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.

  • Letter
  • Published:

Atomic-scale fragmentation and collapse of antiferromagnetic order in a doped Mott insulator

Abstract

Disentangling the relationship between the insulating state with a charge gap and the magnetic order in an antiferromagnetic Mott insulator remains difficult due to inherent phase separation as the Mott state is perturbed1,2,3,4,5,6,7. Measuring magnetic and electronic properties at atomic length scales would provide crucial insight, but this is yet to be experimentally achieved. Here, we use spin-polarized scanning tunnelling microscopy (SP-STM) to visualize the periodic spin-resolved modulations originating from the antiferromagnetic order in a relativistic Mott insulator Sr2IrO4 (refs. 8,9), and how they change as a function of doping. We find that near the insulator-to-metal transition (IMT), the long-range antiferromagnetic order melts into a fragmented state with short-range correlations. Crucially, we discover that the short-range antiferromagnetic order is locally uncorrelated with the observed spectral gap magnitude. This suggests that static short-range antiferromagnetic correlations are unlikely to be the cause of the inhomogeneous closing of the spectral gap and the emergence of pseudogap regions near the IMT. Our work establishes SP-STM as a powerful tool for revealing atomic-scale magnetic information in complex oxides.

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: Measurement schematic, crystal structure and basic electronic characterization.
Fig. 2: Spin-resolved magnetic contrast modulations in lightly doped Sr-214.
Fig. 3: Fragmentation of the spin-resolved magnetic contrast modulations at higher electron doping.
Fig. 4: Relationship between short-range antiferromagnetic modulations and the electronic structure in x ≈ 0.05 Sr-214.

Similar content being viewed by others

Data availability

The data represented in Figs. 1f,g, 2g,h and 4e,f are available as Supplementary information files. All other data that support the plots within this paper and the other findings of this study are available from the corresponding author on reasonable request.

Code availability

The computer code used for data analysis is available on request from the corresponding author.

References

  1. Emery, V., Kivelson, S. & Lin, H. Phase separation in the t-J model. Phys. Rev. Lett. 64, 475–478 (1990).

    Article  ADS  Google Scholar 

  2. Yee, C.-H. & Balents, L. Phase separation in doped Mott insulators. Phys. Rev. X 5, 021007 (2015).

    Google Scholar 

  3. Qazilbash, M. M. et al. Mott transition in VO2 revealed by infrared spectroscopy and nano-imaging. Science 318, 1750–1753 (2007).

    Article  ADS  Google Scholar 

  4. Cai, P. et al. Visualizing the evolution from the Mott insulator to a charge-ordered insulator in lightly doped cuprates. Nat. Phys. 12, 1047–1051 (2016).

    Article  Google Scholar 

  5. Battisti, I. et al. Universality of pseudogap and emergent order in lightly doped Mott insulators. Nat. Phys. 13, 21–25 (2017).

    Article  Google Scholar 

  6. Chen, X. et al. Influence of electron doping on the ground state of (Sr1–xLax)2IrO4. Phys. Rev. B 92, 075125 (2015).

    Article  ADS  Google Scholar 

  7. Yan, Y. J. et al. Electron-doped Sr2IrO4: an analogue of hole-doped cuprate superconductors demonstrated by scanning tunneling microscopy. Phys. Rev. X 5, 041018 (2015).

    Google Scholar 

  8. Kim, B. et al. Novel J eff = 1/2 Mott state induced by relativistic spin-orbit coupling in Sr2IrO4. Phys. Rev. Lett. 101, 076402 (2008).

    Article  ADS  Google Scholar 

  9. Cao, G. & Schlottmann, P. The challenge of spin–orbit-tuned ground states in iridates: a key issues review. Rep. Prog. Phys. 81, 042502 (2018).

    Article  ADS  Google Scholar 

  10. Mott, N. F. The basis of the electron theory of metals, with special reference to the transition metals. Proc. Phys. Soc. A 62, 416–422 (1949).

    Article  ADS  Google Scholar 

  11. Imada, M., Fujimori, A. & Tokura, Y. Metal-insulator transitions. Rev. Mod. Phys. 70, 1039–1263 (1998).

    Article  ADS  Google Scholar 

  12. Lee, P. A., Nagaosa, N. & Wen, X.-G. Doping a Mott insulator: physics of high-temperature superconductivity. Rev. Mod. Phys. 78, 17–85 (2006).

    Article  ADS  Google Scholar 

  13. Rau, J. G., Lee, E. K.-H. & Kee, H.-Y. Spin-orbit physics giving rise to novel phases in correlated systems: iridates and related materials. Annu. Rev. Condens. Matter Phys. 7, 195–221 (2016).

    Article  ADS  Google Scholar 

  14. Wiesendanger, R. Spin mapping at the nanoscale and atomic scale. Rev. Mod. Phys. 81, 1495–1550 (2009).

    Article  ADS  Google Scholar 

  15. Jeon, S. et al. Distinguishing a Majorana zero mode using spin-resolved measurements. Science 358, 772–776 (2017).

    Article  ADS  Google Scholar 

  16. Natterer, F. D. D. et al. Reading and writing single-atom magnets. Nature 543, 226–228 (2017).

    Article  ADS  Google Scholar 

  17. Hirjibehedin, C. F. F., Lutz, C. P. P. & Heinrich, A. J. J. Spin coupling in engineered atomic structures. Science 312, 1021–1024 (2006).

    Article  ADS  Google Scholar 

  18. Enayat, M. et al. Real-space imaging of the atomic-scale magnetic structure of Fe1+yTe. Science 345, 653–656 (2014).

    Article  ADS  Google Scholar 

  19. Manna, S. et al. Interfacial superconductivity in a bi-collinear antiferromagnetically ordered FeTe monolayer on a topological insulator. Nat. Commun. 8, 14074 (2017).

    Article  ADS  Google Scholar 

  20. de la Torre, A. et al. Collapse of the Mott gap and emergence of a nodal liquid in lightly doped Sr2IrO4. Phys. Rev. Lett. 115, 176402 (2015).

    Article  ADS  Google Scholar 

  21. Cao, Y. et al. Hallmarks of the Mott-metal crossover in the hole-doped pseudospin-1/2 Mott insulator Sr2IrO4. Nat. Commun. 7, 11367 (2016).

    Article  ADS  Google Scholar 

  22. Kim, Y. K., Sung, N. H., Denlinger, J. D. & Kim, B. J. Observation of a d-wave gap in electron-doped Sr2IrO4. Nat. Phys. 12, 37–41 (2016).

    Article  Google Scholar 

  23. Kim, Y. K. et al. Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet. Science 345, 187–190 (2014).

    Article  ADS  Google Scholar 

  24. Chen, X. et al. Unidirectional spin density wave state in metallic (Sr1−xLax)2IrO4. Nat. Commun. 9, 103 (2018).

    Article  ADS  Google Scholar 

  25. Wang, F. & Senthil, T. Twisted hubbard model for Sr2IrO4: magnetism and possible high temperature superconductivity. Phys. Rev. Lett. 106, 136402 (2011).

    Article  ADS  Google Scholar 

  26. Ge, M. et al. Lattice-driven magnetoresistivity and metal-insulator transition in single-layered iridates. Phys. Rev. B 84, 100402 (2011).

    Article  ADS  Google Scholar 

  27. Zhao, H. et al. Charge-stripe crystal phase in an insulating cuprate. Nat. Mater. 18, 103–107 (2019).

    Article  ADS  Google Scholar 

  28. Guevara, J. M. et al. Spin-polaron ladder spectrum of the spin–orbit-induced Mott insulator Sr2IrO4 probed by scanning tunneling spectroscopy. Phys. Rev. B 99, 121114 (2019).

    Article  ADS  Google Scholar 

  29. Kyung, B. et al. Pseudogap induced by short-range spin correlations in a doped Mott insulator. Phys. Rev. B 73, 165114 (2006).

    Article  ADS  Google Scholar 

  30. Ye, F. et al. Magnetic and crystal structures of Sr2IrO4: a neutron diffraction study. Phys. Rev. B 87, 140406 (2013).

    Article  ADS  Google Scholar 

  31. Kim, J. et al. Magnetic excitation spectra of Sr2IrO4 probed by resonant inelastic X-ray scattering: establishing links to cuprate superconductors. Phys. Rev. Lett. 108, 177003 (2012).

    Article  ADS  Google Scholar 

  32. Zhou, S., Jiang, K., Chen, H. & Wang, Z. Correlation effects and hidden spin–orbit entangled electronic order in parent and electron-doped iridates Sr2IrO4. Phys. Rev. X 7, 041018 (2017).

    Google Scholar 

  33. Solovyev, I. V., Mazurenko, V. V. & Katanin, A. A. Validity and limitations of the superexchange model for the magnetic properties of Sr2IrO4 and Ba2IrO4 mediated by the strong spin-orbit coupling. Phys. Rev. B 92, 235109 (2015).

    Article  ADS  Google Scholar 

  34. Zhao, L. et al. Evidence of an odd-parity hidden order in a spin–orbit coupled correlated iridate. Nat. Phys. 12, 32–36 (2016).

    Article  Google Scholar 

  35. Lawler, M. J. et al. Intra-unit-cell electronic nematicity of the high-T c copper-oxide pseudogap states. Nature 466, 347–351 (2010).

    Article  ADS  Google Scholar 

  36. Huang, D., Liu, S., Zeljkovic, I., Mitchell, J. F. & Hoffman, J. E. Etching of Cr tips for scanning tunneling microscopy of cleavable oxides. Rev. Sci. Instrum. 88, 023705 (2017).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

We thank J. Hoffman, P. Lee and V. Madhavan for valuable discussions, and G. Gu for supplying the FeTe single crystals for characterizing spin-polarized STM tips. The spin-polarized STM measurements were supported by the US Department of Energy Early Career Award DE-SC0020130. I.Z. also acknowledges the support from the Army Research Office grant number W911NF-17-1-0399 (H.Z.) and the National Science Foundation grant number NSF-DMR-1654041 (A.U.) for developing the spin-polarized STM capability. Z.W. acknowledges the support from the US Department of Energy, Basic Energy Sciences grant no. DE-FG02-99ER45747. S.M. and J.M. would like to acknowledge the Office of Naval Research grant N00014-16-1-2657, the National Science Foundation grant DMR-1700137 and a grant from the John Templeton Foundation. S.D.W. acknowledges the support from the National Science Foundation award no. DMR-1905801 (S.D.W.), and additional funding support from the Army Research Office award W911NF-16-1-0361 (Z.P.).

Author information

Authors and Affiliations

Authors

Contributions

STM experiments were carried out by H.Z. H.Z., S.M. and A.U. were responsible for fabrication and initial characterization of spin-polarized STM tips. Iridate single crystals were grown by Z.P. and X.C., supervised by S.D.W. H.Z. analysed the STM data with guidance from I.Z. Z.W. provided theoretical input on the interpretation of the STM data. I.Z., S.D.W., Z.W., H.Z. and J.M. wrote the manuscript with input from all the authors. I.Z. supervised the project.

Corresponding author

Correspondence to Ilija Zeljkovic.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature Physics thanks Milan Allan 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 Figs. 1–13 and refs. 1–16.

Source data

Source Data Fig. 1

Data plotted in Fig. 1f,g.

Source Data Fig. 2

Data plotted in Fig. 2g,h.

Source Data Fig. 4

Data plotted in Fig. 4e,f.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhao, H., Manna, S., Porter, Z. et al. Atomic-scale fragmentation and collapse of antiferromagnetic order in a doped Mott insulator. Nat. Phys. 15, 1267–1272 (2019). https://doi.org/10.1038/s41567-019-0671-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41567-019-0671-9

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