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Emergent topological spin structures in the centrosymmetric cubic perovskite SrFeO3

S. Ishiwata, T. Nakajima, J.-H. Kim, D. S. Inosov, N. Kanazawa, J. S. White, J. L. Gavilano, R. Georgii, K. M. Seemann, G. Brandl, P. Manuel, D. D. Khalyavin, S. Seki, Y. Tokunaga, M. Kinoshita, Y. W. Long, Y. Kaneko, Y. Taguchi, T. Arima, B. Keimer, and Y. Tokura
Phys. Rev. B 101, 134406 – Published 6 April 2020
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Abstract

The skyrmion crystal (SkX) characterized by a triple-q helical spin modulation has been reported to be a unique topological state that competes with the single-q helimagnetic order in noncentrosymmetric materials with Dzyaloshinskii-Moriya (DM) interactions. Here, we report the discovery of a rich variety of multiple-q helimagnetic spin structures in the centrosymmetric cubic perovskite SrFeO3 without DM interactions. On the basis of neutron diffraction measurements, we have identified two types of robust multiple-q spin structures that appear in the absence of external magnetic fields: an anisotropic double-q spin spiral and an isotropic quadruple-q spiral hosting a three-dimensional lattice of topological singularities. The present system not only diversifies the family of SkX host materials but furthermore provides an experimental missing link between centrosymmetric lattices and topological helimagnetic order. It also offers perspectives for integration of SkXs into oxide electronic devices.

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  • Received 2 December 2019
  • Accepted 25 February 2020

DOI:https://doi.org/10.1103/PhysRevB.101.134406

©2020 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

S. Ishiwata1,2,3,*, T. Nakajima4, J.-H. Kim5, D. S. Inosov5,6, N. Kanazawa1, J. S. White7, J. L. Gavilano7, R. Georgii8,9, K. M. Seemann8,9, G. Brandl9, P. Manuel10, D. D. Khalyavin10, S. Seki4, Y. Tokunaga11, M. Kinoshita1, Y. W. Long4,12, Y. Kaneko4, Y. Taguchi4, T. Arima4,11, B. Keimer5, and Y. Tokura1,4

  • 1Department of Applied Physics and Quantum-Phase Electronics Center, University of Tokyo, Hongo, Tokyo 113-8656, Japan
  • 2JST-PRESTO, Kawaguchi, Saitama 332-0012, Japan
  • 3Division of Materials Physics, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan
  • 4RIKEN Center for Emergent Matter Science, Wako, Saitama 351-0198, Japan
  • 5Max-Planck-Institut für Festkörperforschung, D-70569 Stuttgart, Germany
  • 6Institut für Festkörper- und Materialphysik, TU Dresden, D-01069 Dresden, Germany
  • 7Laboratory for Neutron Scattering and Imaging, Paul Scherrer Institut, CH-5232 Villigen, Switzerland
  • 8Physik Department E21, Technische Universität München, D-85748 Garching, Germany
  • 9Heinz Maier-Leibnitz Zentrum, Technische Universität München, D-85748 Garching, Germany
  • 10ISIS Facility, STFC Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire OX11 0QX, United Kingdom
  • 11Department of Advanced Materials Science, University of Tokyo, Kashiwa 277-8561, Japan
  • 12Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

  • *ishiwata@mp.es.osaka-u.ac.jp

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Vol. 101, Iss. 13 — 1 April 2020

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Images

  • Figure 1
    Figure 1

    (a) Magnetic phase diagram for the applied field direction along [111]. The shaded and the white regions in phase I correspond to states with 12 and 3 domains, respectively. The schematic crystal structure and quadruple-q vectors viewed along [111] are shown on the right-hand side. (b) Double-q spin structure in phase I and (c) quadruple-q spin structure in phase II (the color of each spin corresponds to the spin component along the direction perpendicular to both q1 and q2 for (b) and that along [111] for (c), respectively). The magnified views around the singular points are shown at the bottom. Note that we adopt q1 and q2 instead of q1 and q2 for phase I.

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  • Figure 2
    Figure 2

    (a) Temperature dependence of integrated intensities of the magnetic scattering along qi (i=14) measured at zero field after field cooling. The total intensity for q14 is also shown. Magnetic field dependence of the magnetic scattering intensities for (b) phase I at 50 K and (c) phase II at 100 K. The data with solid lines and dashed lines were measured on increasing and decreasing the field along [111], respectively. The data for (b) and (c) were measured after zero-field cooling from room temperature.

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  • Figure 3
    Figure 3

    (a) Schematic representation describing the crystallographic directions and the azimuthal positions of magnetic scattering peaks in the horizontal configuration for phase I after field cooling (FC). The three red balls indicated by the red square on the gray sphere correspond to the triplet magnetic scattering peaks deviating by 2 from the [111] direction. (b) SANS data measured at 3 K with the relative rocking angle Δω=0. The observed magnetic reflection corresponds to the helimagnetic modulation q1(2), which is indicated by the red arrow in the (a). Stereographic projections of magnetic scattering peaks in (c) phase I after field cooling and (d) phase II. The solid and open circles represent the magnetic reflections for the proper-screw and vertical-cycloid-type spin propagations, respectively. (e) and (f) Integrated magnetic scattering profiles around q1 parallel to [111]. The peaks in (e) and (g) correspond to the triplet red solid circles and a single blue open circle in the (c), respectively. (g) and (h) Integrated magnetic scattering profiles around q2 parallel to [1¯1¯1]. The intensity is normalized by the largest value. The data were collected on heating in zero field after field cooling under a magnetic field of 6.8 T for SrFe0.99Co0.01O3. The data in (b), (e), and (f) were collected with the horizontal configuration, and those in (g) and (h) were collected with the vertical configuration (see Fig. S1 [42]).

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  • Figure 4
    Figure 4

    (a) The magnetic phase diagram of SrFe0.99Co0.01O3 reproduced from [46], on which the magnetic phase diagram of SrFeO3 is superimposed (the phase boundary of SrFeO3 is shown by dashed lines). The integrated neutron scattering intensities as a function of Δω at 3 K and 0.3 T for spin-flip (SF) and non-spin- flip (NSF) geometries are shown in the inset. All the data were collected after field cooling in a magnetic field of 7 T. Temperature dependence of SF and NSF scattering intensities measured on heating at (b) 0.3 T and (c) 7 T. In each case, the applied magnetic field and the incident neutron spin are parallel to [111]. Schematic illustrations of the spiral spin propagation for q2 or q2 with (d) vertical-cycloid-type (phase I), (e) proper-screw-type (phase II), and (f) horizontal-cycloid-type configurations, where the right-hand side shows the effective spin components for spin-polarized SANS.

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