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Title: Evidence for moiré excitons in van der Waals heterostructures

Abstract

Recent advances in the isolation and stacking of monolayers of van der Waals materials have provided approaches for the preparation of quantum materials in the ultimate two-dimensional limit(1,2). In van der Waals heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moire superlattice(3). It is widely recognized that the moire superlattice can modulate the electronic band structure of the material and lead to transport properties such as unconventional superconductivity(4) and insulating behaviour driven by correlations(5-7); however, the influence of the moire superlattice on optical properties has not been investigated experimentally. Here we report the observation of multiple interlayer exciton resonances with either positive or negative circularly polarized emission in a molybdenum diselenide/tungsten diselenide (MoSe 2/WSe 2) heterobilayer with a small twist angle. We attribute these resonances to excitonic ground and excited states confined within the moire potential. This interpretation is supported by recombination dynamics and by the dependence of these interlayer exciton resonances on twist angle and temperature. These results suggest the feasibility of engineering artificial excitonic crystals using van der Waals heterostructures for nanophotonics and quantum information applications.

Authors:
 [1];  [2];  [3];  [4];  [1];  [5];  [5];  [6];  [1];  [1];  [1];  [1];  [1];  [2];  [7];  [7];  [8];  [5];  [2];  [9] more »;  [5];  [4];  [1];  [1] « less
  1. Univ. of Texas, Austin, TX (United States). Dept. of Physics and Center for Complex Quantum Systems
  2. National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  4. Washington Univ., St. Louis, MO (United States). Dept. of Physics
  5. Univ. of Texas, Austin, TX (United States). Microelectronics Research Center, Dept. of Electrical and Computer Engineering
  6. Univ. of Texas, Austin, TX (United States). Dept. of Aerospace Engineering and Engineering Mechanics
  7. National Inst. of Material Science, Ibaraki (Japan)
  8. Univ. of Texas, Austin, TX (United States). Dept. of Aerospace Engineering and Engineering Mechanics, and Texas Materials Inst.
  9. Hanyang Univ., Ansan (Korea). Dept. of Photonics and Nanoelectronics and Dept. of Applied Physics
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); Welch Foundation; China Scholarship Council; US Army Research Office (ARO); Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR); National Research Foundation of Korea (NRF); Japan Society for the Promotion of Science (JSPS) - KAKENHI
OSTI Identifier:
1503250
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Volume: 567; Journal Issue: 7746; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 42 ENGINEERING; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Tran, Kha, Moody, Galan, Wu, Fengcheng, Lu, Xiaobo, Choi, Junho, Kim, Kyounghwan, Rai, Amritesh, Sanchez, Daniel A., Quan, Jiamin, Singh, Akshay, Embley, Jacob, Zepeda, André, Campbell, Marshall, Autry, Travis, Taniguchi, Takashi, Watanabe, Kenji, Lu, Nanshu, Banerjee, Sanjay K., Silverman, Kevin L., Kim, Suenne, Tutuc, Emanuel, Yang, Li, MacDonald, Allan H., and Li, Xiaoqin. Evidence for moiré excitons in van der Waals heterostructures. United States: N. p., 2019. Web. doi:10.1038/s41586-019-0975-z.
Tran, Kha, Moody, Galan, Wu, Fengcheng, Lu, Xiaobo, Choi, Junho, Kim, Kyounghwan, Rai, Amritesh, Sanchez, Daniel A., Quan, Jiamin, Singh, Akshay, Embley, Jacob, Zepeda, André, Campbell, Marshall, Autry, Travis, Taniguchi, Takashi, Watanabe, Kenji, Lu, Nanshu, Banerjee, Sanjay K., Silverman, Kevin L., Kim, Suenne, Tutuc, Emanuel, Yang, Li, MacDonald, Allan H., & Li, Xiaoqin. Evidence for moiré excitons in van der Waals heterostructures. United States. doi:10.1038/s41586-019-0975-z.
Tran, Kha, Moody, Galan, Wu, Fengcheng, Lu, Xiaobo, Choi, Junho, Kim, Kyounghwan, Rai, Amritesh, Sanchez, Daniel A., Quan, Jiamin, Singh, Akshay, Embley, Jacob, Zepeda, André, Campbell, Marshall, Autry, Travis, Taniguchi, Takashi, Watanabe, Kenji, Lu, Nanshu, Banerjee, Sanjay K., Silverman, Kevin L., Kim, Suenne, Tutuc, Emanuel, Yang, Li, MacDonald, Allan H., and Li, Xiaoqin. Mon . "Evidence for moiré excitons in van der Waals heterostructures". United States. doi:10.1038/s41586-019-0975-z. https://www.osti.gov/servlets/purl/1503250.
@article{osti_1503250,
title = {Evidence for moiré excitons in van der Waals heterostructures},
author = {Tran, Kha and Moody, Galan and Wu, Fengcheng and Lu, Xiaobo and Choi, Junho and Kim, Kyounghwan and Rai, Amritesh and Sanchez, Daniel A. and Quan, Jiamin and Singh, Akshay and Embley, Jacob and Zepeda, André and Campbell, Marshall and Autry, Travis and Taniguchi, Takashi and Watanabe, Kenji and Lu, Nanshu and Banerjee, Sanjay K. and Silverman, Kevin L. and Kim, Suenne and Tutuc, Emanuel and Yang, Li and MacDonald, Allan H. and Li, Xiaoqin},
abstractNote = {Recent advances in the isolation and stacking of monolayers of van der Waals materials have provided approaches for the preparation of quantum materials in the ultimate two-dimensional limit(1,2). In van der Waals heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moire superlattice(3). It is widely recognized that the moire superlattice can modulate the electronic band structure of the material and lead to transport properties such as unconventional superconductivity(4) and insulating behaviour driven by correlations(5-7); however, the influence of the moire superlattice on optical properties has not been investigated experimentally. Here we report the observation of multiple interlayer exciton resonances with either positive or negative circularly polarized emission in a molybdenum diselenide/tungsten diselenide (MoSe2/WSe2) heterobilayer with a small twist angle. We attribute these resonances to excitonic ground and excited states confined within the moire potential. This interpretation is supported by recombination dynamics and by the dependence of these interlayer exciton resonances on twist angle and temperature. These results suggest the feasibility of engineering artificial excitonic crystals using van der Waals heterostructures for nanophotonics and quantum information applications.},
doi = {10.1038/s41586-019-0975-z},
journal = {Nature (London)},
issn = {0028-0836},
number = 7746,
volume = 567,
place = {United States},
year = {2019},
month = {2}
}

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Works referenced in this record:

Heterostructures based on two-dimensional layered materials and their potential applications
journal, July 2016


Van der Waals heterostructures and devices
journal, July 2016


Interlayer couplings, Moiré patterns, and 2D electronic superlattices in MoS 2 /WSe 2 hetero-bilayers
journal, January 2017


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


Massive Dirac Fermions and Hofstadter Butterfly in a van der Waals Heterostructure
journal, May 2013


Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices
journal, May 2013


Tunable moiré bands and strong correlations in small-twist-angle bilayer graphene
journal, March 2017

  • Kim, Kyounghwan; DaSilva, Ashley; Huang, Shengqiang
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 13
  • DOI: 10.1073/pnas.1620140114

Tailoring the Electronic Structure in Bilayer Molybdenum Disulfide via Interlayer Twist
journal, June 2014

  • van der Zande, Arend M.; Kunstmann, Jens; Chernikov, Alexey
  • Nano Letters, Vol. 14, Issue 7
  • DOI: 10.1021/nl501077m

Band offsets and heterostructures of two-dimensional semiconductors
journal, January 2013

  • Kang, Jun; Tongay, Sefaattin; Zhou, Jian
  • Applied Physics Letters, Vol. 102, Issue 1
  • DOI: 10.1063/1.4774090

Electronic properties of the MoS 2 -WS 2 heterojunction
journal, February 2013


Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014

  • Hong, Xiaoping; Kim, Jonghwan; Shi, Su-Fei
  • Nature Nanotechnology, Vol. 9, Issue 9
  • DOI: 10.1038/nnano.2014.167

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
  • DOI: 10.1038/ncomms7242

Vertical and in-plane heterostructures from WS2/MoS2 monolayers
journal, September 2014

  • Gong, Yongji; Lin, Junhao; Wang, Xingli
  • Nature Materials, Vol. 13, Issue 12, p. 1135-1142
  • DOI: 10.1038/nmat4091

Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers
journal, January 2018


Topological Exciton Bands in Moiré Heterojunctions
journal, April 2017


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


Interlayer excitons in MoSe 2 / WSe 2 heterostructures from first principles
journal, April 2018


Anomalous Light Cones and Valley Optical Selection Rules of Interlayer Excitons in Twisted Heterobilayers
journal, October 2015


Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
journal, April 2014


Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure
journal, June 2017


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

  • Nagler, Philipp; Ballottin, Mariana V.; Mitioglu, Anatolie A.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/s41467-017-01748-1

Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012

  • Zeng, Hualing; Dai, Junfeng; Yao, Wang
  • Nature Nanotechnology, Vol. 7, Issue 8
  • DOI: 10.1038/nnano.2012.95

Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012


Disorder-dependent valley properties in monolayer WS e 2
journal, July 2017


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
  • DOI: 10.1038/ncomms13747

Ground and excited state energy trend in In As In Ga As quantum dots monitored by scanning photoluminescence spectroscopy
journal, November 2005


Momentum-space indirect interlayer excitons in transition-metal dichalcogenide van der Waals heterostructures
journal, April 2018


Probing Evolution of Twist-Angle-Dependent Interlayer Excitons in MoSe 2 /WSe 2 van der Waals Heterostructures
journal, April 2017


Polarization switching and electrical control of interlayer excitons in two-dimensional van der Waals heterostructures
journal, December 2018


Double Indirect Interlayer Exciton in a MoSe 2 /WSe 2 van der Waals Heterostructure
journal, April 2018

  • Hanbicki, Aubrey T.; Chuang, Hsun-Jen; Rosenberger, Matthew R.
  • ACS Nano, Vol. 12, Issue 5
  • DOI: 10.1021/acsnano.8b01369

Electrical Tuning of Interlayer Exciton Gases in WSe 2 Bilayers
journal, December 2017


Second harmonic microscopy of monolayer MoS 2
journal, April 2013


Observation of intense second harmonic generation from MoS 2 atomic crystals
journal, May 2013

  • Malard, Leandro M.; Alencar, Thonimar V.; Barboza, Ana Paula M.
  • Physical Review B, Vol. 87, Issue 20
  • DOI: 10.1103/PhysRevB.87.201401

Frequency-domain interferometric second-harmonic spectroscopy
journal, January 1999

  • Wilson, P. T.; Jiang, Y.; Aktsipetrov, O. A.
  • Optics Letters, Vol. 24, Issue 7
  • DOI: 10.1364/OL.24.000496

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Linear techniques of phase measurement by femtosecond spectral interferometry for applications in spectroscopy
journal, January 1995

  • Lepetit, L.; Chériaux, G.; Joffre, M.
  • Journal of the Optical Society of America B, Vol. 12, Issue 12, p. 2467-2474
  • DOI: 10.1364/JOSAB.12.002467

Phase-sensitive detection technique for surface nonlinear optics
journal, December 1998


Thermal dissociation of inter-layer excitons in MoS 2 /MoSe 2 hetero-bilayers
journal, January 2017

  • Mouri, Shinichiro; Zhang, Wenjing; Kozawa, Daichi
  • Nanoscale, Vol. 9, Issue 20
  • DOI: 10.1039/C7NR01598D

Combined influence of Coulomb interaction and polarons on the carrier dynamics in InGaAs quantum dots
journal, November 2013


Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers
journal, May 2018


Probing the Spin-Polarized Electronic Band Structure in Monolayer Transition Metal Dichalcogenides by Optical Spectroscopy
journal, January 2017


In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
journal, July 2017


    Works referencing / citing this record:

    Tunable Moiré Superlattice of Artificially Twisted Monolayers
    journal, July 2019

    • Chen, Po‐Yen; Zhang, Xin‐Quan; Lai, Ying‐Yu
    • Advanced Materials, Vol. 31, Issue 37
    • DOI: 10.1002/adma.201901077

    Nonlinear optics of two‐dimensional transition metal dichalcogenides
    journal, July 2019


    Tunable Moiré Superlattice of Artificially Twisted Monolayers
    journal, July 2019

    • Chen, Po‐Yen; Zhang, Xin‐Quan; Lai, Ying‐Yu
    • Advanced Materials, Vol. 31, Issue 37
    • DOI: 10.1002/adma.201901077

    Nonlinear optics of two‐dimensional transition metal dichalcogenides
    journal, July 2019


    General synthesis of two-dimensional van der Waals heterostructure arrays
    journal, March 2020