjun
- Physical Review Letters, Vol. 115, Issue 18
Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006
- Grimme, Stefan
- Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
Moiré trions in MoSe2/WSe2 heterobilayers
journal, September 2021
- Wang, Xi; Zhu, Jiayi; Seyler, Kyle L.
- Nature Nanotechnology, Vol. 16, Issue 11
Competing magnetic states in transition metal dichalcogenide moiré materials
journal, December 2021
- Hu, Nai Chao; MacDonald, Allan H.
- Physical Review B, Vol. 104, Issue 21
Stripe phases in WSe2/WS2 moiré superlattices
journal, March 2021
- Jin, Chenhao; Tao, Zui; Li, Tingxin
- Nature Materials
Imaging two-dimensional generalized Wigner crystals
journal, September 2021
- Li, Hongyuan; Li, Shaowei; Regan, Emma C.
- Nature, Vol. 597, Issue 7878
Strongly correlated electrons and hybrid excitons in a moiré heterostructure
journal, April 2020
- Shimazaki, Yuya; Schwartz, Ido; Watanabe, Kenji
- Nature, Vol. 580, Issue 7804
Moiré-Trapped Interlayer Trions in a Charge-Tunable Heterobilayer
journal, August 2021
- Brotons-Gisbert, Mauro; Baek, Hyeonjun; Campbell, Aidan
- Physical Review X, Vol. 11, Issue 3
Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures
journal, March 2019
- Alexeev, Evgeny M.; Ruiz-Tijerina, David A.; Danovich, Mark
- Nature, Vol. 567, Issue 7746
Interlayer valley excitons in heterobilayers of transition metal dichalcogenides
journal, August 2018
- Rivera, Pasqual; Yu, Hongyi; Seyler, Kyle L.
- Nature Nanotechnology, Vol. 13, Issue 11
Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures
journal, February 2015
- Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M.
- Nature Communications, Vol. 6, Issue 1