DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Tuning moiré excitons and correlated electronic states through layer degree of freedom

Abstract

Moiré coupling in transition metal dichalcogenides (TMDCs) superlattices introduces flat minibands that enable strong electronic correlation and fascinating correlated states, and it also modifies the strong Coulomb-interaction-driven excitons and gives rise to moiré excitons. Here, we introduce the layer degree of freedom to the WSe2/WS2 moiré superlattice by changing WSe2 from monolayer to bilayer and trilayer. We observe systematic changes of optical spectra of the moiré excitons, which directly confirm the highly interfacial nature of moiré coupling at the WSe2/WS2 interface. In addition, the energy resonances of moiré excitons are strongly modified, with their separation significantly increased in multilayer WSe2/monolayer WS2 moiré superlattice. The additional WSe2 layers also modulate the strong electronic correlation strength, evidenced by the reduced Mott transition temperature with added WSe2 layer(s). The layer dependence of both moiré excitons and correlated electronic states can be well described by our theoretical model. Our study presents a new method to tune the strong electronic correlation and moiré exciton bands in the TMDCs moiré superlattices, ushering in an exciting platform to engineer quantum phenomena stemming from strong correlation and Coulomb interaction.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [3];  [2];  [5]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [5]; ORCiD logo [7]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [2]
  1. University of Electronic Science and Technology of China, Chengdu (China); Rensselaer Polytechnic Institute, Troy, NY (United States)
  2. Rensselaer Polytechnic Institute, Troy, NY (United States)
  3. University of California, Riverside, CA (United States)
  4. University of Texas at Dallas, TX (United States)
  5. Arizona State University, Tempe, AZ (United States)
  6. National Institute for Materials Science, Tsukuba (Japan)
  7. University of Electronic Science and Technology of China, Chengdu (China)
Publication Date:
Research Org.:
Florida State Univ., Tallahassee, FL (United States); Arizona State Univ., Tempe, AZ (United States)
Sponsoring Org.:
USDOE Office of Science (SC); US Air Force Office of Scientific Research (AFOSR); NYSTAR; National Science Foundation (NSF); Army Research Office (ARO); National Natural Science Foundation of China (NSFC); Japan Society for the Promotion of Science (JSPS)
OSTI Identifier:
1904628
Grant/Contract Number:  
FG02-07ER46451; SC0020653; FA9550-20-1-0179; C150117; DMR-1945420; DMR-2104902; FA9550-18-1-0312; DMR- 2104805; PHY-2110212; PHY-1806227; W911NF17-1-0128; FA9550-20-1-0220; 62004032; DMR-1904716; DMR-1838443; CMMI-1933214; JPMXP0112101001; DMR-1644779
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 42 ENGINEERING; electronic properties and materials; two-dimensional materials

Citation Formats

Chen, Dongxue, Lian, Zhen, Huang, Xiong, Su, Ying, Rashetnia, Mina, Yan, Li, Blei, Mark, Taniguchi, Takashi, Watanabe, Kenji, Tongay, Sefaattin, Wang, Zenghui, Zhang, Chuanwei, Cui, Yong-Tao, and Shi, Su-Fei. Tuning moiré excitons and correlated electronic states through layer degree of freedom. United States: N. p., 2022. Web. doi:10.1038/s41467-022-32493-9.
Chen, Dongxue, Lian, Zhen, Huang, Xiong, Su, Ying, Rashetnia, Mina, Yan, Li, Blei, Mark, Taniguchi, Takashi, Watanabe, Kenji, Tongay, Sefaattin, Wang, Zenghui, Zhang, Chuanwei, Cui, Yong-Tao, & Shi, Su-Fei. Tuning moiré excitons and correlated electronic states through layer degree of freedom. United States. https://doi.org/10.1038/s41467-022-32493-9
Chen, Dongxue, Lian, Zhen, Huang, Xiong, Su, Ying, Rashetnia, Mina, Yan, Li, Blei, Mark, Taniguchi, Takashi, Watanabe, Kenji, Tongay, Sefaattin, Wang, Zenghui, Zhang, Chuanwei, Cui, Yong-Tao, and Shi, Su-Fei. Tue . "Tuning moiré excitons and correlated electronic states through layer degree of freedom". United States. https://doi.org/10.1038/s41467-022-32493-9. https://www.osti.gov/servlets/purl/1904628.
@article{osti_1904628,
title = {Tuning moiré excitons and correlated electronic states through layer degree of freedom},
author = {Chen, Dongxue and Lian, Zhen and Huang, Xiong and Su, Ying and Rashetnia, Mina and Yan, Li and Blei, Mark and Taniguchi, Takashi and Watanabe, Kenji and Tongay, Sefaattin and Wang, Zenghui and Zhang, Chuanwei and Cui, Yong-Tao and Shi, Su-Fei},
abstractNote = {Moiré coupling in transition metal dichalcogenides (TMDCs) superlattices introduces flat minibands that enable strong electronic correlation and fascinating correlated states, and it also modifies the strong Coulomb-interaction-driven excitons and gives rise to moiré excitons. Here, we introduce the layer degree of freedom to the WSe2/WS2 moiré superlattice by changing WSe2 from monolayer to bilayer and trilayer. We observe systematic changes of optical spectra of the moiré excitons, which directly confirm the highly interfacial nature of moiré coupling at the WSe2/WS2 interface. In addition, the energy resonances of moiré excitons are strongly modified, with their separation significantly increased in multilayer WSe2/monolayer WS2 moiré superlattice. The additional WSe2 layers also modulate the strong electronic correlation strength, evidenced by the reduced Mott transition temperature with added WSe2 layer(s). The layer dependence of both moiré excitons and correlated electronic states can be well described by our theoretical model. Our study presents a new method to tune the strong electronic correlation and moiré exciton bands in the TMDCs moiré superlattices, ushering in an exciting platform to engineer quantum phenomena stemming from strong correlation and Coulomb interaction.},
doi = {10.1038/s41467-022-32493-9},
journal = {Nature Communications},
number = 1,
volume = 13,
place = {United States},
year = {Tue Aug 16 00:00:00 EDT 2022},
month = {Tue Aug 16 00:00:00 EDT 2022}
}

Works referenced in this record:

Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices
journal, November 2017


Electrically tunable correlated and topological states in twisted monolayer–bilayer graphene
journal, October 2020


Correlated electronic phases in twisted bilayer transition metal dichalcogenides
journal, June 2020


Unconventional superconductivity in magic-angle graphene superlattices
journal, March 2018


Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices
journal, March 2020


Intrinsic quantized anomalous Hall effect in a moiré heterostructure
journal, December 2019


Emergent ferromagnetism near three-quarters filling in twisted bilayer graphene
journal, July 2019


Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

Nanoscale Conductivity Imaging of Correlated Electronic States in WSe 2 / WS 2 Moiré Superlattices
journal, October 2020


Imaging moiré flat bands in three-dimensional reconstructed WSe2/WS2 superlattices
journal, February 2021


Evidence of a gate-tunable Mott insulator in a trilayer graphene moiré superlattice
journal, January 2019


Correlated insulating states at fractional fillings of the WS2/WSe2 moiré lattice
journal, February 2021


Simulation of Hubbard model physics in WSe2/WS2 moiré superlattices
journal, March 2020


Correlated insulating states at fractional fillings of moiré superlattices
journal, November 2020


Tunable correlated Chern insulator and ferromagnetism in a moiré superlattice
journal, March 2020


Observation of moiré excitons in WSe2/WS2 heterostructure superlattices
journal, February 2019


Electrical switching of magnetic order in an orbital Chern insulator
journal, November 2020


Bilayer Wigner crystals in a transition metal dichalcogenide heterostructure
journal, June 2021


Exciton band structure of monolayer MoS 2
journal, February 2015


Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moiré superlattice
journal, June 2021


Tailoring excitonic states of van der Waals bilayers through stacking configuration, band alignment, and valley spin
journal, December 2019


Moire bands in twisted double-layer graphene
journal, July 2011

  • Bistritzer, R.; MacDonald, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 30
  • DOI: 10.1073/pnas.1108174108

Tunable spin-polarized correlated states in twisted double bilayer graphene
journal, July 2020


Correlated insulator behaviour at half-filling in magic-angle graphene superlattices
journal, March 2018


One-Dimensional Electrical Contact to a Two-Dimensional Material
journal, October 2013


Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States
journal, November 2013


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

Atomically Thin MoS2 A New Direct-Gap Semiconductor
journal, September 2010


Tunable van Hove singularities and correlated states in twisted monolayer–bilayer graphene
journal, February 2021


Spin–layer locking effects in optical orientation of exciton spin in bilayer WSe2
journal, January 2014

  • Jones, Aaron M.; Yu, Hongyi; Ross, Jason S.
  • Nature Physics, Vol. 10, Issue 2
  • DOI: 10.1038/nphys2848

Signatures of tunable superconductivity in a trilayer graphene moiré superlattice
journal, July 2019


Tunable correlated states and spin-polarized phases in twisted bilayer–bilayer graphene
journal, May 2020


Correlated states in twisted double bilayer graphene
journal, March 2020


Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides
journal, May 2014

  • Yu, Hongyi; Liu, Gui-Bin; Gong, Pu
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4876

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2
journal, August 2014


Topological Exciton Bands in Moiré Heterojunctions
journal, April 2017


Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014

  • Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
  • Nature Materials, Vol. 13, Issue 12
  • DOI: 10.1038/nmat4061

Signatures of Wigner crystal of electrons in a monolayer semiconductor
journal, June 2021