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A chiral superlattice route to spin-split topological antiferromagnetism

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Acknowledgements

We thank S.-W. Cheong, A. Devarakonda, R. M. Fernandez, T. Kurumaji, I. Mazin, N. Nagaosa and L. Ye for the discussions.

Funding

T.D., J.-X.Q., M.S., J.M.B., R.M., Q.M., J. Shi, I.M., A.V. and S.-Y.X. were supported through the Center for the Advancement of Topological Semimetals (CATS), an Energy Frontier Research Center (EFRC) funded by the US Department of Energy (DOE) Office of Science, through the Ames National Laboratory under contract DE-AC0207CH11358. The work in SYX group was supported by the Office of Naval Research (ONR) grant no. N000142512285 (charge and spin transport), the National Science Foundation (NSF) career grant no. DMR-2143177 (fabrication), CATS (data analysis) and the Army Research Office (ARO) under W911NF2420195 Cooperative Agreement no. W911NF-24-2-0195 (manuscript writing). S.-Y.X. acknowledges the Alfred P. Sloan Foundation, the Camille and Henry Dreyfus Foundation, and Corning Fund for Faculty Development. P.K. acknowledges support from AFOSR grant no. FA9550-25-1-0019. T.D. acknowledges a partial support from AFOSR MURI grant no. FA9550-25-1-0262 (fabrication in the Kim group). Q.M. acknowledges support from the National Science Foundation (NSF) under award no. DMREF-2522383. H.P. and M.D.L. were supported by the GBMF grant no. 7797-01 and NSF CUA (PHY-1125846 for H.P. and M.D.L.). H.P., M.D.L., P.K. and S.-Y.X. are supported by the Samsung Electronics award no. A61703. TSG was supported by the Dutch Research Council (NWO) through a Rubicon grant (no. 019.222EN.013) and a Veni grant (no. VI.Veni.242.281). M.L. acknowledges the Harvard Quantum Initiative Postdoctoral Fellowship and the start-up funds at University of Texas at Dallas. J.E.H. was supported by the EPiQS Initiative of the Gordon and Betty Moore Foundation (GBMF) through grant GBMF10215. I.E.B. and S.H.S. acknowledge support by the Rowland Institute at Harvard. Research at Washington University was supported by the US DOE, Office of Science, Basic Energy Sciences grant no. DE-SC0026267 (sample synthesis) and the National Science Foundation (NSF) Division of Materials Research Award DMR-2236528 (high magnetic field measurement). Electron microscopy experiments were performed at the Michigan Center for Materials Characterization ((MC)2, RRID: SCR_026770) and MIT.nano. Focused ion beam samples were prepared at (MC)2 as well as at the Harvard University Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF award no. ECCS-2025158. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation Cooperative Agreement no. DMR-2128556, the US DOE and the State of Florida. K.W. and T.T. were supported by the JSPS KAKENHI (21H05233 and 23H02052), the CREST (JPMJCR24A5), JST and World Premier International Research Center Initiative (WPI), MEXT, Japan. C.F. was supported by Deutsche Forschungsgemeinschaft through SFB 1143 (project ID 24731007) and the Würzburg-Dresden Cluster of Excellence ctd.qmat—Complexity, Topology and Dynamics in Quantum Matter (EXC 2147, project ID 390858490). H. Lin was supported by the National Science and Technology Council (NSTC) in Taiwan under grant no. NSTC 114-2112-M-001-055-MY3. T.R.C. was supported by the National Science and Technology Council (NSTC) in Taiwan (NSTC 114-2628-M-006-005-MY3 and NSTC113-2124-M-006-009-MY3), the National Cheng Kung University (NCKU), Taiwan, and the National Center for Theoretical Sciences, Taiwan. This research was supported, in part, by the Higher Education Sprout Project, Ministry of Education to the Headquarters of University Advancement at NCKU. T.-R.C. thanks the National Center for High performance Computing (NCHC) of the National Applied Research Laboratories in Taiwan for computational and storage resources. The work at the S. N. Bose National Centre for Basic Sciences (SNBNCBS) was supported by the Prime Minister Early Career Research Grant (PM-ECRG) from the Anusandhan National Research Foundation (ANRF), file number ANRF/ECRG/2024/003677/PMS, and also benefited from the PARAM-Rudra computational facility at SNBNCBS. The work at Northeastern University was supported by the National Science Foundation through the Expand-QISE award NSF-OMA-2329067 and benefited from the resources of the Advanced Scientific Computation Center of the Northeastern University, the Explorer Cluster, the Massachusetts Technology Collaborative award MTC-22032 and the Quantum Materials and Sensing Institute (QMSI). J. Sinova was supported by the US DOE, Office of Science, under award no. DE-SC0026038. We acknowledge the support to the X-ray core facility from the Major Research Instrumentation Program of the NSF under award no. 2216066. K.S. was supported by the GBMF10694.

Author information

Author notes

  1. These authors contributed equally: Thao Dinh, Mengke Liu

Authors and Affiliations

  1. Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA

    Thao Dinh, Jian-Xiang Qiu, Xuan Hoang Le, Chengfeng Zhu, Yu-Fei Liu, Xiaoyu Zeng, Houchen Li, Peng Guo, Jinchen Liu, Tianye Huang, Iván E. Arvizo, Dongtao Cui, Shao-Liang Zheng, Anyuan Gao, Hongkun Park & Su-Yang Xu

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

    Thao Dinh, Mengke Liu, Xuan Hoang Le, Yu-Fei Liu, Ashvin Vishwanath, Mikhail D. Lukin, Jennifer E. Hoffman, Talieh S. Ghiasi, Hongkun Park & Philip Kim

  3. Department of Physics, University of Texas at Dallas, Richardson, TX, USA

    Mengke Liu

  4. Department of Physics and Astronomy, Howard University, Washington, DC, USA

    Sougata Mardanya, Vineet Kumar Sharma & Sugata Chowdhury

  5. The Rowland Institute at Harvard, Harvard University, Cambridge, MA, USA

    Suk Hyun Sung & Ismail El Baggari

  6. Michigan Center for Materials Characterization, University of Michigan, Ann Arbor, MI, USA

    Suk Hyun Sung

  7. Department of Physics, Washington University in St. Louis, St. Louis, MO, USA

    Christopher Broyles, Qiaozhi Xu, Haotian Chen, Zack Rehfuss & Sheng Ran

  8. Materials Science Division, Argonne National Laboratory, Lemont, IL, USA

    Jingtian Shi, Michael Smith & Ivar Martin

  9. National High Magnetic Field Laboratory, Los Alamos National Laboratory, Los Alamos, NM, USA

    Joanna M. Blawat, John Singleton & Ross McDonald

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

    Kenji Watanabe

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

    Takashi Taniguchi

  12. S. N. Bose National Centre for Basic Sciences, Kolkata, India

    Sudip Ghorai & Barun Ghosh

  13. Institute of Physics, Academia Sinica, Taipei, Taiwan

    Hsin Lin

  14. Department of Physics, National Cheng Kung University, Tainan, Taiwan

    Ting Yong Lim & Tay-Rong Chang

  15. Department of Physics, Northeastern University, Boston, MA, USA

    Arun Bansil

  16. Quantum Materials and Sensing Institute, Northeastern University, Burlington, MA, USA

    Arun Bansil

  17. Department of Chemistry, Michigan State University, Michigan, MI, USA

    Weiwei Xie

  18. Max Planck Institute for Chemical Physics of Solids, Dresden, Germany

    Claudia Felser

  19. Institut für Physik, Johannes Gutenberg University, Mainz, Germany

    Jairo Sinova

  20. Department of Physics, Texas A&M University, College Station, TX, USA

    Jairo Sinova

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

    Qiong Ma

  22. Department of Physics, University of Michigan Ann Arbor, Ann Arbor, MI, USA

    Kai Sun

  23. Kavli Institute of Nanoscience, Delft University of Technology, Delft, The Netherlands

    Talieh S. Ghiasi

Authors

  1. Thao Dinh
  2. Mengke Liu
  3. Jian-Xiang Qiu
  4. Sougata Mardanya
  5. Suk Hyun Sung
  6. Xuan Hoang Le
  7. Christopher Broyles
  8. Chengfeng Zhu
  9. Qiaozhi Xu
  10. Haotian Chen
  11. Zack Rehfuss
  12. Yu-Fei Liu
  13. Xiaoyu Zeng
  14. Houchen Li
  15. Peng Guo
  16. Jinchen Liu
  17. Tianye Huang
  18. Jingtian Shi
  19. Michael Smith
  20. Joanna M. Blawat
  21. John Singleton
  22. Ross McDonald
  23. Iván E. Arvizo
  24. Dongtao Cui
  25. Shao-Liang Zheng
  26. Kenji Watanabe
  27. Takashi Taniguchi
  28. Vineet Kumar Sharma
  29. Sudip Ghorai
  30. Barun Ghosh
  31. Hsin Lin
  32. Ting Yong Lim
  33. Tay-Rong Chang
  34. Arun Bansil
  35. Ivar Martin
  36. Ashvin Vishwanath
  37. Weiwei Xie
  38. Claudia Felser
  39. Jairo Sinova
  40. Anyuan Gao
  41. Mikhail D. Lukin
  42. Jennifer E. Hoffman
  43. Sugata Chowdhury
  44. Qiong Ma
  45. Kai Sun
  46. Ismail El Baggari
  47. Sheng Ran
  48. Talieh S. Ghiasi
  49. Hongkun Park
  50. Philip Kim
  51. Su-Yang Xu

Contributions

T.D. fabricated the devices. S.H.S. performed the TEM measurements with help from M.L., T.D. and I.E.B., inspired by early STM measurements of M.L. and J.E.H.; J.-X.Q. initiated the optical measurements and performed optical linear and circular dichroism experiments with help from T.D. and X.Z.; T.D. performed the charge transport measurements with help from C.Z., M.L., Y.-F.L. and A.G.; T.S.G. conceived and designed the spin-transport and Hanle experiments, and supervised the measurements performed by T.D.; X.H.L. performed the nitrogen-vacancy centre magnetometry measurements with the help from T.D., M.D.L., H.P.; J.M.B., J. Singleton and R.M. performed the high-field magnetization measurements at LANL with the help from T.D.; I.E.A. performed the MPMS measurements with help from T.D. and D.C.; S.-L.Z. performed the single-crystal X-ray diffraction measurements with help from T.D.; C.B., Q.X., Z.R., H.C., W.X. and S.R. grew the UOTe single crystals. K.W. and T.T. grew the bulk hBN single crystals. S.M. performed first-principles calculations with help from B.G., V.K.S., S.G., H. Lin, T.-R.C., T.Y.L., A.B. and S.C.; K.S. performed effective modelling with help from J. Sinova and A.V.; M.S., J. Shi and I.M. proposed the free-energy model for the chiral superlattice. H. Li, P.G., J.L., T.H., C.F. and Q.M. helped with the charge transport experiments. T.D., M.L., J.-X.Q., P.K. and S.-Y.X. wrote the manuscript with contributions from others. S.-Y.X., P.K., and M.L. conceived the experiments. S.-Y.X. and P.K. supervised the project.

Corresponding authors

Correspondence to Mengke Liu, Jian-Xiang Qiu, Philip Kim or Su-Yang Xu.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature thanks Wei Jiang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Peer reviewer reports are available.

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Extended data figures and tables

Extended Data Fig. 1 Additional TEM at 300 K and 100 K in UOTe.

a-c, Additional TEM data at 300 K. a, Cross-sectional STEM image of UOTe showing a monoclinic distortion. The red line connecting U atoms across layers deviates from the vertical yellow reference line, visualizing the cumulative shear associated with the monoclinic distortion. Inset: Electron diffraction pattern acquired from the same cross-sectional region, revealing a monoclinic distortion angle of α ~ 1.23°. b, Fitted displacement parameters of U atoms across 15 UOTe layers. See Methods.3 for the expressions for fitting the TEM data. The in-plane displacements of different layers have different lineshapes (for example, one can compare the highlighted red boxes). Therefore \(t{\mathcal{T}}\) symmetry is also broken. c, Fitted values for each layer. d-f, Same as panels a-c but for TEM data at 100 K.

Source data

Extended Data Fig. 2 DFT-calculated phonon band structure and displacement of UOTe without superlattice.

a, DFT-calculated phonon band structure of UOTe. One branch of phonon has negative frequency at \({\bf{q}}=\left(\frac{1}{6.7}\frac{2{\rm{\pi }}}{a},0,\frac{1}{2}\frac{2{\rm{\pi }}}{c}\right)\), consistent with the experimentally observed q for the superlattice. b, Atomic displacements corresponding to that unstable phonon at the negative frequency. U1 and U2 (also Te1 and Te2) have opposite chiral winding structures, consistent with the experimental findings.

Source data

Extended Data Fig. 3 Theoretical tight-binding modeling of the chiral superlattice quantum geometry.

a, Chiral superlattice band structure. b, Berry curvature k-space distribution of the low-energy superlattice band. c, Calculated Berry curvature dipole. d, Schematic of the chiral superlattice containing the z + ix U1 and z − ix U2 chiral displacements. e, Spatially-resolved Berry curvature at different x values in the superlattice, calculated by treating the slowly varying superlattice modulation as an adiabatic parameter and approximating each local region by a homogeneous tight-binding Hamiltonian H(k; x). f-j, The same as panels (a-e) but for chiral superlattice plus the AFM order. Panel h shows the calculated AHE angle.

Source data

Extended Data Fig. 4 Excluding weak ferromagnetism and the regular Hall effect as the main contribution of the AHE.

a, Temperature dependence of in-plane and out-of-plane magnetic susceptibilities (χ// and χ⊥). b, AHE and magnetization (measured by magnetic circular dichroism). The magnetic circular dichroism is the antisymmetric part of the optical circular dichroism, which naturally excludes the chiral circular dichroism (see details in SI.III.3). The net magnetization under finite magnetic field is given by M = Ms + χ⊥B. Ms is the spontaneous magnetization which was measured by the NV center magnetometry to be ~ 10 mμB per U ion. Due to the small Ms and large coercive field, large AHE is observed at zero magnetization, therefore demonstrating that the small net magnetization is a side product of the symmetry breaking. c, AHE as a function of the magnetization using the data in panel (b) for 129 K. d, We can further discern the different contributions to the Hall effect including the regular Hall effect, the weak ferromagnetism and the intrinsic AFM, i.e., RAHE = R0B + RsMs + RAFM. R0 and Rs are slopes of the AHE vs. B field and AHE vs. magnetization curves. The different contributions at 129 K are shown here. The intrinsic AFM contribution strongly dominates.

Source data

Extended Data Fig. 5 Superlattice formation mechanism 1 - A comparison between UOS and UOTe.

These two compounds are isostructural, but UOS has no supermodulation. A comparison of the nominal crystal structure shows that UOS has an additional interlayer bond connecting the U with the S in the next layer. This is enabled by the large S-U-S angle (82°), which resembles opening arms. Such an interlayer bond lowers energy. Forming similar interlayer bonding in UOTe is too energetically costly as the much longer U-Te bond length would laterally stretch the U-O-U central block at a similarly large bond angle. As a result, in the nominal unit cell of UOTe, the Te-U-Te bond angle is much smaller (77°), protecting the U-O-U central block from being stretched but in turn hindering the interlayer bonding.

Extended Data Fig. 6 Superlattice formation mechanism 2 - Supermodulation as an intermediate phase.

a, To form the interlayer bonding while keeping the central block unstretched, the layers decide to locally curve up/down with opposite signs in adjacent layers, which is the supermodulation. In this way, at specific locations, the Te-U-Te angle opens up (81°), allowing the interlayer bonding. At some other locations, the Te-U-Te angle decreases (73°), leading to an intralayer repulsion. The competition between the interlayer bonding and intralayer repulsion gives rise to the supermodulation in UOTe. b, More generally, we can consider three distinct phases: (1) 3D covalent, (2) 2D vdW, (3) supermodulation as an intermediate phase. The phase diagram is described by a Ginzburg-Landau theory (see main text). c, DFT-calculated phonon dispersions of UOS, UOTe and UOTe with artificially increased vdW gap.

Source data

Extended Data Fig. 7 Bond-mismatch superlattice and lattice-mismatch superlattice.

UOTe is a bond-mismatch superlattice, in which the superlattice strongly modifies the local U-O and U-Te bonding environment itself. This provides a real-space handle on the orbital composition and hopping amplitudes, which in turn produces spatially modulated Berry curvature, Berry-curvature dipole, and related quantum-geometric responses (see SI.II.5).

Extended Data Fig. 8 Proposed design principle for chiral supermodulation.

Based on the above mechanism and phenomenological theory, we propose a design principle that goes from chemistry to physics to materials. a, From chemistry, we can tune the size of the ions and the strength of chemical bonds. b, To physics, the above chemical tuning of ion size and bond strength effectively controls the interlayer bonding and intralayer repulsion energies. c, To materials, there are around 500 compounds isostructural to UOTe in the ICSD database. We have developed an empirical rule based on material parameters such as the ion size, the C-A-C bond angle, and the ratios of bond lengths including \({r}_{1}=\frac{{\rm{I}}{\rm{n}}{\rm{t}}{\rm{e}}{\rm{r}}{\rm{l}}{\rm{a}}{\rm{y}}{\rm{e}}{\rm{r}}\,{\rm{A}}-{\rm{C}}\,{\rm{b}}{\rm{o}}{\rm{n}}{\rm{d}}\,{\rm{l}}{\rm{e}}{\rm{n}}{\rm{g}}{\rm{t}}{\rm{h}}}{{\rm{I}}{\rm{n}}{\rm{t}}{\rm{r}}{\rm{a}}{\rm{l}}{\rm{a}}{\rm{y}}{\rm{e}}{\rm{r}}\,{\rm{A}}-{\rm{C}}\,{\rm{b}}{\rm{o}}{\rm{n}}{\rm{d}}\,{\rm{l}}{\rm{e}}{\rm{n}}{\rm{g}}{\rm{t}}{\rm{h}}}\) and \({r}_{2}=\frac{{\rm{I}}{\rm{n}}{\rm{t}}{\rm{r}}{\rm{a}}{\rm{l}}{\rm{a}}{\rm{y}}{\rm{e}}{\rm{r}}\,{\rm{A}}-{\rm{C}}\,{\rm{b}}{\rm{o}}{\rm{n}}{\rm{d}}\,{\rm{l}}{\rm{e}}{\rm{n}}{\rm{g}}{\rm{t}}{\rm{h}}}{{\rm{I}}{\rm{n}}{\rm{t}}{\rm{r}}{\rm{a}}{\rm{l}}{\rm{a}}{\rm{y}}{\rm{e}}{\rm{r}}\,{\rm{A}}-{\rm{B}}\,{\rm{b}}{\rm{o}}{\rm{n}}{\rm{d}}\,{\rm{l}}{\rm{e}}{\rm{n}}{\rm{g}}{\rm{t}}{\rm{h}}}\). d, Based on empirical rules, we can sift through the material database to identify the most promising materials (see SI.II.4).

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Extended Data Table 1 TEM displacement fitting values at 300 K

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Extended Data Table 2 TEM displacement fitting values at 100 K

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Supplementary information

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Dinh, T., Liu, M., Qiu, JX. et al. A chiral superlattice route to spin-split topological antiferromagnetism. Nature 658, 342–349 (2026). https://doi.org/10.1038/s41586-026-11073-7

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