Abstract
Although ferromagnets have many applications, their large magnetization and the resulting energy cost for switching magnetic moments bring into question their suitability for reliable low-power spintronic devices. Non-collinear antiferromagnetic systems do not suffer from this problem, and often have extra functionalities: non-collinear spin order1 may break space-inversion symmetry2,3 and thus allow electric-field control of magnetism4,5, or may produce emergent spin–orbit effects6 that enable efficient spin–charge interconversion7. To harness these traits for next-generation spintronics, the nanoscale control and imaging capabilities that are now routine for ferromagnets must be developed for antiferromagnetic systems. Here, using a non-invasive, scanning single-spin magnetometer based on a nitrogen–vacancy defect in diamond8,9,10, we demonstrate real-space visualization of non-collinear antiferromagnetic order in a magnetic thin film at room temperature. We image the spin cycloid of a multiferroic bismuth ferrite (BiFeO3) thin film and extract a period of about 70 nanometres, consistent with values determined by macroscopic diffraction11,12. In addition, we take advantage of the magnetoelectric coupling present in BiFeO3 to manipulate the cycloid propagation direction by an electric field. Besides highlighting the potential of nitrogen–vacancy magnetometry for imaging complex antiferromagnetic orders at the nanoscale, these results demonstrate how BiFeO3 can be used in the design of reconfigurable nanoscale spin textures.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on SpringerLink
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Coey, J. M. D. Noncollinear spin structures. Can. J. Phys. 65, 1210–1232 (1987)
Kimura, T. et al. Magnetic control of ferroelectric polarization. Nature 426, 55–58 (2003)
Cheong, S.-W. & Mostovoy, M. Multiferroics: a magnetic twist for ferroelectricity. Nat. Mater. 6, 13–20 (2007)
Lottermoser, T. et al. Magnetic phase control by an electric field. Nature 430, 541–544 (2004)
Heron, J. T. et al. Deterministic switching of ferromagnetism at room temperature using an electric field. Nature 516, 370–373 (2014)
Nayak, A. K. et al. Large anomalous Hall effect driven by a nonvanishing Berry curvature in the noncolinear antiferromagnet Mn3Ge. Sci. Adv. 2, e1501870 (2016)
Zhang, W. et al. Giant facet-dependent spin-orbit torque and spin Hall conductivity in the triangular antiferromagnet IrMn3 . Sci. Adv. 2, e1600759 (2016)
Maze, J. R. et al. Nanoscale magnetic sensing with an individual electronic spin in diamond. Nature 455, 644–647 (2008)
Balasubramanian, G. et al. Nanoscale imaging magnetometry with diamond spins under ambient conditions. Nature 455, 648–651 (2008)
Rondin, L. et al. Magnetometry with nitrogen-vacancy defects in diamond. Rep. Prog. Phys. 77, 056503 (2014)
Sosnowska, I., Neumaier, T. P., Steichele, E., Peterlin-Neumaier, T. & Steichele, E. Spiral magnetic ordering in bismuth ferrite. J. Phys. Chem. 15, 4835–4846 (1982)
Lebeugle, D. et al. Electric-field-induced spin flop in BiFeO3 single crystals at room temperature. Phys. Rev. Lett. 100, 227602 (2008)
Hartmann, U. Magnetic force microscopy. Annu. Rev. Mater. Sci. 29, 53–87 (1999)
Locatelli, A. & Bauer, E. Recent advances in chemical and magnetic imaging of surfaces and interfaces by XPEEM. J. Phys. Condens. Matter 20, 093002 (2008)
Wiesendanger, R. Spin mapping at the nanoscale and atomic scale. Rev. Mod. Phys. 81, 1495–1550 (2009)
Jungwirth, T., Marti, X., Wadley, P. & Wunderlich, J. Antiferromagnetic spintronics. Nature Nanotechnol. 11, 231–241 (2016)
Catalan, G. & Scott, J. F. Physics and applications of bismuth ferrite. Adv. Mater. 21, 2463–2485 (2009)
Rovillain, P. et al. Electric-field control of spin waves at room temperature in multiferroic BiFeO3 . Nat. Mater. 9, 975–979 (2010)
Balke, N. et al. Enhanced electric conductivity at ferroelectric vortex cores in BiFeO3 . Nat. Phys. 8, 81–88 (2011)
Catalan, G., Seidel, J., Ramesh, R. & Scott, J. F. Domain wall nanoelectronics. Rev. Mod. Phys. 84, 119–156 (2012)
Park, J.-G., Le, M. D., Jeong, J. & Lee, S. Structure and spin dynamics of multiferroic BiFeO3 . J. Phys. Cond. Mat. 26, 433202 (2014)
Sando, D. et al. Crafting the magnonic and spintronic response of BiFeO3 films by epitaxial strain. Nat. Mater. 12, 641–646 (2013)
Maletinsky, P. et al. A robust scanning diamond sensor for nanoscale imaging with single nitrogen-vacancy centres. Nature Nanotechnol. 7, 320–324 (2012)
Tetienne, J. P. et al. The nature of domain walls in ultrathin ferromagnets revealed by scanning nanomagnetometry. Nat. Commun. 6, 6733 (2015)
Agbelele, A. et al. Strain and magnetic field induced spin-structure transitions in multiferroic BiFeO3 . Adv. Mater. 29, 1602327 (2017)
Bertinshaw, J. et al. Direct evidence for the spin cycloid in strained nanoscale bismuth ferrite thin films. Nat. Commun. 7, 12664 (2016)
Ederer, C. & Spaldin, N. A. Weak ferromagnetism and magnetoelectric coupling in bismuth ferrite. Phys. Rev. B 71, 060401(R) (2005)
Ramazanoglu, M. et al. Local weak ferromagnetism in single-crystalline ferroelectric BiFeO3 . Phys. Rev. Lett. 107, 207206 (2011)
Mikuszeit, N., Meckler, S., Wiesendanger, R. & Miranda, R. Magnetostatics and the rotational sense of cycloidal spin spirals. Phys. Rev. B 84, 054404 (2011)
He, Q. et al. Magnetotransport at domain walls in BiFeO3 . Phys. Rev. Lett. 108, 067203 (2012)
Uecker, R. et al. Properties of rare-earth scandate single crystals (Re=Nd-Dy). J. Cryst. Growth 310, 2649–2658 (2008)
Johann, F., Morelli, A., Biggemann, D., Arredondo, M. & Vrejoiu, I. Epitaxial strain and electric boundary condition effects on the structural and ferroelectric properties of BiFeO3 films. Phys. Rev. B 84, 094105 (2011)
Chen, Z. H., Damodaran, A. R., Xu, R., Lee, S. & Martin, L. W. Effect of symmetry mismatch on the domain structure of rhombohedral BiFeO3 thin films. Appl. Phys. Lett. 104, 182908 (2014)
Zavaliche, F. et al. Multiferroic BiFeO3 films: domain structure and polarization dynamics. Phase Transitions 79, 991–1017 (2006)
Balke, N. et al. Deterministic control of ferroelastic switching in multiferroic materials. Nat. Nanotechnol. 4, 868–875 (2009)
Crassous, A., Sluka, T., Tagantsev, A. K. & Setter, N. Polarization charge as a reconfigurable quasi-dopant in ferroelectric thin films. Nat. Nanotechnol. 10, 614–618 (2015)
Rondin, L. et al. Nanoscale magnetic field mapping with a single spin scanning probe magnetometer. Appl. Phys. Lett. 100, 153118 (2012)
Appel, P. et al. Fabrication of all diamond scanning probes for nanoscale magnetometry. Rev. Sci. Instrum. 87, 063703 (2016)
Rondin, L. et al. Stray-field imaging of magnetic vortices with a single diamond spin. Nat. Commun. 4, 2279 (2013)
Hingant, T. et al. Measuring the magnetic moment density in patterned ultrathin ferromagnets with submicrometer resolution. Phys. Rev. Appl. 4, 014003 (2015)
Blakely, R. J. Potential Theory in Gravity and Magnetic Applications (Cambridge Univ. Press, 1996)
Acknowledgements
We thank J. P. Tetienne and T. Hingant for experimental assistance in the early stages of the project. We are grateful to J. M. D. Coey for discussions. This research was supported by the European Research Council (ERC-StG-2014, IMAGINE), the European Union Seventh Framework Program (FP7/2007-2013) under the project DIADEMS, and by the French Agence Nationale de la Recherche (ANR) through project FERROMON and PIAF. This work is supported by a public grant overseen by the French National Research Agency (ANR) as part of the ‘Investissements d’Avenir’ program (Labex NanoSaclay, reference: ANR-10-LABX-0035).
Author information
Authors and Affiliations
Contributions
I.G., W.A., L.J.M. and S.C. performed the NV magnetometry experiments; I.G., W.A., L.J.M. and V.J. analysed the data and performed magnetic modelling with assistance from M.V.; K.G. and C.C. fabricated the BFO sample; V.G. and S.F. performed the structural analysis and the piezoresponse force microscopy experiments; P.A. and P.M. engineered diamond tips hosting single NV defects; I.G., W.A., V.G., S.F., M.B. and V.J. wrote the manuscript. All authors contributed to the interpretation of the data and commented on the manuscript.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Additional information
Reviewer Information Nature thanks J. Mundy 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.
Extended data figures and tables
Extended Data Figure 1 Structural properties of the magnetic thin film.
a, The surface topography of the 6 μm × 6 μm 32-nm-thick BiFeO3 (BFO) thin film grown on a DyScO3 substrate, showing single-unit-cell atomic steps. b, X-ray diffraction ω–2θ pattern of the same film displays only (00l) peaks for BFO and DyScO3 (in monoclinic notation). D (in red colour) and B (in blue colour) subscripts stand for DyScO3 and BiFeO3, respectively. c, Zoom along the (001) peak of DyScO3, showing clear Laue fringes.
Extended Data Figure 2 Reciprocal space mappings (RSMs) of the 32-nm-thick BFO film grown on SrRuO3/DyScO3.
Shown are RSMs around a, (002)D, b, (004)D, c, , d, (013)D, e, , f, (113)D, g, and h, (103)D planes of DyScO3. All the planes are indexed in monoclinic notation and the subscripts D and B correspond to DyScO3 and BFO, respectively. Two different domains can be identified for monoclinic BFO (green and blue). Qx,y and Qz indicate the in-plane and out-of-plane reciprocal space units, respectively.
Extended Data Figure 3 Determination of polarization variants in BFO thin films.
a, Local out-of-plane PFM hysteresis loop with bias voltage. d33 is the out-of-plane piezoelectric coefficient. b, Homogeneous out-of-plane PFM phase corresponding to polarization variants pointing downward in a 6 μm × 6 μm area. c, In-plane PFM phase and d, amplitude for the cantilever parallel to [100]c. e, Sketch of the PFM cantilever and the four possible in-plane variants of polarization in BFO. f, Sketch of the [110]c direction of the cantilever, with the corresponding in-plane PFM amplitude (g) and phase (h). i, Sketch of the direction of the cantilever with the corresponding in-plane PFM amplitude (j) and phase (k). All the images in c to k have been acquired in the same 3 μm × 3 μm area.
Extended Data Figure 4 Measurement of the probe-to-sample distance.
a, The scanning-NV magnetometer (‘diamond tip’) is used to measure the magnetic field (grey arrows) produced at the edges of an uniformly magnetized ferromagnetic wire (blue arrows). b, Typical Zeeman-shift profile measured by scanning the NV defect across the edges of a 500-nm-wide wire of Pt/Co(0.6nm)/AlOx with perpendicular magnetic anisotropy. The circles are experimental data and the red solid line is data fitting from which distance d is extracted24,40. We note that only the absolute value of the magnetic field is measured in this experiment.
Extended Data Figure 5 Schematic of the geometry used for the stray field calculation.
The thickness, t, of the film is divided into N monolayers of thickness a. The blue plane represents the observation plane at a distance d from the BFO film. (x, y, z) and (x′, y′, z′) represent, respectively, the coordinates of the observation point and the magnetic moment with respect to the laboratory frame. The red dashed lines indicate the remaining monolayers in the film that are not illustrated.
Extended Data Figure 6 Data fitting and uncertainty analysis.
a, Magnetic field distribution reproduced from Fig. 4a of the main text. b, The black symbols are the experimental data and the coloured solid curve is the result of a two-dimensional fit using equation (17) with d = 49 nm, meff = 0.07μB, λ = 70 nm, a = 0.396 nm, t = 32 nm and (θ, ϕ) = (128°, 80°). The linecut shown in Fig. 4c of the main text corresponds to the white dashed line in a. c, Summary of the relative uncertainties on the fitting parameter mDM for the six parameters pi = {λ, meff, t, d, θ, ϕ} (see Methods for details).
Rights and permissions
About this article
Cite this article
Gross, I., Akhtar, W., Garcia, V. et al. Real-space imaging of non-collinear antiferromagnetic order with a single-spin magnetometer. Nature 549, 252–256 (2017). https://doi.org/10.1038/nature23656
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nature23656
This article is cited by
-
Voltage control of multiferroic magnon torque for reconfigurable logic-in-memory
Nature Communications (2024)
-
Revealing emergent magnetic charge in an antiferromagnet with diamond quantum magnetometry
Nature Materials (2024)
-
Switching the spin cycloid in BiFeO3 with an electric field
Nature Communications (2024)
-
Electric-field-induced multiferroic topological solitons
Nature Materials (2024)
-
High frequency magnetometry with an ensemble of spin qubits in hexagonal boron nitride
npj Quantum Information (2024)