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Charge order landscape and competition with superconductivity in kagome metals

Nature Materials volume 22, pages 186–193 (2023)Cite this article

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Abstract

In the kagome metals AV3Sb5 (A = K, Rb, Cs), three-dimensional charge order is the primary instability that sets the stage for other collective orders to emerge, including unidirectional stripe order, orbital flux order, electronic nematicity and superconductivity. Here, we use high-resolution angle-resolved photoemission spectroscopy to determine the microscopic structure of three-dimensional charge order in AV3Sb5 and its interplay with superconductivity. Our approach is based on identifying an unusual splitting of kagome bands induced by three-dimensional charge order, which provides a sensitive way to refine the spatial charge patterns in neighbouring kagome planes. We found a marked dependence of the three-dimensional charge order structure on composition and doping. The observed difference between CsV3Sb5 and the other compounds potentially underpins the double-dome superconductivity in CsV3(Sb,Sn)5 and the suppression of Tc in KV3Sb5 and RbV3Sb5. Our results provide fresh insights into the rich phase diagram of AV3Sb5.

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Fig. 1: Possible microscopic structures of the 3D CO in kagome metal AV3Sb5.
Fig. 2: Two distinct types of electronic reconstruction in CsV3Sb5 induced by 3D CO.
Fig. 3: Theoretical calculation of electronic reconstruction in AV3Sb5 and its dependence on the microscopic structure of 3D CO.
Fig. 4: Electronic reconstructions in KV3Sb5, RbV3Sb5 and Sn-doped CsV3Sb5 in the 3D-CO state.
Fig. 5: Phase diagram of the 3D CO in CsV3Sb5–xSnx and its correlation with double-dome superconductivity.

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Data associated with this paper are available on the Harvard Dataverse at https://doi.org/10.7910/DVN/KJRGXU.

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Acknowledgements

This work was supported by the Air Force Office of Scientific Research Young Investigator Program under grant FA9550-19-1-0063, and by the STC Center for Integrated Quantum Materials (National Science Foundation grant no. DMR-1231319). The work is funded in part by the Gordon and Betty Moore Foundation’s EPiQS Initiative, grant GBMF9070 to J.G.C. The work at Max Planck POSTECH/Korea Research Initiative was supported by the National Research Foundation of Korea funded by the Ministry of Science and ICT, grant nos 2022M3H4A1A04074153 and 2020M3H4A2084417. B.R.O. and S.D.W. were supported by the National Science Foundation through the programme Enabling Quantum Leap: Convergent Accelerated Discovery Foundries for Quantum Materials Science, Engineering and Information (Q-AMASE-i) and the Quantum Foundry at University of California Santa Barbara (DMR-1906325). This research used resources of the Advanced Light Source, a US Department of Energy Office of Science User Facility under contract no. DE-AC02-05CH11231. M.K. acknowledges a Samsung Scholarship from the Samsung Foundation of Culture. B.R.O. acknowledges support from the California NanoSystems Institute through the Elings Fellowship programme.

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Author notes

  1. These authors contributed equally: Mingu Kang, Shiang Fang, Jonggyu Yoo.

Authors and Affiliations

  1. Center for Complex Phase of Materials, Max Planck POSTECH/Korea Research Initiative, Pohang, Republic of Korea

    Mingu Kang, Jonggyu Yoo, Jonghyeok Choi & Jae-Hoon Park

  2. Department of Physics, Massachusetts Institute of Technology, Cambridge, MA, USA

    Mingu Kang, Shiang Fang, Joseph G. Checkelsky & Riccardo Comin

  3. Department of Physics, Pohang University of Science and Technology, Pohang, Republic of Korea

    Jonggyu Yoo, Jonghyeok Choi & Jae-Hoon Park

  4. Materials Department, University of California Santa Barbara, Santa Barbara, CA, USA

    Brenden R. Ortiz, Yuzki M. Oey & Stephen D. Wilson

  5. Advanced Light Source, E. O. Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Sae Hee Ryu, Chris Jozwiak, Aaron Bostwick & Eli Rotenberg

  6. Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science (IBS), Pohang, Republic of Korea

    Jimin Kim

  7. Department of Physics, Harvard University, Cambridge, MA, USA

    Efthimios Kaxiras

  8. John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA

    Efthimios Kaxiras

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Contributions

M.K., J.-H.P. and R.C. conceived the project; M.K. and J.Y. performed the ARPES experiments and analysed the resulting data with help from S.H.R., J.K., C.J., A.B. and E.R.; S.F. performed the theoretical calculations with help from E.K. and J.C.; and B.R.O., Y.M.O. and S.D.W. synthesized and characterized the crystals. M.K. and R.C. wrote the manuscript with input from all coauthors.

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Correspondence to Mingu Kang, Jae-Hoon Park or Riccardo Comin.

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Extended data

Extended Data Fig. 1 Fermi surface and overall electronic structure of pristine and Sn-doped AV3Sb5 (A=K, Rb, Cs).

a-d, Fermi surfaces of KV3Sb5, RbV3Sb5, CsV3Sb5 and Sn-doped CsV3Sb5, respectively. e-h, Wide energy-momentum range ARPES spectra of KV3Sb5, RbV3Sb5, CsV3Sb5 and Sn-doped CsV3Sb5, respectively. All data are acquired at the base temperature 6 K, that is in the charge ordered state.

Extended Data Fig. 2 kz dispersion of (K,Rb,Cs)V3Sb5.

a-c, kx-kz map of KV3Sb5, RbV3Sb5, and CsV3Sb5 respectively, acquired at 0.5 eV binding energy. d-f, Corresponding kz-E map acquired at kx=0. The pronounced kz dispersion of the G band is clearly visible in panels d-f from which we determined the inner potential for each sample, 5.4, 4.3, and 7.3 eV, respectively.

Extended Data Fig. 3 Momentum- and energy-distribution-curves highlighting the band splitting in 3D-CO phase.

a-c, Momentum-distribution-curves (MDCs) across the lower K1 Dirac band above (140 K, panel b) and below (6 K, panel c) the 3D-CO transition. The dashed line in panel a marks the region where the MDCs are extracted. The doubling of the lower K1-Dirac band is observed only in the case of CsV3Sb5. d-f, Energy-distribution-curves (EDCs) across the K1 vHs above (140 K, panel e) and below (6 K, panel f) the 3D-CO transition. The dashed line in panel d marks the region where the EDCs are extracted. The doubling of the K1 vHs is universally observed at the low temperature as marked with the arrows in panel f.

Extended Data Fig. 4 Domain-resolved electronic structures of CsV3Sb5 in C2 symmetric 3D-CO phases.

a-c, Domain-resolved dispersion of CsV3Sb5 in the inverse MLL 3D-CO phase. The location of three different k-paths with respect to the C2 rotation axis is schematically displayed above each panel. d-f, Same with a-c but in the MLL phase. Corresponding domain-averaged electronic structures are shown in Fig. 3d, e.

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Supplementary Figs. 1 and 2, Table 1, Discussion and references.

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Kang, M., Fang, S., Yoo, J. et al. Charge order landscape and competition with superconductivity in kagome metals. Nat. Mater. 22, 186–193 (2023). https://doi.org/10.1038/s41563-022-01375-2

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