Intercell moiré exciton complexes in electron lattices

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

doi:10.1038/s41563-023-01496-2

Intercell moiré exciton complexes in electron lattices

Journal Article · Thu Mar 09 00:00:00 EST 2023 · Nature Materials

DOI:https://doi.org/10.1038/s41563-023-01496-2· OSTI ID:1986201

^[1]; Zhang, Xiaowei ^[1]; Zhu, Jiayi ^[1]; ^[1]; ^[1]; ^[1]; Holtzmann, William G. ^[1]; ^[2]; ^[2]; ^[3]; ^[1]; ^[4]; ^[5]; ^[1]; ^[1]

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)

Excitons, Coulomb-bound electron–hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here, in this work, we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moiré superlattices, which results in many-body ground states composed of moiré excitons and correlated electron lattices. In an H-stacked (60^o-twisted) WS₂/WSe₂ heterobilayer, we found an interlayer moiré exciton whose hole is surrounded by its partner electron’s wavefunction distributed among three adjacent moiré traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moiré excitons to the charges in neighbouring moiré cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moiré charge orders.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Army Research Office (ARO); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC05-76RL01830; SC0012509; SC0018171; SC0019443

OSTI ID:: 1986201

Alternate ID(s):: OSTI ID: 2283190

Report Number(s):: PNNL-SA--170857

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 5 Vol. 22; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Many-body correlations and excitonic effects in semiconductor spectroscopy Kira, M.; Koch, S. W. Progress in Quantum Electronics, Vol. 30, Issue 5 https://doi.org/10.1016/j.pquantelec.2006.12.002	journal	January 2006
Moiré Intralayer Excitons in a MoSe ₂ /MoS ₂ Heterostructure Zhang, Nan; Surrente, Alessandro; Baranowski, Michał Nano Letters, Vol. 18, Issue 12 https://doi.org/10.1021/acs.nanolett.8b03266	journal	November 2018
Directional interlayer spin-valley transfer in two-dimensional heterostructures Schaibley, John R.; Rivera, Pasqual; Yu, Hongyi Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13747	journal	December 2016
Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7242	journal	February 2015
Fermi polaron-polaritons in charge-tunable atomically thin semiconductors Sidler, Meinrad; Back, Patrick; Cotlet, Ovidiu Nature Physics, Vol. 13, Issue 3 https://doi.org/10.1038/nphys3949	journal	October 2016
Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moiré superlattice Miao, Shengnan; Wang, Tianmeng; Huang, Xiong Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23732-6	journal	June 2021
Magic in twisted transition metal dichalcogenide bilayers Devakul, Trithep; Crépel, Valentin; Zhang, Yang Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-27042-9	journal	November 2021
Imaging moiré flat bands in three-dimensional reconstructed WSe2/WS2 superlattices Li, Hongyuan; Li, Shaowei; Naik, Mit H. Nature Materials, Vol. 20, Issue 7 https://doi.org/10.1038/s41563-021-00923-6	journal	February 2021
Stripe phases in WSe2/WS2 moiré superlattices Jin, Chenhao; Tao, Zui; Li, Tingxin Nature Materials https://doi.org/10.1038/s41563-021-00959-8	journal	March 2021
Interlayer valley excitons in heterobilayers of transition metal dichalcogenides Rivera, Pasqual; Yu, Hongyi; Seyler, Kyle L. Nature Nanotechnology, Vol. 13, Issue 11 https://doi.org/10.1038/s41565-018-0193-0	journal	August 2018
Moiré trions in MoSe2/WSe2 heterobilayers Wang, Xi; Zhu, Jiayi; Seyler, Kyle L. Nature Nanotechnology, Vol. 16, Issue 11 https://doi.org/10.1038/s41565-021-00969-2	journal	September 2021
Moiré heterostructures as a condensed-matter quantum simulator Kennes, Dante M.; Claassen, Martin; Xian, Lede Nature Physics, Vol. 17, Issue 2 https://doi.org/10.1038/s41567-020-01154-3	journal	February 2021
Correlated insulating states at fractional fillings of the WS2/WSe2 moiré lattice Huang, Xiong; Wang, Tianmeng; Miao, Shengnan Nature Physics https://doi.org/10.1038/s41567-021-01171-w	journal	February 2021
Dipolar excitonic insulator in a moiré lattice Gu, Jie; Ma, Liguo; Liu, Song Nature Physics, Vol. 18, Issue 4 https://doi.org/10.1038/s41567-022-01532-z	journal	March 2022
Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers Seyler, Kyle L.; Rivera, Pasqual; Yu, Hongyi Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0957-1	journal	February 2019
Evidence for moiré excitons in van der Waals heterostructures Tran, Kha; Moody, Galan; Wu, Fengcheng Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0975-z	journal	February 2019
Observation of moiré excitons in WSe2/WS2 heterostructure superlattices Jin, Chenhao; Regan, Emma C.; Yan, Aiming Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0976-y	journal	February 2019
Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures Alexeev, Evgeny M.; Ruiz-Tijerina, David A.; Danovich, Mark Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0986-9	journal	March 2019
Simulation of Hubbard model physics in WSe2/WS2 moiré superlattices Tang, Yanhao; Li, Lizhong; Li, Tingxin Nature, Vol. 579, Issue 7799 https://doi.org/10.1038/s41586-020-2085-3	journal	March 2020
Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices Regan, Emma C.; Wang, Danqing; Jin, Chenhao Nature, Vol. 579, Issue 7799 https://doi.org/10.1038/s41586-020-2092-4	journal	March 2020
Strongly correlated electrons and hybrid excitons in a moiré heterostructure Shimazaki, Yuya; Schwartz, Ido; Watanabe, Kenji Nature, Vol. 580, Issue 7804 https://doi.org/10.1038/s41586-020-2191-2	journal	April 2020
Correlated insulating states at fractional fillings of moiré superlattices Xu, Yang; Liu, Song; Rhodes, Daniel A. Nature, Vol. 587, Issue 7833 https://doi.org/10.1038/s41586-020-2868-6	journal	November 2020
Signatures of moiré trions in WSe2/MoSe2 heterobilayers Liu, Erfu; Barré, Elyse; van Baren, Jeremiah Nature, Vol. 594, Issue 7861 https://doi.org/10.1038/s41586-021-03541-z	journal	June 2021
Bilayer Wigner crystals in a transition metal dichalcogenide heterostructure Zhou, You; Sung, Jiho; Brutschea, Elise Nature, Vol. 595, Issue 7865 https://doi.org/10.1038/s41586-021-03560-w	journal	June 2021
Quantum criticality in twisted transition metal dichalcogenides Ghiotto, Augusto; Shih, En-Min; Pereira, Giancarlo S. S. G. Nature, Vol. 597, Issue 7876 https://doi.org/10.1038/s41586-021-03815-6	journal	September 2021
Imaging two-dimensional generalized Wigner crystals Li, Hongyuan; Li, Shaowei; Regan, Emma C. Nature, Vol. 597, Issue 7878 https://doi.org/10.1038/s41586-021-03874-9	journal	September 2021
Quantum anomalous Hall effect from intertwined moiré bands Li, Tingxin; Jiang, Shengwei; Shen, Bowen Nature, Vol. 600, Issue 7890 https://doi.org/10.1038/s41586-021-04171-1	journal	December 2021
The SIESTA method for ab initio order- N materials simulation Soler, José M.; Artacho, Emilio; Gale, Julian D. Journal of Physics: Condensed Matter, Vol. 14, Issue 11 https://doi.org/10.1088/0953-8984/14/11/302	journal	March 2002
Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers Yu, Hongyi; Liu, Gui-Bin; Yao, Wang 2D Materials, Vol. 5, Issue 3 https://doi.org/10.1088/2053-1583/aac065	journal	May 2018
Quantum phase diagram of a Moiré-Hubbard model Pan, Haining; Wu, Fengcheng; Das Sarma, Sankar Physical Review B, Vol. 102, Issue 20 https://doi.org/10.1103/PhysRevB.102.201104	journal	November 2020
Electronic structures, charge transfer, and charge order in twisted transition metal dichalcogenide bilayers Zhang, Yang; Liu, Tongtong; Fu, Liang Physical Review B, Vol. 103, Issue 15 https://doi.org/10.1103/PhysRevB.103.155142	journal	April 2021
Hartree-Fock study of the moiré Hubbard model for twisted bilayer transition metal dichalcogenides Zang, Jiawei; Wang, Jie; Cano, Jennifer Physical Review B, Vol. 104, Issue 7 https://doi.org/10.1103/PhysRevB.104.075150	journal	August 2021
Competing magnetic states in transition metal dichalcogenide moiré materials Hu, Nai Chao; MacDonald, Allan H. Physical Review B, Vol. 104, Issue 21 https://doi.org/10.1103/PhysRevB.104.214403	journal	December 2021
Optimized norm-conserving Vanderbilt pseudopotentials Hamann, D. R. Physical Review B, Vol. 88, Issue 8 https://doi.org/10.1103/PhysRevB.88.085117	journal	August 2013
Spin liquid phase of the S = 1 2 J 1 − J 2 Heisenberg model on the triangular lattice Zhu, Zhenyue; White, Steven R. Physical Review B, Vol. 92, Issue 4 https://doi.org/10.1103/PhysRevB.92.041105	journal	July 2015
Anomalous Light Cones and Valley Optical Selection Rules of Interlayer Excitons in Twisted Heterobilayers Yu, Hongyi; Wang, Yong; Tong, Qingjun Physical Review Letters, Vol. 115, Issue 18 https://doi.org/10.1103/PhysRevLett.115.187002	journal	October 2015
Hubbard Model Physics in Transition Metal Dichalcogenide Moiré Bands Wu, Fengcheng; Lovorn, Timothy; Tutuc, Emanuel Physical Review Letters, Vol. 121, Issue 2 https://doi.org/10.1103/PhysRevLett.121.026402	journal	July 2018
Excitonic and Valley-Polarization Signatures of Fractional Correlated Electronic Phases in a WSe 2 / WS 2 Moiré Superlattice Liu, Erfu; Taniguchi, Takashi; Watanabe, Kenji Physical Review Letters, Vol. 127, Issue 3 https://doi.org/10.1103/PhysRevLett.127.037402	journal	July 2021
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Moiré-Trapped Interlayer Trions in a Charge-Tunable WSe 2 / MoSe 2 Heterobilayer Brotons-Gisbert, Mauro; Baek, Hyeonjun; Campbell, Aidan Physical Review X, Vol. 11, Issue 3 https://doi.org/10.1103/PhysRevX.11.031033	journal	August 2021
Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices Yu, Hongyi; Liu, Gui-Bin; Tang, Jianju Science Advances, Vol. 3, Issue 11 https://doi.org/10.1126/sciadv.1701696	journal	November 2017
Highly energy-tunable quantum light from moiré-trapped excitons Baek, H.; Brotons-Gisbert, M.; Koong, Z. X. Science Advances, Vol. 6, Issue 37 https://doi.org/10.1126/sciadv.aba8526	journal	September 2020

Similar Records

Quadrupolar excitons and hybridized interlayer Mott insulator in a trilayer moiré superlattice

Journal Article · Mon Jul 31 20:00:00 EDT 2023 · Nature Communications · OSTI ID:2421625

Exciton Superposition across Moiré States in a Semiconducting Moiré Superlattice

Journal Article · Fri Aug 18 20:00:00 EDT 2023 · Nature Communications · OSTI ID:2421626

Related Subjects

36 MATERIALS SCIENCE
electronic properties and materials
two-dimensional materials

Intercell moiré exciton complexes in electron lattices

Citation Formats

References (43)

Similar Records

Related Subjects