Atomic scale imaging of magnetic circular dichroism by achromatic electron microscopy

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.

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.

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

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.

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

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

Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden

Graduate School of Pure & Applied Science and Faculty of Pure & Applied Science, University of Tsukuba, Tsukuba, Japan

Central Facility for Electron Microscopy, RWTH Aachen University, Aachen, Germany

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.

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A correction to this article is available online at https://doi.org/10.1038/s41563-018-0039-z.

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