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Superconductivity in twisted double bilayer graphene stabilized by WSe2

Nature Materials volume 22, pages 1332–1337 (2023)Cite this article

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Abstract

Identifying the essential components of superconductivity in graphene-based systems remains a critical problem in two-dimensional materials research. This field is connected to the mysteries that underpin investigations of unconventional superconductivity in condensed-matter physics. Superconductivity has been observed in magic-angle twisted stacks of monolayer graphene but conspicuously not in twisted stacks of bilayer graphene, although both systems host topological flat bands and symmetry-broken states. Here we report the discovery of superconductivity in twisted double bilayer graphene (TDBG) in proximity to WSe2. Samples with twist angles 1.24° and 1.37° superconduct in small pockets of the gate-tuned phase diagram within the valence and conduction band, respectively. Superconductivity emerges from unpolarized phases near van Hove singularities and next to regions with broken isospin symmetry. Our results show the correlation between a high density of states and the emergence of superconductivity in TDBG while revealing a possible role for isospin fluctuations in the pairing.

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Fig. 1: Device characterization.
Fig. 2: Signatures of superconductivity.
Fig. 3: Metrics of superconductivity in D1.
Fig. 4: Van Hove singularities and isospin-polarized phases.

Data availability

Source data are provided with this paper. All other data are available from the corresponding author upon reasonable request.

Code availability

Codes used for data analysis in this study are also available from the corresponding author upon reasonable request.

References

  1. Cao, Y. et al. Unconventional superconductivity in magic-angle graphene superlattices. Nature 556, 43–50 (2018).

    Article  CAS  Google Scholar 

  2. Park, J. M., Cao, Y., Watanabe, K., Taniguchi, T. & Jarillo-Herrero, P. Tunable strongly coupled superconductivity in magic-angle twisted trilayer graphene. Nature 590, 249–255 (2021).

    Article  CAS  Google Scholar 

  3. Hao, Z. et al. Electric field–tunable superconductivity in alternating-twist magic-angle trilayer graphene. Science 371, 1133–1138 (2021).

    Article  CAS  Google Scholar 

  4. Park, J. M. et al. Robust superconductivity in magic-angle multilayer graphene family. Nat. Mater. 21, 877–883 (2022).

    Article  CAS  Google Scholar 

  5. Zhang, Y. et al. Promotion of superconductivity in magic-angle graphene multilayers. Science 377, 1538–1543 (2022).

    Article  CAS  Google Scholar 

  6. Zhou, H., Xie, T., Taniguchi, T., Watanabe, K. & Young, A. F. Superconductivity in rhombohedral trilayer graphene. Nature 598, 434–438 (2021).

    Article  CAS  Google Scholar 

  7. Zhou, H. et al. Isospin magnetism and spin-polarized superconductivity in Bernal bilayer graphene. Science 375, 774–778 (2022).

    Article  CAS  Google Scholar 

  8. Bistritzer, R. & MacDonald, A. H. Moiré bands in twisted double-layer graphene. Proc. Natl Acad. Sci. USA 108, 12233–12237 (2011).

    Article  CAS  Google Scholar 

  9. Balents, L., Dean, C. R., Efetov, D. K. & Young, A. F. Superconductivity and strong correlations in moiré flat bands. Nat. Phys. 16, 725–733 (2020).

    Article  CAS  Google Scholar 

  10. You, Y.-Z. & Vishwanath, A. Kohn–Luttinger superconductivity and intervalley coherence in rhombohedral trilayer graphene. Phys. Rev. B 105, 134524 (2022).

    Article  CAS  Google Scholar 

  11. Chou, Y.-Z., Wu, F., Sau, J. D. & Sarma, S. D. Correlation-induced triplet pairing superconductivity in graphene-based moiré systems. Phys. Rev. Lett. 127, 217001 (2021).

    Article  CAS  Google Scholar 

  12. Lian, B., Wang, Z. & Bernevig, B. A. Twisted bilayer graphene: a phonon-driven superconductor. Phys. Rev. Lett. 122, 257002 (2019).

    Article  CAS  Google Scholar 

  13. Wu, F., MacDonald, A. H. & Martin, I. Theory of phonon-mediated superconductivity in twisted bilayer graphene. Phys. Rev. Lett. 121, 257001 (2018).

    Article  CAS  Google Scholar 

  14. Khalaf, E., Chatterjee, S., Bultinck, N., Zaletel, M. P. & Vishwanath, A. Charged skyrmions and topological origin of superconductivity in magic-angle graphene. Sci. Adv. 7, eabf5299 (2021).

    Article  CAS  Google Scholar 

  15. You, Y.-Z. & Vishwanath, A. Superconductivity from valley fluctuations and approximate SO(4) symmetry in a weak coupling theory of twisted bilayer graphene. NPJ Quantum Mater. 4, 16 (2019).

    Article  Google Scholar 

  16. Lee, J. Y. et al. Theory of correlated insulating behaviour and spin-triplet superconductivity in twisted double bilayer graphene. Nat. Commun. 10, 5333 (2019).

    Article  Google Scholar 

  17. Arora, H. S. et al. Superconductivity in metallic twisted bilayer graphene stabilized by WSe2. Nature 583, 379–384 (2020).

    Article  CAS  Google Scholar 

  18. Zhang, Y. et al. Enhanced superconductivity in spin–orbit proximitized bilayer graphene. Nature 613, 268–273 (2023).

    Article  CAS  Google Scholar 

  19. Holleis, L. et al. Ising superconductivity and nematicity in Bernal bilayer graphene with strong spin orbit coupling. Preprint at arXiv https://doi.org/10.48550/arXiv.2303.00742 (2023).

  20. Lu, X. et al. Superconductors, orbital magnets and correlated states in magic-angle bilayer graphene. Nature 574, 653–657 (2019).

    Article  CAS  Google Scholar 

  21. Shen, C. et al. Correlated states in twisted double bilayer graphene. Nat. Phys. 16, 520–525 (2020).

    Article  CAS  Google Scholar 

  22. Liu, X. et al. Tunable spin-polarized correlated states in twisted double bilayer graphene. Nature 583, 221–225 (2020).

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  24. He, M. et al. Symmetry breaking in twisted double bilayer graphene. Nat. Phys. 17, 26–30 (2021).

    Article  CAS  Google Scholar 

  25. Burg, G. W. et al. Correlated insulating states in twisted double bilayer graphene. Phys. Rev. Lett. 123, 197702 (2019).

    Article  CAS  Google Scholar 

  26. Liu, L. et al. Isospin competitions and valley polarized correlated insulators in twisted double bilayer graphene. Nat. Commun. 13, 3292 (2022).

    Article  CAS  Google Scholar 

  27. Choi, Y. W. & Choi, H. J. Intrinsic band gap and electrically tunable flat bands in twisted double bilayer graphene. Phys. Rev. B 100, 201402 (2019).

    Article  CAS  Google Scholar 

  28. Cao, Y. et al. Correlated insulator behaviour at half-filling in magic-angle graphene superlattices. Nature 556, 80–84 (2018).

    Article  CAS  Google Scholar 

  29. Sharpe, A. L. et al. Emergent ferromagnetism near three-quarters filling in twisted bilayer graphene. Science 365, 605–608 (2019).

    Article  CAS  Google Scholar 

  30. Kuiri, M. et al. Spontaneous time-reversal symmetry breaking in twisted double bilayer graphene. Nat. Commun. 13, 6468 (2022).

    Article  CAS  Google Scholar 

  31. Koshino, M. Band structure and topological properties of twisted double bilayer graphene. Phys. Rev. B 99, 235406 (2019).

    Article  CAS  Google Scholar 

  32. Zhang, Y.-H., Mao, D., Cao, Y., Jarillo-Herrero, P. & Senthil, T. Nearly flat Chern bands in moiré superlattices. Phys. Rev. B 99, 075127 (2019).

    Article  CAS  Google Scholar 

  33. Samajdar, R. & Scheurer, M. S. Microscopic pairing mechanism, order parameter, and disorder sensitivity in moiré superlattices: applications to twisted double-bilayer graphene. Phys. Rev. B 102, 064501 (2020).

    Article  CAS  Google Scholar 

  34. Hsu, Y.-T., Wu, F. & Sarma, S. D. Topological superconductivity, ferromagnetism, and valley-polarized phases in moiré systems: renormalization group analysis for twisted double bilayer graphene. Phys. Rev. B 102, 085103 (2020).

    Article  CAS  Google Scholar 

  35. Lin, J.-X. et al. Spin–orbit-driven ferromagnetism at half moiré filling in magic-angle twisted bilayer graphene. Science 375, 437–441 (2022).

    Article  CAS  Google Scholar 

  36. Maharaj, A. V., Esterlis, I., Zhang, Y., Ramshaw, B. J. & Kivelson, S. A. Hall number across a van Hove singularity. Phys. Rev. B 96, 045132 (2017).

    Article  Google Scholar 

  37. Tinkham, M. Introduction to Superconductivity (Courier Corporation, 2004).

  38. Clogston, A. M. Upper limit for the critical field in hard superconductors. Phys. Rev. Lett. 9, 266–267 (1962).

    Article  Google Scholar 

  39. Cao, Y., Park, J. M., Watanabe, K., Taniguchi, T. & Jarillo-Herrero, P. Pauli-limit violation and re-entrant superconductivity in moiré graphene. Nature 595, 526–531 (2021).

    Article  CAS  Google Scholar 

  40. Huang, C., Wei, N., Qin, W. & MacDonald, A. H. Pseudospin paramagnons and the superconducting dome in magic angle twisted bilayer graphene. Phys. Rev. Lett. 129, 187001 (2022).

    Article  CAS  Google Scholar 

  41. Chou, Y.-Z., Wu, F. & Sarma, S. D. Enhanced superconductivity through virtual tunneling in Bernal bilayer graphene coupled to WSe2. Phys. Rev. B 106, L180502 (2022).

    Article  CAS  Google Scholar 

  42. Wang, Z. et al. Origin and magnitude of ‘designer’ spin–orbit interaction in graphene on semiconducting transition metal dichalcogenides. Phys. Rev. X 6, 041020 (2016).

    Google Scholar 

  43. Klemm, R. A., Luther, A. & Beasley, M. Theory of the upper critical field in layered superconductors. Phys. Rev. B 12, 877 (1975).

    Article  Google Scholar 

  44. Lake, E., Patri, A. S. & Senthil, T. Pairing symmetry of twisted bilayer graphene: a phenomenological synthesis. Phys. Rev. B 106, 104506 (2022).

    Article  CAS  Google Scholar 

  45. Kim, K. et al. van der Waals heterostructures with high accuracy rotational alignment. Nano Lett. 16, 1989–1995 (2016).

    Article  CAS  Google Scholar 

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Acknowledgements

We thank A. MacDonald, J. Zhu, N. Wei, S. D. Sarma, Y.-Z. Chou, A. Potter and M. Franz for fruitful discussions. M.K. acknowledges a postdoctoral research fellowship from the Stewart Blusson Quantum Matter Institute (SBQMI). Experiments at the University of British Columbia were undertaken with support from SBQMI, the Natural Sciences and Engineering Research Council of Canada, the Canada Foundation for Innovation, the Canadian Institute for Advanced Research and the Canada First Research Excellence Fund, Quantum Materials and Future Technologies Program (J.F.). Growing the hBN crystals received support from the Japan Society for the Promotion of Science (KAKENHI grant nos. 19H05790, 20H00354 and 21H05233) to K.W. and T.T.

Author information

Authors and Affiliations

  1. Stewart Blusson Quantum Matter Institute, University of British Columbia, Vancouver, British Columbia, Canada

    Ruiheng Su, Manabendra Kuiri & Joshua Folk

  2. Department of Physics and Astronomy, University of British Columbia, Vancouver, British Columbia, Canada

    Ruiheng Su, Manabendra Kuiri & Joshua Folk

  3. Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

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

    Takashi Taniguchi

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  1. Ruiheng Su
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  2. Manabendra Kuiri
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Contributions

R.S. fabricated the devices, with help from M.K. R.S. performed the measurements. R.S., M.K. and J.F. interpreted the data and wrote the paper. J.F. supervised the experiment. K.W. and T.T. provided the hBN crystals.

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Correspondence to Joshua Folk.

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Nature Materials thanks Guangyu Zhang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Sections A–L, each containing a multi-panel figure and discussion in the figure caption.

Source data

Source Data Fig. 1

Experimental data for Fig. 1.

Source Data Fig. 2

Experimental data for Fig. 2.

Source Data Fig. 3

Experimental data for Fig. 3.

Source Data Fig. 4

Experimental data for Fig. 4.

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Su, R., Kuiri, M., Watanabe, K. et al. Superconductivity in twisted double bilayer graphene stabilized by WSe2. Nat. Mater. 22, 1332–1337 (2023). https://doi.org/10.1038/s41563-023-01653-7

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