Letter

Atomic scale imaging of magnetic circular dichroism by achromatic electron microscopy

  • Nature Materialsvolume 17pages221225 (2018)
  • doi:10.1038/s41563-017-0010-4
  • Download Citation
Received:
Accepted:
Published online:

Abstract

In order to obtain a fundamental understanding of the interplay between charge, spin, orbital and lattice degrees of freedom in magnetic materials and to predict and control their physical properties1,2,3, experimental techniques are required that are capable of accessing local magnetic information with atomic-scale spatial resolution. Here, we show that a combination of electron energy-loss magnetic chiral dichroism4 and chromatic-aberration-corrected transmission electron microscopy, which reduces the focal spread of inelastically scattered electrons by orders of magnitude when compared with the use of spherical aberration correction alone, can achieve atomic-scale imaging of magnetic circular dichroism and provide element-selective orbital and spin magnetic moments atomic plane by atomic plane. This unique capability, which we demonstrate for Sr2FeMoO6, opens the door to local atomic-level studies of spin configurations in a multitude of materials that exhibit different types of magnetic coupling, thereby contributing to a detailed understanding of the physical origins of magnetic properties of materials at the highest spatial resolution.

  • Subscribe to Nature Materials for full access:

    $59

    Subscribe

Additional access options:

Already a subscriber?  Log in  now or  Register  for online access.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Change history

  • Correction 14 February 2018

    In Fig. 1 of the version of this Letter originally published, the word ‘Subtract’ was missing from the green box to the left of panel f. This has now been corrected in all versions of the Letter.

References

  1. 1.

    Tokura, Y. & Nagaosa, N. Orbital physics in transition-metal oxides. Science 288, 462–468 (2000).

  2. 2.

    Zubko, P., Gariglio, S., Gabay, M., Ghosez, P. & Triscone, J. M. Interface physics in complex oxide heterostructures. Annu. Rev. Condens. Matter Phys. 2, 141–165 (2011).

  3. 3.

    Hwang, H. Y. et al. Emergent phenomena at oxide interfaces. Nat. Mater. 11, 103–113 (2012).

  4. 4.

    Schattschneider, P. et al. Detection of magnetic circular dichroism using a transmission electron microscope. Nature 441, 486–488 (2006).

  5. 5.

    Wiesendanger, R. et al. Topographic and magnetic-sensitive scanning tunneling microscopy study of magnetite. Science 255, 583–586 (1992).

  6. 6.

    Heinze, S. et al. Real-space imaging of two-dimensional antiferromagnetism on the atomic scale. Science 294, 1488–1495 (2001).

  7. 7.

    Kaiser, U., Schwarz, A. & Wiesendanger, R. Magnetic exchange force microscopy with atomic resolution. Nature 446, 522–525 (2007).

  8. 8.

    Beaurepaire, E, Bulou, H, Scheurer, F. & Kappler, J. P. Magnetism and Synchrotron Radiation. (Springer: Heidelberg, 2009).

  9. 9.

    Chao, W. L., Harteneck, B. D., Liddle, J. A., Anderson, E. H. & Attwood, D. T. Soft X-ray microscopy at a spatial resolution better than 15nm. Nature 435, 1210–1213 (2005).

  10. 10.

    Zhu, X. H. et al Measuring spectroscopy and magnetism of extracted and intracellular magnetosomes using soft X-ray ptychography. Proc. Natl Acad. Sci. USA 113, E8219–E8227 (2016).

  11. 11.

    Midgley, P. A. & Dunin-Borkowski, R. E. Electron tomography and holography in materials science. Nat. Mater. 8, 271–280 (2009).

  12. 12.

    Lidbaum, H. et al. Quantitative magnetic information from reciprocal space maps in transmission electron microscopy. Phys. Rev. Lett. 102, 037201 (2009).

  13. 13.

    Wang, Z. Q., Zhong, X. Y., Yu, R., Cheng, Z. Y. & Zhu, J. Quantitative experimental determination of site-specific magnetic structures by transmitted electrons. Nat. Commun. 4, 1395 (2013).

  14. 14.

    Song, D. S., Li, G., Cai, J. W. & Zhu, J. A general way for quantitative magnetic measurement by transmitted electrons. Sci. Rep. 6, 18489 (2016).

  15. 15.

    Wang, Z. C. et al. Effects of dynamic diffraction conditions on magnetic parameter determination in a double perovskite Sr2FeMoO6 using electron energy-loss magnetic chiral dichroism. Ultramicroscopy 176, 212–217 (2017).

  16. 16.

    Schattschneider, P. et al. Detection of magnetic circular dichroism on the two-nanometer scale. Phys. Rev. B 78, 104413 (2008).

  17. 17.

    Jin, L. et al. Direct demonstration of a magnetic dead layer resulting from A-site cation inhomogeneity in a (La,Sr)MnO3 epitaxial film system. Adv. Mater. Interfaces 3, 1600414 (2016).

  18. 18.

    Thersleff, T., Rusz, J., Hjorvarsson, B. & Leifer, K. Detection of magnetic circular dichroism with subnanometer convergent electron beams. Phys. Rev. B 94, 134430 (2016).

  19. 19.

    Rusz, J. et al. Magnetic measurements with atomic-plane resolution. Nat. Commun. 7, 12672 (2016).

  20. 20.

    Rusz, J. et al. Achieving atomic resolution magnetic dichroism by controlling the phase symmetry of an electron probe. Phys. Rev. Lett. 113, 145501 (2014).

  21. 21.

    Idrobo, J. C. et al. Detecting magnetic ordering with atomic size electron probes. Adv. Struct. Chem. Imag. 2, 5 (2016).

  22. 22.

    Reimer, L., Fromn, I., Hirsch, P., Plate, U. & Rennekamp, R. Combination of EELS modes and electron spectroscopic imaging and diffraction in an energy-filtering electron microscope. Ultramicroscopy 46, 335–347 (1992).

  23. 23.

    Kimoto, K., Sekiguchi, T. & Aoyama, T. Chemical shift mapping of Si L and K edges using spatially resolved EELS and energy-filtering TEM. J. Electron Microsc. 46, 369–374 (1997).

  24. 24.

    Walther, T. Electron energy-loss spectroscopic profiling of thin film structures: 0.39 nm line resolution and 0.04 eV precision measurement of near-edge structure shifts at interfaces. Ultramicroscopy 96, 401–411 (2003).

  25. 25.

    Kabius, B. et al. First application of Cc-corrected imaging for high-resolution and energy-filtered TEM. J. Electron Microsc. 58, 147–155 (2009).

  26. 26.

    Urban, K. W. et al. Achromatic elemental mapping beyond the nanoscale in the transmission electron microscope. Phys. Rev. Lett. 110, 185507 (2013).

  27. 27.

    Forbes, B. D., Houben, L., Mayer, J., Dunin-Borkowski, R. E. & Allen, L. J. Elemental mapping in achromatic atomic-resolution energy-filtered transmission electron microscopy. Ultramicroscopy 147, 98–105 (2014).

  28. 28.

    Calmels, L. et al. Experimental application of sum rules for electron energy loss magnetic chiral dichroism. Phys. Rev. B 76, 060409 (2007).

  29. 29.

    Rusz, J., Eriksson, O., Novák, P. & Oppeneer, P. Sum rules for electron energy loss near edge spectra. Phys. Rev. B 89, 134428 (2014).

  30. 30.

    Koide, T. et al. Microscopic origin of ferrimagnetism of a double perovskite Sr2FeMoO6: an X-ray magnetic circular dichroism study. J. Phys. Conf. Ser. 502, 012003 (2014).

  31. 31.

    Kobayashi, K.-I., Kimura, T., Sawada, H., Terakura, K. & Tokura, Y. Room-temperature magnetoresistance in an oxide material with an ordered double-perovskite structure. Nature 395, 677–680 (1998).

  32. 32.

    Moritomo, Y. et al. Crystal and magnetic structure of conducting double perovskite Sr2FeMoO6. J. Phys. Soc. Jap 69, 1723–1726 (2000).

  33. 33.

    Serrate, D., De Teresa, J. M. & Ibarra, M. R. Double perovskites with ferromagnetism above room temperature. J. Phys. Condens. Matter 19, 023201 (2007).

  34. 34.

    Barthel, J., Houben, L. & Tillmann, K. J. Large-Scale Res. Facil. 1, A34 (2015).

  35. 35.

    Varela, M. et al. Atomic-resolution imaging of oxidation states in manganites. Phys. Rev. B 79, 085117 (2009).

  36. 36.

    Cueva, P. C., Hovden, R., Mundy, J. A., Xin, H. L. & Muller, D. A. Data processing for atomic resolution electron energy loss spectroscopy. Microsc. Microanal. 18, 667–669 (2012).

  37. 37.

    Rusz, J., Bhowmick, S., Eriksson, M. & Karlsson, N. Scattering of electron vortex beams on a magnetic crystal: Towards atomic-resolution magnetic measurements. Phys. Rev. B 89, 134428 (2014).

  38. 38.

    Song, D. S., Wang, Z. Q. & Zhu, J. Effect of the asymmetry of dynamical electron diffraction on intensity of acquired EMCD signals. Ultramicroscopy 148, 42–51 (2015).

Download references

Acknowledgements

This work was supported by the National Key Research and Development Program (2016YFB0700402), the National Natural Science Foundation of China (51671112, 5171101391, 51471096, 11374174, 51390471, 51527803, 51525102, 51390475, 51371102), the National Basic Research Program of China (2015CB921700, 2015CB654902), Tsinghua University (20141081200), National Key Scientific Instruments and Equipment Development Project (2013YQ120353) and the “Strategic Partnership RWTH-Aachen University and Tsinghua University” Program. R.D.-B. is grateful for funding from the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007-2013)/ ERC grant agreement number 320832. This work made use of resources in Forschungszentrum Jülich, Germany and the National Center for Electron Microscopy in Beijing, China. J.R. acknowledges the Swedish Research Council and Göran Gustafsson’s Foundation for financial support. Calculations were performed using the Swedish National Infrastructure for Computing (SNIC) on a Triolith cluster at the National Supercomputer Center (NSC) of Linköping University. L. Houben, C.-L. Jia, M. Lentzen, M. Luysberg, C. B. Boothroyd, A. Schwedt, D. Meertens, M. Kruth, M. Duchamp, E. Kita, H. Yanagihara, P. Ercius, C. Kisielowski, F.-R. Chen, M. Linck, H. Müller and M. Haider are gratefully acknowledged for helpful discussions and assistance.

Author information

Affiliations

  1. National Center for Electron Microscopy in Beijing, Key Laboratory of Advanced Materials (MOE), The State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, China

    • Zechao Wang
    • , Hanbo Jiang
    • , Rong Yu
    • , Jing Zhu
    •  & Xiaoyan Zhong
  2. Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute, Forschungszentrum Jülich GmbH, Jülich, Germany

    • Amir H. Tavabi
    • , Lei Jin
    • , Joachim Mayer
    •  & Rafal E. Dunin-Borkowski
  3. Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden

    • Ján Rusz
    •  & Dmitry Tyutyunnikov
  4. Graduate School of Pure & Applied Science and Faculty of Pure & Applied Science, University of Tsukuba, Tsukuba, Japan

    • Yutaka Moritomo
  5. Central Facility for Electron Microscopy, RWTH Aachen University, Aachen, Germany

    • Joachim Mayer

Authors

  1. Search for Zechao Wang in:

  2. Search for Amir H. Tavabi in:

  3. Search for Lei Jin in:

  4. Search for Ján Rusz in:

  5. Search for Dmitry Tyutyunnikov in:

  6. Search for Hanbo Jiang in:

  7. Search for Yutaka Moritomo in:

  8. Search for Joachim Mayer in:

  9. Search for Rafal E. Dunin-Borkowski in:

  10. Search for Rong Yu in:

  11. Search for Jing Zhu in:

  12. Search for Xiaoyan Zhong in:

Contributions

X.Y.Z. initiated the idea and developed the principles. Z.C.W. prepared the TEM samples, performed HRTEM/STEM experiments, processed the experimental data under the supervision of L.J. and X.Y.Z., and drafted the manuscript. A.T., L.J. and X.Y.Z. carried out achromatic atomic-scale SREELS and EMCD measurements in Jülich. J.R. and D.T. carried out theoretical simulations of atomic-scale mapping of MCD. R.Y. and J.Z. participated in the development of the principles and experimental design. Y.M. provided the bulk sample. J.M., R.D.-B., R.Y. and J.Z. contributed to the scientific discussions. All of the authors participated in discussions and writing the manuscript.

Competing interests

The authors declare no competing financial interests

Corresponding author

Correspondence to Xiaoyan Zhong.

Supplementary information

  1. Supplementary Information

    Supplementary Figures 1–3, Supplementary Table 1