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  Quadrupolar–dipolar excitonic transition in a tunnel-coupled van der Waals heterotrilayer

Li, W., Hadjri, Z., Devenica, L. M., Zhang, J., Liu, S., Hone, J., et al. (2023). Quadrupolar–dipolar excitonic transition in a tunnel-coupled van der Waals heterotrilayer. Nature Materials, 22(12), 1478-1484. doi:10.1038/s41563-023-01667-1.

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Item Permalink: https://hdl.handle.net/21.11116/0000-000A-D878-C Version Permalink: https://hdl.handle.net/21.11116/0000-000E-07AF-6
Genre: Journal Article

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Supplementary information: Supplementary Figs. 1–13 and Notes 1–3 (pdf), Calculations of model in Extended Data Fig. 1 (m); Source data: Optical measurement source data Fig. 1-4 (xlsx), Optical measurement source data Fig. 4 (xlsx), Optical measurement source data Fig. 1 (xlsx), Optical measurement source data Fig. 2 (xlsx)
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News & Views article "Quadrupolar excitons take the stage" by E. Barré, M. Dandu and A. Raja
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 Creators:
Li, W.1, Author
Hadjri, Z.1, Author
Devenica, L. M.1, Author
Zhang, J.2, 3, Author           
Liu, S.4, 5, Author
Hone, J.4, Author
Watanabe, K.6, Author
Taniguchi, T.7, Author
Rubio, A.2, 3, 8, 9, Author           
Srivastava, A.1, 10, Author
Affiliations:
1Department of Physics, Emory University, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science, ou_persistent22              
4Department of Mechanical Engineering, Columbia University, ou_persistent22              
5Institute of Microelectronics, Chinese Academy of Sciences, ou_persistent22              
6Research Center for Electronic and Optical Materials, National Institute for Materials Science, ou_persistent22              
7Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, ou_persistent22              
8Center for Computational Quantum Physics, Simons Foundation Flatiron Institute, ou_persistent22              
9Nano-Bio Spectroscopy Group, Departamento de Fisica de Materiales, Universidad del Paìs Vasco, ou_persistent22              
10Department of Quantum Matter Physics, University of Geneva, ou_persistent22              

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 Abstract: Strongly bound excitons determine light–matter interactions in van der Waals heterostructures of two-dimensional semiconductors. Unlike fundamental particles, quasiparticles in condensed matter, such as excitons, can be tailored to alter their interactions and realize emergent quantum phases. Here, using a WS2/WSe2/WS2 heterotrilayer, we create a quantum superposition of oppositely oriented dipolar excitons—a quadrupolar exciton—wherein an electron is layer-hybridized in WS2 layers while the hole localizes in WSe2. In contrast to dipolar excitons, symmetric quadrupolar excitons only redshift in an out-of-plane electric field. At higher densities and a finite electric field, the nonlinear Stark shift of quadrupolar excitons becomes linear, signalling a transition to dipolar excitons resulting from exciton–exciton interactions, while at a vanishing electric field, the reduced exchange interaction suggests antiferroelectric correlations between dipolar excitons. Our results present van der Waals heterotrilayers as a field-tunable platform to engineer light–matter interactions and explore quantum phase transitions between spontaneously ordered many-exciton phases.

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Language(s): eng - English
 Dates: 2022-09-272023-08-212023-10-192023-12
 Publication Status: Issued
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2208.05490
DOI: 10.1038/s41563-023-01667-1
 Degree: -

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Project name : -
Grant ID : 886291
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)
Project name : We thank H. Harutyunyan for help with lifetime measurements and T. Heinz, L. Yu, B. Shklovskii, R. Rapaport and M. Claassen for insightful discussions. This work was supported by the National Science Foundation (NSF) Emerging Frontiers in Research and Innovation programme (grant no. EFMA-1741691 to A.S.), the NSF Division of Materials Research (award no. 1905809 to A.S.) and the State Secretariat for Education, Research and Innovation (SERI)-funded European Research Council Consolidator Grant TuneInt2Quantum (no. 101043957 to A.S.). The computational work was supported by the European Research Council (no. ERC-2015-AdG694097), the Cluster of Excellence ‘Advanced Imaging of Matter’, the collaborative research centre SFB925 and Grupos Consolidados (no. IT1249-19). We acknowledge support by the Max Planck Institute – New York City Center for Non-equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. J.Z. acknowledges funding received from the European Union Horizon 2020 research and innovation programme under Marie Sklodowska-Curie Grant Agreement 886291 (PeSD-NeSL). Synthesis of WSe2 (S.L. and J.H.) was supported by the NSF Materials Research Science and Engineering Centers programme through the Columbia University Center for Precision-Assembled Quantum Materials (DMR-2011738). K.W. and T.T. acknowledge support from the Japan Society for the Promotion of Science KAKENHI (grant nos 21H05233 and 23H02052) and World Premier International Research Center Initiative, Ministry of Education, Culture, Sports, Science and Technology, Japan.
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Title: Nature Materials
  Abbreviation : Nat. Mater.
Source Genre: Journal
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Publ. Info: London, UK : Nature Pub. Group
Pages: - Volume / Issue: 22 (12) Sequence Number: - Start / End Page: 1478 - 1484 Identifier: ISSN: 1476-1122
CoNE: https://pure.mpg.de/cone/journals/resource/111054835734000