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Observation of quadrupolar and dipolar excitons in a semiconductor heterotrilayer

Nature Materials volume 22, pages 1485–1491 (2023)Cite this article

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Abstract

Van der Waals (vdW) materials have opened up many avenues for discovery through layer assembly, as epitomized by interlayer dipolar excitons that exhibit electrically tunable luminescence, lasing and exciton condensation. Extending interlayer excitons to more vdW layers, however, raises fundamental questions concerning coherence within excitons and coupling between moiré superlattices at multiple interfaces. Here, by assembling angle-aligned WSe2/WS2/WSe2 heterotrilayers, we demonstrate the emergence of quadrupolar excitons. We confirm the exciton’s quadrupolar nature by the decrease in its energy of 12 meV from coherent hole tunnelling between the two outer layers, its tunable static dipole moment under an external electric field and the reduced exciton–exciton interactions. At high exciton density, we also see signatures of a phase of oppositely aligned dipolar excitons, consistent with a staggered dipolar phase predicted to be driven by attractive dipolar interactions. Our demonstration paves the way for discovering emergent exciton orderings for three vdW layers and beyond.

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Fig. 1: Device structure and electric-field control of different exciton species.
Fig. 2: Electrical-field tuning of dipolar and quadrupolar interlayer excitons observed in the PL.
Fig. 3: Density-dependent spectra showing the interactions between excitons.
Fig. 4: PFM images of heterobilayers and heterotrilayers.
Fig. 5: Signatures of dipolar exciton ordering in a heterotrilayer at elevated exciton densities.

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Source data are provided with this paper. All other datasets generated during and/or analysed during this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

This work was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under award number DE-SC0020115 and, for sample preparation, under SLAC FWP 100459. Additional support was provided for sample preparation and analysis by the Betty and Gordon Moore Foundation EPiQS Initiative through Grant No. GBMF9462 and for a graduate fellowship for J.H. by NTT Research. Sample fabrication and the PFM characterization were performed at the Stanford Nano Shared Facilities, supported by the National Science Foundation under award ECCS-2026822. K.W. and T.T. acknowledge support from the Japan Society for the Promotion of Science (KAKENHI Grant Numbers 21H05233 and 23H02052) and the World Premier International Research Center Initiative, Ministry of Education, Culture, Sports, Science and Technology, Japan.

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Author notes

  1. These authors contributed equally: Leo Yu, Kateryna Pistunova.

Authors and Affiliations

  1. E. L. Ginzton Laboratory, Stanford University, Stanford, CA, USA

    Leo Yu, Kateryna Pistunova, Jenny Hu & Tony F. Heinz

  2. SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Leo Yu, Kateryna Pistunova & Tony F. Heinz

  3. Research Center for Electronic and Optical Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

  4. Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

    Takashi Taniguchi

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  1. Leo Yu
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Contributions

L.Y. conceived the project. K.P. and L.Y. fabricated the samples. L.Y. and K.P. performed the optical measurements. K.P. and J.H. performed the PFM measurements. T.T. and K.W. synthesized the h-BN crystals. T.F.H. supervised the project. L.Y., T.F.H. and K.P. wrote the paper with input from all authors.

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Correspondence to Leo Yu or Tony F. Heinz.

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Supplementary Notes 1–8 and Figs. 1–8.

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Yu, L., Pistunova, K., Hu, J. et al. Observation of quadrupolar and dipolar excitons in a semiconductor heterotrilayer. Nat. Mater. 22, 1485–1491 (2023). https://doi.org/10.1038/s41563-023-01678-y

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