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Atomic manipulation of the emergent quasi-2D superconductivity and pair density wave in a kagome metal

Nature Nanotechnology volume 20, pages 1017–1025 (2025) Cite this article

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Abstract

The unconventional charge density wave (CDW) order in layered kagome lattice superconductors AV3Sb5 (A = K, Cs or Rb) triggers the emergence of novel quantum states such as time-reversal symmetry breaking and electronic liquid crystal states. However, atomic-scale manipulation and control of such phases remains elusive. Here we observe the emergent superconductivity and a primary pair density wave at the 2 × 2 Cs reconstructed surface of CsV3Sb5 by means of low-temperature scanning tunnelling microscopy/spectroscopy paired with density functional theory calculations. This quasi-two-dimensional kagome superconducting state with a critical temperature of ~5.4 K is intertwined with the bulk CDW order and exhibits a unique vortex core spectrum and a 4 × 4 pair density wave modulation of the superconducting gap. The emergent phenomena happen at a π-phase-shift dislocation in the periodicity of the CDW along the stacking direction if the 2 × 2 Cs superstructures are out of phase with the bulk CDW. Furthermore, we switched on and off the quasi-two-dimensional superconductivity through tip-assisted atomic manipulation of the 2 × 2 Cs superstructure. Thus, control of the surface reconstruction permits the creation, manipulation and control of quantum many-body states at antiphase boundaries in kagome lattice superconductors and, potentially, in other correlated materials.

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Fig. 1: Emergent low-energy gap and incipient surface band inside the bulk CDW gap on the 2 × 2 Cs ordered surface of CsV3Sb5.
The alternative text for this image may have been generated using AI.
Fig. 2: Superconductivity origin of Δ2D at the 2 × 2 Cs ordered surface of CsV3Sb5.
The alternative text for this image may have been generated using AI.
Fig. 3: Observation of the 4 × 4 PDW modulation of Δ2D at the 2 × 2 Cs ordered surface of CsV3Sb5.
The alternative text for this image may have been generated using AI.
Fig. 4: Atomic manipulation of quasi-2D superconducting states through artificial control of the size of 2 × 2 Cs ordered region.
The alternative text for this image may have been generated using AI.
Fig. 5: Atomic manipulation of the quasi-2D superconducting state through artificial control the phase twist of bulk CDW.
The alternative text for this image may have been generated using AI.

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Data availability

The data that support the plots within this paper are available via Figshare at https://doi.org/10.6084/m9.figshare.28723703 (ref. 53). Other data and information are available from the corresponding authors upon reasonable request.

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Acknowledgements

The work is supported by grants from the National Natural Science Foundation of China (grant no. 62488201), the National Key Research and Development Projects of China (grant nos. 2022YFA1204100 and 2019YFA0308500), the CAS Project for Young Scientists in Basic Research (grant no. YSBR-003) and the Innovation Program of Quantum Science and Technology (grant no. 2021ZD0302700). B.Y. acknowledges the financial support by the Israel Science Foundation (grant nos. 2932/21 and 2974/23), German Research Foundation (DFG, CRC-183, A02) and by a research grant from the Estate of Gerald Alexander. Z.W. is supported by the US DOE, Basic Energy Sciences (grant no. DE-FG02-99ER45747) and by Research Corporation for Science Advancement (Cottrell SEED award no. 27856).

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  1. These authors contributed equally: Xianghe Han, Hui Chen.

Authors and Affiliations

  1. Beijing National Center for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, People’s Republic of China

    Xianghe Han, Hui Chen, Zhongyi Cao, Zihao Huang, Yuhan Ye, Zhen Zhao, Chengmin Shen, Haitao Yang & Hong-Jun Gao

  2. School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, People’s Republic of China

    Xianghe Han, Hui Chen, Zhongyi Cao, Zihao Huang, Yuhan Ye, Zhen Zhao, Chengmin Shen, Haitao Yang & Hong-Jun Gao

  3. Department of Condensed Matter Physics, Weizmann Institute of Science, Rehovot, Israel

    Hengxin Tan & Binghai Yan

  4. Department of Physics, Boston College, Chestnut Hill, MA, USA

    Ziqiang Wang

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Contributions

H.-J.G. and H.C. designed the experiments. X.H., H.C., Z.C., Z.H. and Y.Y. performed the STM/STS experiments and data analysis with technical assistance from C.S. Z.Z. and H.Y. prepared the CsV3Sb5 samples. H.T. and B.Y. did the DFT calculations. Z.W. did the theoretical consideration. X.H., H.C., Z.W. and H.-J.G. wrote the manuscript with input from all other authors. H.-J.G. supervised the project.

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Correspondence to Hui Chen, Ziqiang Wang or Hong-Jun Gao.

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Extended data

Extended Data Fig. 1 Statistical analysis and real-space distribution of emergent energy gap Δ2D on the 2×2 ordered Cs surfaces.

a, Histograms of Δbulk and Δ2D, fitted by normal distributions, showing the averag values of Δ2D = 1.70 meV, Δbulk = 0.56 meV. b-e, STM topography of a boundary region consisting of both 2×2 and √3×√3R30°reconstructions (b) and three dI/dV maps at 2 mV (c), 5 mV (d), and 0 mV (e), showing that the electronic states with Δ2D and P2D only distribute on 2×2 ordered regions. Yellow dashed curves represent the boundary of the two regions. For all dI/dV data, Vset = 100 mV, It = 3 nA, Vmod = 0.1 mV.

Extended Data Fig. 2 Calculated stacking fault of CDW phases in CsV3Sb5 crystal with 2×2 Cs ordered surfaces before and after relaxation.

Calculated stacking fault of CDW phases in CsV3Sb5 crystal with 2×2 Cs ordered surfaces before (a) and after (b) surface relaxation, showing that the inverse star of David pattern of 2×2 CDW in the top kagome layer will shift, following the 2×2 Cs atom sites while the inverse star of David pattern of 2×2 CDW in the second kagome layer remains unchanged.

Extended Data Fig. 3 Localized nature of P2D.

a, STM topography of a typical 2×2 Cs reconstruction. b, Waterfall (left) and intensity plot (right) of a dI/dV linecut along the dots and red arrow in (a), showing that the resonance peak P2D is localized at each Cs atom of 2×2 Cs ordered surfaces. Vset = 100 mV, It = 1 nA, Vmod = 0.5 mV. c, The dI/dV spectra obtained on (red) and off (yellow) a vacancy in the 2×2 Cs triangle (inset STM topography), respectively, showing that P2D is significantly suppressed at the vacancy site while the Δ2D show little changes. Vset = 50 mV, It = 1.5 nA, Vmod = 0.15 mV.

Extended Data Fig. 4 Absence of quasi-2D superconductivity at the 2×2 ordered Cs surface in CsV2.85Ti0.15Sb5.

a, Spatially-averaged dI/dV spectra over the 2×2, √3×√3R30° ordered Cs and Sb surface regions, respectively, showing that only the bulk superconducting gap is observed on all surfaces. There is no additional energy gap at low energies for the 2×2 ordered Cs surface. b, STM topography, dI/dV (r, -2 mV) and dI/dV (r, 5 mV) of a boundary region between 2×2 and √3×√3R30° Cs ordered surfaces, showing there is no differnece in density of states between two surfaces (Vset = 100 mV, It = 3 nA, Vmod = 0.1 mV).

Extended Data Fig. 5 Emergent low-energy gap and incipient bound state on the 2×2 alkali ordered surface of AV3Sb5 (A = Rb, K).

a, The STM topography showing the 2×2 Rb ordered surface region of RbV3Sb5. Vset = 900 mV, It = 50 pA. b, Spatially-averaged dI/dV spectra obtained at the 2×2 Rb ordered surface region of RbV3Sb5, showing the emergence of a new quasi-2D superconducting gap Δ2D with a size of ~1.4 meV and a pronounce peak at -2.8 mV (P2D). c, The STM topography showing the 2×2 K ordered surface region of KV3Sb5. Vset = 900 mV, It = 50 pA. d, Spatially-averaged dI/dV spectra obtained at the 2×2 K ordered surface region of KV3Sb5, showing the emergence of a new quasi-2D superconducting gap Δ2D with a size of ~0.8 meV and a pronounced peak at -4.7 mV (P2D). The spectrum is normalized with respect to the average value. For all dI/dV data, Vset = 100 mV, It = 3 nA, Vmod = 0.1 mV.

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Video showing the process of assembling Cs reconstructed nanoislands.

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Han, X., Chen, H., Tan, H. et al. Atomic manipulation of the emergent quasi-2D superconductivity and pair density wave in a kagome metal. Nat. Nanotechnol. 20, 1017–1025 (2025). https://doi.org/10.1038/s41565-025-01940-1

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