Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Evidence for a monolayer excitonic insulator

Abstract

The interplay between topology and correlations can generate a variety of quantum phases, many of which remain to be explored. Recent advances have identified monolayer WTe2 as a promising material for doing so in a highly tunable fashion. The ground state of this two-dimensional crystal can be electrostatically tuned from a quantum spin Hall insulator to a superconductor. However, much remains unknown about the gap-opening mechanism of the insulating state. Here we report evidence that the quantum spin Hall insulator is also an excitonic insulator, arising from the spontaneous formation of electron–hole bound states, namely excitons. We reveal the presence of an intrinsic insulating state at the charge neutrality point in clean samples and confirm the correlated nature of this charge-neutral insulator by tunnelling spectroscopy. We provide evidence against alternative scenarios of a band insulator or a localized insulator and support the existence of an excitonic insulator phase in the clean limit. These observations lay the foundation for understanding a new class of correlated insulators with nontrivial topology and identify monolayer WTe2 as a promising candidate for exploring quantum phases of ground-state excitons.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Possible scenarios of the ground states at the charge neutrality point in monolayer WTe2.
Fig. 2: The insulating state at charge neutrality in monolayer WTe2.
Fig. 3: Hall anomaly in the monolayer insulator.
Fig. 4: Signature of correlations and the metal–insulator transition revealed by tunnelling spectroscopy.

Similar content being viewed by others

Data availability

The data that support the plots within this paper are available at https://doi.org/10.7910/DVN/FFGQOX. Other data that support the findings of this study are available from the corresponding authors upon reasonable request.

References

  1. Ren, Y., Qiao, Z. & Niu, Q. Topological phases in two-dimensional materials: a review. Rep. Prog. Phys. 79, 066501 (2016).

    Article  ADS  Google Scholar 

  2. Jérome, D., Rice, T. M. & Kohn, W. Excitonic insulator. Phys. Rev. 158, 462–475 (1967).

    Article  ADS  Google Scholar 

  3. Kohn, W. Excitonic phases. Phys. Rev. Lett. 19, 439–442 (1967).

    Article  ADS  Google Scholar 

  4. Blatt, J. M., Böer, K. W. & Brandt, W. Bose-Einstein condensation of excitons. Phys. Rev. 126, 1691–1692 (1962).

    Article  ADS  Google Scholar 

  5. Kotov, V. N., Uchoa, B., Pereira, V. M., Guinea, F. & Castro Neto, A. H. Electron-electron interactions in graphene: current status and perspectives. Rev. Mod. Phys. 84, 1067–1125 (2012).

    Article  ADS  Google Scholar 

  6. Elias, D. C. et al. Dirac cones reshaped by interaction effects in suspended graphene. Nat. Phys. 7, 701–704 (2011).

    Article  Google Scholar 

  7. Varsano, D., Palummo, M., Molinari, E. & Rontani, M. A monolayer transition-metal dichalcogenide as a topological excitonic insulator. Nat. Nanotechnol. 15, 367–372 (2020).

    Article  ADS  Google Scholar 

  8. Zheng, B. & Fu, L. Excitonic density wave and spin-valley superfluid in bilayer transition metal dichalcogenide. Nat. Commun. 12, 642 (2021).

    Article  Google Scholar 

  9. Barkeshli, M., Nayak, C., Papić, Z., Young, A. & Zaletel, M. Topological exciton Fermi surfaces in two-component fractional quantized Hall insulators. Phys. Rev. Lett. 121, 026603 (2018).

    Article  ADS  Google Scholar 

  10. Pikulin, D. I. & Hyart, T. Interplay of exciton condensation and the quantum spin Hall effect in InAs/GaSb bilayers. Phys. Rev. Lett. 112, 176403 (2014).

    Article  ADS  Google Scholar 

  11. Blason, A. & Fabrizio, M. Exciton topology and condensation in a model quantum spin Hall insulator. Phys. Rev. B 102, 035146 (2020).

    Article  ADS  Google Scholar 

  12. Hu, Y., Venderbos, J. W. F. & Kane, C. L. Fractional excitonic insulator. Phys. Rev. Lett. 121, 126601 (2018).

    Article  ADS  Google Scholar 

  13. Chowdhury, D., Sodemann, I. & Senthil, T. Mixed-valence insulators with neutral Fermi surfaces. Nat. Commun. 9, 1766 (2018).

    Article  ADS  Google Scholar 

  14. Cercellier, H. et al. Evidence for an excitonic insulator phase in 1T–TiSe2. Phys. Rev. Lett. 99, 146403 (2007).

    Article  ADS  Google Scholar 

  15. Li, Z. et al. Possible excitonic insulating phase in quantum-confined Sb nanoflakes. Nano Lett. 19, 4960–4964 (2019).

    Article  ADS  Google Scholar 

  16. Kogar, A. et al. Signatures of exciton condensation in a transition metal dichalcogenide. Science 358, 1314–1317 (2017).

    Article  ADS  Google Scholar 

  17. Du, L. et al. Evidence for a topological excitonic insulator in InAs/GaSb bilayers. Nat. Commun. 8, 1971 (2017).

    Article  ADS  Google Scholar 

  18. Wakisaka, Y. et al. Excitonic insulator state in Ta2NiSe5 probed by photoemission spectroscopy. Phys. Rev. Lett. 103, 026402 (2009).

    Article  ADS  Google Scholar 

  19. Lu, Y. F. et al. Zero-gap semiconductor to excitonic insulator transition in Ta2NiSe5. Nat. Commun. 8, 14408 (2017).

    Article  ADS  Google Scholar 

  20. Fukutani, K. et al. Electrical tuning of the excitonic insulator ground state of Ta2NiSe5. Phys. Rev. Lett. 123, 206401 (2019).

    Article  ADS  Google Scholar 

  21. Yu, W. et al. Anomalously large resistance at the charge neutrality point in a zero-gap InAs/GaSb bilayer. New J. Phys. 20, 053062 (2018).

    Article  ADS  Google Scholar 

  22. Eisenstein, J. P. Exciton condensation in bilayer quantum Hall systems. Annu. Rev. Condens. Matter Phys. 5, 159–181 (2014).

    Article  ADS  Google Scholar 

  23. Liu, X., Watanabe, K., Taniguchi, T., Halperin, B. I. & Kim, P. Quantum Hall drag of exciton condensate in graphene. Nat. Phys. 13, 746–750 (2017).

    Article  Google Scholar 

  24. Li, J. I. A., Taniguchi, T., Watanabe, K., Hone, J. & Dean, C. R. Excitonic superfluid phase in double bilayer graphene. Nat. Phys. 13, 751–755 (2017).

    Article  Google Scholar 

  25. Qian, X., Liu, J., Fu, L. & Li, J. Quantum spin Hall effect in two-dimensional transition metal dichalcogenides. Science 346, 1344–1347 (2014).

    Article  ADS  Google Scholar 

  26. Fei, Z. et al. Edge conduction in monolayer WTe2. Nat. Phys. 13, 677–682 (2017).

    Article  Google Scholar 

  27. Tang, S. et al. Quantum spin Hall state in monolayer 1T′-WTe2. Nat. Phys. 13, 683–687 (2017).

    Article  Google Scholar 

  28. Wu, S. et al. Observation of the quantum spin Hall effect up to 100 kelvin in a monolayer crystal. Science 359, 76–79 (2018).

    Article  ADS  MathSciNet  MATH  Google Scholar 

  29. Fatemi, V. et al. Electrically tunable low-density superconductivity in a monolayer topological insulator. Science 362, 926–929 (2018).

    Article  ADS  MathSciNet  Google Scholar 

  30. Sajadi, E. et al. Gate-induced superconductivity in a monolayer topological insulator. Science 362, 922–925 (2018).

    Article  ADS  Google Scholar 

  31. Muechler, L., Alexandradinata, A., Neupert, T. & Car, R. Topological nonsymmorphic metals from band inversion. Phys. Rev. X 6, 041069 (2016).

    Google Scholar 

  32. Zheng, F. et al. On the quantum spin Hall gap of monolayer 1T′-WTe2. Adv. Mater. 28, 4845–4851 (2016).

    Article  Google Scholar 

  33. Xu, S.-Y. et al. Electrically switchable Berry curvature dipole in the monolayer topological insulator WTe2. Nat. Phys. 14, 900–906 (2018).

    Article  Google Scholar 

  34. Song, Y.-H. et al. Observation of Coulomb gap in the quantum spin Hall candidate single-layer 1T′-WTe2. Nat. Commun. 9, 4071 (2018).

    Article  ADS  Google Scholar 

  35. Rhodes, D., Chae, S. H., Ribeiro-Palau, R. & Hone, J. Disorder in van der Waals heterostructures of 2D materials. Nat. Mater. 18, 541–549 (2019).

    Article  ADS  Google Scholar 

  36. Ali, M. N. et al. Correlation of crystal quality and extreme magnetoresistance of WTe2. Europhys. Lett. 110, 67002 (2015).

    Article  ADS  Google Scholar 

  37. Efros, A. L. & Shklovskii, B. I. Coulomb gap and low temperature conductivity of disordered systems. J. Phys. C 8, L49–L51 (1975).

    Article  ADS  Google Scholar 

  38. Kivelson, S., Lee, D.-H. & Zhang, S.-C. Global phase diagram in the quantum Hall effect. Phys. Rev. B 46, 2223–2238 (1992).

    Article  ADS  Google Scholar 

  39. Hilke, M. et al. Experimental evidence for a two-dimensional quantized Hall insulator. Nature 395, 675–677 (1998).

    Article  ADS  Google Scholar 

  40. Ebisawa, H. & Fukuyama, H. Hall effect in excitonic insulator. Prog. Theor. Phys. 42, 512–522 (1969).

    Article  ADS  Google Scholar 

  41. Campbell, D. J. et al. Intrinsic insulating ground state in transition metal dichalcogenide TiSe2. Phys. Rev. Mater. 3, 053402 (2019).

    Article  Google Scholar 

  42. Li, G. et al. Semimetal-to-semimetal charge density wave transition in 1T−TiSe2. Phys. Rev. Lett. 99, 027404 (2007).

    Article  ADS  Google Scholar 

  43. Ponomarenko, L. A. et al. Cloning of Dirac fermions in graphene superlattices. Nature 497, 594–597 (2013).

    Article  ADS  Google Scholar 

  44. Cao, Y. et al. Tunable correlated states and spin-polarized phases in twisted bilayer–bilayer graphene. Nature 583, 215–220 (2020).

    Article  ADS  Google Scholar 

  45. Chandni, U., Watanabe, K., Taniguchi, T. & Eisenstein, J. P. Signatures of phonon and defect-assisted tunneling in planar metal–hexagonal boron nitride–graphene junctions. Nano Lett. 16, 7982–7987 (2016).

    Article  ADS  Google Scholar 

  46. Raja, A. et al. Coulomb engineering of the bandgap and excitons in two-dimensional materials. Nat. Commun. 8, 15251 (2017).

    Article  ADS  Google Scholar 

  47. Zhao, C. et al. Strain tunable semimetal–topological-insulator transition in monolayer 1T′–WTe2. Phys. Rev. Lett. 125, 046801 (2020).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

We acknowledge helpful discussions with N. P. Ong and P. A. Lee. Work in the Wu lab was primarily supported by the National Science Foundation (NSF) through a CAREER award to S.W. (DMR-1942942). Device fabrication was supported by NSF-MRSEC through the Princeton Center for Complex Materials (DMR-1420541 and DMR-2011750). S.W. and L.M.S. acknowledge the support from the Eric and Wendy Schmidt Transformative Technology Fund at Princeton. Part of the measurements was performed at the National High Magnetic Field Laboratory, which is supported by NSF cooperative agreement no. DMR-1644779 and the State of Florida. Work in the Yazdani lab was primarily supported by the Gordon and Betty Moore Foundation EPiQS initiative grants GBMF4530 and GBMF9469 and by the Department of Energy (DOE) BES grant DE-FG02-07ER46419. Other support for the experimental work by A.Y. was provided by NSF (DMR-1904442), ExxonMobil through the Andlinger Center for Energy and the Environment at Princeton, and the Princeton Catalysis Initiative. B.A.B. is supported by DOE grant no. DE-SC0016239, the Schmidt Fund for Innovative Research, Simons Investigator grant no. 404513 and the Packard Foundation for the numerical work. The analytical part was supported by NSF EAGER grant no. DMR-1643312, United States–Israel BSF grant no. 2018226, ONR grant no. N00014-20-1-2303 and the Princeton Global Network Funds. Additional support to B.A.B. was provided by the Gordon and Betty Moore Foundation through grant no. GBMF8685 towards the Princeton theory program. B.J. acknowledges funding through a postdoctoral fellowship of the Alexander-von-Humboldt Foundation. K.W. and T.T. acknowledge support from MEXT Element Strategy Initiative (Japan) grant no. JPMXP0112101001, JSPS KAKENHI grant no. JP20H00354 and the JST CREST (JPMJCR15F3). F.A.C. and R.J.C. acknowledge support from the ARO MURI on Topological Insulators (grant no. W911NF1210461). S.L, S.K. and L.M.S. acknowledge support from the Gordon and Betty Moore Foundation through grant no. GBMF9064 awarded to L.M.S.

Author information

Authors and Affiliations

Authors

Contributions

S.W. supervised transport and vdW tunnelling studies. A.Y. supervised STM studies. P.W. and G.Y. fabricated transport devices. Y.J. fabricated the vdW tunnelling devices, assisted by P.W., G.Y., M.O., N.F. and B.J. Y.J., P.W., and S.W. performed transport and vdW tunnelling measurements and analysed data. C.-L.C., Y.J., P.W. and X.L. fabricated the STM device. C.-L.C., G.F., X.L. and B.J. performed STM measurements and analysed data. Z.S., F.X., Y.X. and B.A.B. provided theoretical support. S.L., S.K., L.M.S., F.A.C. and R.J.C. grew and characterized bulk WTe2 crystals. K.W. and T.T. provided hBN crystals. All authors discussed the result and contributed to the writing of the paper.

Corresponding authors

Correspondence to Ali Yazdani or Sanfeng Wu.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature Physics thanks Vitor Pereira, Jinfeng Jia and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Sections 1–14.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jia, Y., Wang, P., Chiu, CL. et al. Evidence for a monolayer excitonic insulator. Nat. Phys. 18, 87–93 (2022). https://doi.org/10.1038/s41567-021-01422-w

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41567-021-01422-w

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing