- Physical Review Journals
All JournalsPhysics Magazine

Physical Review B

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Long-range magnetic interactions in Nd2PdSi3 and the formation of skyrmion phases in centrosymmetric metals

Viviane Peçanha-Antonio1,2,*, Zhaoyang Shan3, Michael Smidman3, Juba Bouaziz4, Bachir Ouladdiaf5, Iurii Kibalin5, Marie-Hélène Lemée-Cailleau5, Christian Balz2, Jakob Lass6 et al.

Daniel A. Mayoh7, Geetha Balakrishnan7, Julie B. Staunton7, Devashibhai Adroja2,8, and Andrew T. Boothroyd1,†

  • *Contact author: viviane.antonio@stfc.ac.uk
  • †Contact author: andrew.boothroyd@physics.ox.ac.uk
PDF

Phys. Rev. B 114, 074421 – Published 14 August, 2026

DOI: https://doi.org/10.1103/vpy4-9zgh

Abstract

We present an extensive x-ray and neutron scattering study of the structure and magnetic excitations of Nd2PdSi3, a sister compound of Gd2PdSi3 that was recently found to host a skyrmion lattice phase despite its centrosymmetric crystal structure. Dispersive magnetic excitations were measured throughout the Brillouin zone and modeled to determine the magnetic interactions between Nd ions. Our analysis reveals that the magnetic interactions in this system extend over large distances and are significantly affected by a crystallographic superstructure formed by ordering of the Pd and Si atoms. The results suggest that the mechanism for the skyrmion phase formation in this family of materials, specifically Gd2PdSi3, is through the long-range Ruderman-Kittel-Kasuya-Yosida interactions rather than short-range triangular-lattice frustration.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (66)

  1. S. Mühlbauer, B. Binz, F. Jonietz, C. Pfleiderer, A. Rosch, A. Neubauer, R. Georgii, and P. Böni, Skyrmion lattice in a chiral magnet, Science 323, 915 (2009).
  2. C. Pappas, E. Lelièvre-Berna, P. Falus, P. M. Bentley, E. Moskvin, S. Grigoriev, P. Fouquet, and B. Farago, Chiral paramagnetic skyrmion-like phase in MnSi, Phys. Rev. Lett. 102, 197202 (2009).
  3. X. Z. Yu, Y. Onose, N. Kanazawa, J. H. Park, J. H. Han, Y. Matsui, N. Nagaosa, and Y. Tokura, Real-space observation of a two-dimensional skyrmion crystal, Nature (London) 465, 901 (2010).
  4. A. Fert, V. Cros, and J. Sampaio, Skyrmions on the track, Nat. Nanotechnol. 8, 152 (2013).
  5. T. Lancaster, Skyrmions in magnetic materials, Contemp. Phys. 60, 246 (2019).
  6. A. N. Bogdanov and C. Panagopoulos, Physical foundations and basic properties of magnetic skyrmions, Nat. Rev. Phys. 2, 492 (2020).
  7. L. Thomas, F. Lionti, R. Ballou, D. Gatteschi, R. Sessoli, and B. Barbara, Macroscopic quantum tunnelling of magnetization in a single crystal of nanomagnets, Nature (London) 383, 145 (1996).
  8. R. Wiesendanger, Nanoscale magnetic skyrmions in metallic films and multilayers: A new twist for spintronics, Nat. Rev. Mater. 1, 16044 (2016).
  9. C. Moreau-Luchaire, C. Moutafis, N. Reyren, J. Sampaio, C. A. F. Vaz, N. Van Horne, K. Bouzehouane, K. Garcia, C. Deranlot, P. Warnicke, P. Wohlhüter, J. M. George, M. Weigand, J. Raabe, V. Cros, and A. Fert, Additive interfacial chiral interaction in multilayers for stabilization of small individual skyrmions at room temperature, Nat. Nanotechnol. 11, 444 (2016).
  10. C. Psaroudaki and C. Panagopoulos, Skyrmion qubits: A new class of quantum logic elements based on nanoscale magnetization, Phys. Rev. Lett. 127, 067201 (2021).
  11. J. Xia, X. Zhang, X. Liu, Y. Zhou, and M. Ezawa, Universal quantum computation based on nanoscale skyrmion helicity qubits in frustrated magnets, Phys. Rev. Lett. 130, 106701 (2023).
  12. T. Okubo, S. Chung, and H. Kawamura, Multiple-q states and the skyrmion lattice of the triangular-lattice Heisenberg antiferromagnet under magnetic fields, Phys. Rev. Lett. 108, 017206 (2012).
  13. A. O. Leonov and M. Mostovoy, Multiply periodic states and isolated skyrmions in an anisotropic frustrated magnet, Nat. Commun. 6, 8275 (2015).
  14. V. Lohani, C. Hickey, J. Masell, and A. Rosch, Quantum skyrmions in frustrated ferromagnets, Phys. Rev. X 9, 041063 (2019).
  15. Z. Wang, Y. Su, S.-Z. Lin, and C. D. Batista, Skyrmion crystal from RKKY interaction mediated by 2D electron gas, Phys. Rev. Lett. 124, 207201 (2020).
  16. Z. Wang, Y. Su, S.-Z. Lin, and C. D. Batista, Meron, skyrmion, and vortex crystals in centrosymmetric tetragonal magnets, Phys. Rev. B 103, 104408 (2021).
  17. S. Hayami, R. Ozawa, and Y. Motome, Effective bilinear-biquadratic model for noncoplanar ordering in itinerant magnets, Phys. Rev. B 95, 224424 (2017).
  18. T. Nomoto, T. Koretsune, and R. Arita, Formation mechanism of the helical Q structure in Gd-based skyrmion materials, Phys. Rev. Lett. 125, 117204 (2020).
  19. S.-Z. Lin and S. Hayami, Ginzburg–Landau theory for skyrmions in inversion-symmetric magnets with competing interactions, Phys. Rev. B 93, 064430 (2016).
  20. O. I. Utesov, Mean-field description of skyrmion lattice in hexagonal frustrated antiferromagnets, Phys. Rev. B 105, 054435 (2022).
  21. S. Hayami and Y. Motome, Square skyrmion crystal in centrosymmetric itinerant magnets, Phys. Rev. B 103, 024439 (2021).
  22. K. Mitsumoto and H. Kawamura, Replica symmetry breaking in the RKKY skyrmion-crystal system, Phys. Rev. B 104, 184432 (2021).
  23. J. Bouaziz, E. Mendive-Tapia, S. Blügel, and J. B. Staunton, Fermi-surface origin of skyrmion lattices in centrosymmetric rare-earth intermetallics, Phys. Rev. Lett. 128, 157206 (2022).
  24. Y. Dong, Y. Arai, K. Kuroda, M. Ochi, N. Tanaka, Y. Wan, M. D. Watson, T. K. Kim, C. Cacho, M. Hashimoto, D. Lu, Y. Aoki, T. D. Matsuda, and T. Kondo, Fermi surface nesting driving the RKKY interaction in the centrosymmetric skyrmion magnet Gd2PdSi3, Phys. Rev. Lett. 133, 016401 (2024).
  25. T. Kurumaji, T. Nakajima, M. Hirschberger, A. Kikkawa, Y. Yamasaki, H. Sagayama, H. Nakao, Y. Taguchi, T. Arima, and Y. Tokura, Skyrmion lattice with a giant topological Hall effect in a frustrated triangular-lattice magnet, Science 365, 914 (2019).
  26. M. Hirschberger, T. Nakajima, S. Gao, L. Peng, A. Kikkawa, T. Kurumaji, M. Kriener, Y. Yamasaki, H. Sagayama, H. Nakao, K. Ohishi, K. Kakurai, Y. Taguchi, X. Yu, T.-h. Arima, and Y. Tokura, Skyrmion phase and competing magnetic orders on a breathing kagomé lattice, Nat. Commun. 10, 5831 (2019).
  27. N. D. Khanh, T. Nakajima, X. Yu, S. Gao, K. Shibata, M. Hirschberger, Y. Yamasaki, H. Sagayama, H. Nakao, L. Peng, K. Nakajima, R. Takagi, T.-h. Arima, Y. Tokura, and S. Seki, Nanometric square skyrmion lattice in a centrosymmetric tetragonal magnet, Nat. Nanotechnol. 15, 444 (2020).
  28. R. Takagi, N. Matsuyama, V. Ukleev, L. Yu, J. S. White, S. Francoual, J. R. L. Mardegan, S. Hayami, H. Saito, K. Kaneko, K. Ohishi, Y. Ōnuki, A. Taka-Hisa, Y. Tokura, T. Nakajima, and S. Seki, Square and rhombic lattices of magnetic skyrmions in a centrosymmetric binary compound, Nat. Commun. 13, 1472 (2022).
  29. S. Gao, H. D. Rosales, F. A. G. Albarracín, V. Tsurkan, G. Kaur, T. Fennell, P. Steffens, M. Boehm, P. Čermák, A. Schneidewind, E. Ressouche, D. C. Cabra, C. Rüegg, and O. Zaharko, Fractional antiferromagnetic skyrmion lattice induced by anisotropic couplings, Nature (London) 586, 37 (2020).
  30. R. Mallik, E. V. Sampathkumaran, M. Strecker, and G. Wortmann, Observation of a minimum in the temperature-dependent electrical resistance above the magnetic-ordering temperature in Gd2PdSi3, Europhys. Lett. 41, 315 (1998).
  31. P. Kotsanidis, J. Yakinthos, and E. Gamari-Seale, Magnetic properties of the ternary rare earth silicides R2PdSi3 (R=Pr, Nd, Gd, Tb, Dy, Ho, Er, Tm and Y), J. Magn. Magn. Mater. 87, 199 (1990).
  32. R. Mallik, E. Sampathkumaran, and P. Paulose, Large low temperature magnetoresistance and magnetic anomalies in Tb2PdSi3 and Dy2PdSi3, Solid State Commun. 106, 169 (1998).
  33. S. R. Saha, H. Sugawara, T. D. Matsuda, Y. Aoki, H. Sato, and E. V. Sampathkumaran, Magnetic, thermal, and transport properties of single crystals of antiferromagnetic Kondo-lattice Ce2PdSi3, Phys. Rev. B 62, 425 (2000).
  34. A. Szytuła, M. Hofmann, B. Penc, M. Ślaski, S. Majumdar, E. Sampathkumaran, and A. Zygmunt, Magnetic behaviour of R2PdSi3 compounds with R=Ce, Nd, Tb–Er, J. Magn. Magn. Mater. 202, 365 (1999).
  35. M. Frontzek, A. Kreyssig, M. Doerr, A. Schneidewind, J.-U. Hoffmann, and M. Loewenhaupt, Frustration in R2PdSi3 (R=Tb, Er) compounds: Spin-glass or magnetic short range order? Neutron diffraction studies, J. Phys.: Condens. Matter 19, 145276 (2007).
  36. M. Frontzek, A. Kreyssig, M. Doerr, M. Rotter, G. Behr, W. Löser, I. Mazilu, and M. Loewenhaupt, Magneto-crystalline anisotropy in R2PdSi3 (R=Tb, Dy, Ho, Er, Tm) single crystals, J. Magn. Magn. Mater. 301, 398 (2006).
  37. D. X. Li, S. Nimori, Y. Shiokawa, Y. Haga, E. Yamamoto, and Y. Onuki, ac susceptibility and magnetic relaxation of R2PdSi3 (R = Nd, Tb, and Dy), Phys. Rev. B 68, 012413 (2003).
  38. S. Majumdar, E. V. Sampathkumaran, P. L. Paulose, H. Bitterlich, W. Löser, and G. Behr, Anisotropic giant magnetoresistance, magnetocaloric effect, and magnetic anomalies in single crystalline Tb2PdSi3, Phys. Rev. B 62, 14207 (2000).
  39. S. Majumdar, H. Bitterlich, G. Behr, W. Löser, P. L. Paulose, and E. V. Sampathkumaran, Magnetic and transport behavior of single-crystalline Dy2PdSi3, Phys. Rev. B 64, 012418 (2001).
  40. P. L. Paulose, E. V. Sampathkumaran, H. Bitterlich, G. Behr, and W. Löser, Anisotropic spin-glass-like and quasi-one-dimensional magnetic behavior in the intermetallic compound Tb2PdSi3, Phys. Rev. B 67, 212401 (2003).
  41. S. R. Saha, H. Sugawara, T. D. Matsuda, H. Sato, R. Mallik, and E. V. Sampathkumaran, Magnetic anisotropy, first-order-like metamagnetic transitions, and large negative magnetoresistance in single-crystal Gd2PdSi3, Phys. Rev. B 60, 12162 (1999).
  42. M. Gomilšek, T. J. Hicken, M. N. Wilson, K. J. A. Franke, B. M. Huddart, A. Štefančič, S. J. R. Holt, G. Balakrishnan, D. A. Mayoh, M. T. Birch, S. H. Moody, H. Luetkens, Z. Guguchia, M. T. F. Telling, P. J. Baker, S. J. Clark, and T. Lancaster, Anisotropic skyrmion and multi-q spin dynamics in centrosymmetric Gd2PdSi3, Phys. Rev. Lett. 134, 046702 (2025).
  43. J. A. M. Paddison, B. K. Rai, A. F. May, S. Calder, M. B. Stone, M. D. Frontzek, and A. D. Christianson, Magnetic interactions of the centrosymmetric skyrmion material Gd2PdSi3, Phys. Rev. Lett. 129, 137202 (2022).
  44. J. Ju, H. Saito, T. Kurumaji, M. Hirschberger, A. Kikkawa, Y. Taguchi, T. H. Arima, Y. Tokura, and T. Nakajima, Polarized neutron scattering study of the centrosymmetric skyrmion host material Gd2PdSi3, Phys. Rev. B 107, 024405 (2023).
  45. D. Mayoh, A. Štefančič, M. Lees, and G. Balakrishnan, Crystal growth of the R2PdSi3 (R=rare earth) materials using the optical floating zone technique, J. Cryst. Growth 642, 127774 (2024).
  46. M. Smidman, C. Ritter, D. T. Adroja, S. Rayaprol, T. Basu, E. V. Sampathkumaran, and A. D. Hillier, Magnetic order in Nd2PdSi3 investigated using neutron scattering and muon spin relaxation, Phys. Rev. B 100, 134423 (2019).
  47. R. I. Bewley, R. S. Eccleston, K. A. McEwen, S. M. Hayden, M. T. Dove, S. M. Bennington, J. R. Treadgold, and R. L. S. Coleman,, MERLIN: A new high count rate spectrometer at ISIS, Phys. B: Condens. Matter 385, 1029 (2006).
  48. R. Bewley, J. Taylor, and S. Bennington, LET, a cold neutron multi-disk chopper spectrometer at ISIS, Nucl. Instrum. Methods Phys. Res. Sect. A 637, 128 (2011).
  49. J. Lass et al., Commissioning of the novel continuous angle multi-energy analysis spectrometer at the Paul Scherrer Institut, Rev. Sci. Instrum. 94, 023302 (2023).
  50. J. Lass, H. Jacobsen, D. G. Mazzone, and K. Lefmann, MJOLNIR: A software package for multiplexing neutron spectrometers, SoftwareX 12, 100600 (2020).
  51. F. Tang, M. Frontzek, J. Dshemuchadse, T. Leisegang, M. Zschornak, R. Mietrach, J.-U. Hoffmann, W. Löser, S. Gemming, D. C. Meyer, and M. Loewenhaupt, Crystallographic superstructure in R2PdSi3 compounds (R= heavy rare earth), Phys. Rev. B 84, 104105 (2011).
  52. See Supplemental Material at http://link.aps.org/supplemental/10.1103/vpy4-9zgh for details of the sample characterization, x-ray and neutron diffraction data of the Pd/Si superstructure and magnetic structure, data analysis, model, ab initio electronic structure calculations, and for additional figures showing fits to the data, which includes Refs. [23, 63, 64, 65, 66].
  53. J. Rodríguez-Carvajal, Recent advances in magnetic structure determination by neutron powder diffraction, Phys. B (Amsterdam, Neth.) 192, 55 (1993).
  54. Y. Xu, W. Löser, F. Tang, C. G. F. Blum, L. Liu, and B. Büchner, Crystal growth of the intermetallic compound Nd2PdSi3, Cryst. Res. Technol. 46, 135 (2011).
  55. K. Mukherjee, T. Basu, K. K. Iyer, and E. V. Sampathkumaran, 4f hybridization effect on the magnetism of Nd2PdSi3, Phys. Rev. B 84, 184415 (2011).
  56. J. Jensen and A. R. Mackintosh, Rare Earth Magnetism (Clarendon Press, Oxford, 1991).
  57. A. T. Boothroyd, Principles of Neutron Scattering from Condensed Matter (Oxford University Press, Oxford, UK, 2020).
  58. D. S. Inosov, D. V. Evtushinsky, A. Koitzsch, V. B. Zabolotnyy, S. V. Borisenko, A. A. Kordyuk, M. Frontzek, M. Loewenhaupt, W. Löser, I. Mazilu, H. Bitterlich, G. Behr, J.-U. Hoffmann, R. Follath, and B. Büchner, Electronic structure and nesting-driven enhancement of the RKKY interaction at the magnetic ordering propagation vector in Gd2PdSi3 and Tb2PdSi3, Phys. Rev. Lett. 102, 046401 (2009).
  59. M. Smidman, G. Balakrishnan, D. Le, D. Mayoh, E. V. Sampathkumaran, D. T. Adroja, Z. Shan, and V. Peçanha-Antonio, Spin-waves in Nd2PdSi3 with coexistent ferromagnetism and antiferromagnetism, STFC ISIS Neutron and Muon Source (2020), https://doi.org/10.5286/ISIS.E.RB2010616.
  60. M. Smidman, D. Le, D. Mayoh, D. T. Adroja, G. Balakrishnan, and Z. Shan, Spin-waves in Nd2PdSi3 with coexistent ferromagnetism and antiferromagnetism, STFC ISIS Neutron and Muon Source (2020), https://doi.org/10.5286/ISIS.E.RB2000180.
  61. V. Peçanha-Antonio, C. Balz, D. T. Adroja, Z. Shan, M. Smidman, and A. T. Boothroyd, Magnetic excitons in the frustrated topological Nd2PdSi3, STFC ISIS Neutron and Muon Source (2023), https://doi.org/10.5286/ISIS.E.RB2310234.
  62. V. Peçanha-Antonio, D. T. Adroja, N. A. Katcho, A. T. Boothroyd, B. Ouladdiaf, and M. Smidman, Magnetic structure of the frustrated, triangular-lattice metallic magnet Nd2PdSi3, Institut Laue-Langevin (ILL) (2023), https://doi.ill.fr/10.5291/ILL-DATA.5-41-1185.
  63. C. E. Patrick and J. B. Staunton, MARMOT: Magnetism, anisotropy, and more, using the relativistic disordered local moment picture at finite temperature, Electron. Struct. 4, 017001 (2022).
  64. M. Lüders, A. Ernst, M. Däne, Z. Szotek, A. Svane, D. Ködderitzsch, W. Hergert, B. L. Györffy, and W. M. Temmerman, Self-interaction correction in multiple scattering theory, Phys. Rev. B 71, 205109 (2005).
  65. M. Hoffmann, A. Ernst, W. Hergert, V. N. Antonov, W. A. Adeagbo, R. M. Geilhufe, and H. Ben Hamed, Magnetic and electronic properties of complex oxides from first-principles, Phys. Status Solidi B 257, 1900671 (2020).
  66. J. Bouaziz, G. Bihlmayer, C. E. Patrick, J. B. Staunton, and S. Blügel, Origin of incommensurate magnetic order in the RAlSi magnetic Weyl semimetals (R = Pr, Nd, Sm), Phys. Rev. B 109, L201108 (2024).

Outline

Information

Phys. Rev. B 114, 074421– Published 14 August, 2026
  • Received 21 April 2025
  • Revised 19 May 2026
  • Accepted 10 June 2026
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation