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

Visualizing bulk band structure in Fe4N thin films by spin- and angle-resolved photoelectron spectroscopy

Karen Nakanishi1,*, Masaaki Kakoki1,*, Kiyotaka Ohwada1, Kenta Kuroda1,2,3, Kazuki Sumida4,5, Hitoshi Sato5, Koji Miyamoto5, Taichi Okuda2,3,5, Shinji Isogami6,† et al.

Keisuke Masuda6,‡, Yuya Sakuraba6, and Akio Kimura1,2,3,7,§

  • 1Physics Program, Graduate School of Advanced Science and Engineering, Hiroshima University, 1-3-1 Kagamiyama, Higashi-Hiroshima 739-8526, Japan
  • 2International Institute for Sustainability with Knotted Chiral Meta Matter (WPI-SKCM2), 1-3-1 Kagamiyama, Higashi-Hiroshima 739-8531, Japan
  • 3Research Institute for Semiconductor Engineering, 1-4-2 Kagamiyama, Higashi-Hiroshima, Hiroshima 739-8527, Japan
  • 4Materials Sciences Research Center, Japan Atomic Energy Agency, Hyogo 679-5148, Japan
  • 5Research Institute for Synchrotron Radiation Science (HiSOR), Hiroshima University, 2-313 Kagamiyama, Higashi-Hiroshima 739-0046, Japan
  • 6National Institute for Materials Science, 1-2-1 Sengen, Tsukuba 305-0047, Japan
  • 7Synchrotron Radiation Research Center, National Institutes for Quantum Science and Technology (QST), Sayo, Hyogo, Japan

  • *These authors contributed equally to this work.
  • †Contact author: isogami.shinji@nims.go.jp
  • ‡Contact author: masuda.keisuke@nims.go.jp
  • §Contact author: akiok@hiroshima-u.ac.jp

Phys. Rev. Research 8, 023257 – Published 8 June, 2026

DOI: https://doi.org/10.1103/mlcy-gszb

Abstract

The bulk band structure of an in situ prepared ferromagnetic Fe4N thin film has been investigated using spin- and angle-resolved photoelectron spectroscopy with synchrotron radiation. It was observed that most of the bands near the Fermi level are of minority spin. The experimental results are well reproduced by first-principles calculations. Our orbital analysis of the band structure has revealed that the electron pocket near the Γ point is primarily attributed to the Fe 3dxy orbital of the Fe(II) site, while the electron pocket near the M point is associated with the Fe(II) 3dz2 orbital. Our observation of real band structure in Fe4N thin films could provide valuable insight into the properties of anisotropic magnetoresistance and anomalous Nernst effect.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (45)

  1. T. Miyazaki and N. Tezuka, Giant magnetic tunneling effect in Fe/Al2O3/Fe junction, J. Magn. Magn. Mater. 139, L231 (1995).
  2. J. S. Moodera, L. R. Kinder, T. M. Wong, and R. Meservey, Large magnetoresistance at room temperature in ferromagnetic thin film tunnel junctions, Phys. Rev. Lett. 74, 3273 (1995).
  3. S. Matsunaga, J. Hayakawa, S. Ikeda, K. Miura, H. Hasegawa, T. Endoh, H. Ohno, and T. Hanyu, Fabrication of a nonvolatile full adder based on logic-in-memory architecture using magnetic tunnel junctions, Appl. Phys. Express 1, 091301 (2008).
  4. S. I. Kiselev, J. C. Sankey, I. N. Krivorotov, N. C. Emley, R. J. Schoelkopf, R. A. Buhrman, and D. C. Ralph, Microwave oscillations of a nanomagnet driven by a spin-polarized current, Nature (London) 425, 380 (2003).
  5. S. Isogami and Y. K. Takahashi, Antiperovskite magnetic materials with 2p light elements for future practical applications, Adv. Electron. Mater. 9, 2200515 (2023).
  6. J. M. D. Coey, D. Givord, and D. Fruchart, Metallic nitride and carbide perovskites: History and prospects, ECS J. Solid State Sci. Technol. 11, 055002 (2022).
  7. Z. Zhang and W. Mi, Progress in ferrimagnetic Mn4N films and its heterostructures for spintronics applications, J. Phys. D: Appl. Phys. 55, 013001 (2022).
  8. K. Ito, S. Honda, and T. Suemasu, Transition metal nitrides and their mixed crystals for spintronics, Nanotechnology 33, 062001 (2022).
  9. S. Kokado, N. Fujima, K. Harigaya, H. Shimizu, and A. Sakuma, Theoretical analysis of highly spin-polarized transport in the iron nitride Fe4N, Phys. Rev. B 73, 172410 (2006).
  10. J. L. Costa-Krämer, D. M. Borsa, J. M. García-Martín, M. S. Martín-González, D. O. Boerma, and F. Briones, Structure and magnetism of single-phase epitaxial γ′−Fe4N, Phys. Rev. B 69, 144402 (2004).
  11. M. Kimura and S. Hasegawa, Growth evolution of γ′−Fe4N films on GaN(0001) and their interfacial structure, Jpn. J. Appl. Phys. 55, 05FD02 (2016).
  12. H. Chatbi, M. Vergnat, P. Bauer, and G. Marchal, Growth and characterization studies of Fe4N thin films prepared by ion beam assisted evaporation, Appl. Phys. Lett. 67, 430 (1995).
  13. K. R. Nikolaev, I. N. Krivorotov, E. D. Dahlberg, V. A. Vas’ko, S. Urazhdin, R. Loloee, and W. P. J. Pratt, Structural and magnetic properties of triode-sputtered epitaxial γ′−Fe4N films deposited on SrTiO3 (001) substrates, Appl. Phys. Lett. 82, 4534 (2003).
  14. L. L. Wang, X. Wang, W. T. Zheng, N. Ma, Q. F. Guan, J. Zhao, Y. Chen, and S. H. Feng, Synthesis of single nanocrystal phase γ′−Fe4N on NaCl substrate by DC magnetron sputtering, Mater. Chem. Phys. 100, 304 (2006).
  15. T. Ohgai, R. Shimono, H. Saitoh, and Y. Hayashi, Structure and soft magnetic properties of Fe–N thin films RF-sputtered on heated substrate, Mater. Trans. JIM 38, 503 (1997).
  16. L. L. Wang, W. T. Zheng, J. Gong, H. B. Li, X. Wang, N. Ma, P. J. Cao, and X. C. Ma, Investigation on the structure and magnetic properties at low temperature for nanocrystalline γ′−Fe4N thin films, J. Alloys Compd. 467, 1 (2009).
  17. Y. Na, C. Wang, J. Xiang, N. Ji, and J. Wang, Investigation of γ′−Fe4N thin films deposited on Si(100) and GaAs(100) substrates by facing target magnetron sputtering, J. Cryst. Growth 426, 117 (2015).
  18. N. Pandey, S. Pütter, S. M. Amir, V. R. Reddy, D. M. Phase, J. Stahn, A. Gupta, and M. Gupta, Effect of interfacial interdiffusion on magnetism in epitaxial Fe4N films on LaAlO3 substrates, Phys. Rev. Mater. 3, 114414 (2019).
  19. S. Nagakura, Electronic structure of iron nitrides studied by electron diffraction. I. γ′−Fe4N, J. Phys. Soc. Jpn. 25, 488 (1968).
  20. S. Matar, P. Mohn, G. Demazeau, and B. Siberchicot, The calculated electronic and magnetic structures of Fe4N and Mn4N, J. Phys. France 49, 1761 (1988).
  21. K. Sunaga, M. Tsunoda, K. Komagaki, Y. Uehara, and M. Takahashi, Inverse tunnel magnetoresistance in magnetic tunnel junctions with an Fe4N electrode, J. Appl. Phys. 102, 013917 (2007).
  22. Y. Komasaki, M. Tsunoda, S. Isogami, and M. Takahashi, 75% inverse magnetoresistance at room temperature in Fe4N/MgO/CoFeB magnetic tunnel junctions fabricated on Cu underlayer, J. Appl. Phys. 105, 07C928 (2009).
  23. S. Isogami, M. Tsunoda, Y. Komasaki, A. Sakuma, and M. Takahasi, Inverse current-induced magnetization switching in magnetic tunnel junctions with Fe4N free layer, Appl. Phys. Express 3, 103002 (2010).
  24. X. Li, H. Li, M. Jamali, and J.-P. Wang, Damping constant measurement and inverse giant magnetoresistance in spintronic devices with Fe4N, AIP Adv. 7, 125303 (2017).
  25. M. Tsunoda, H. Takahashi, S. Kokado, Y. Komasaki, A. Sakuma, and M. Takahashi, Anomalous anisotropic magnetoresistance in pseudo-single-crystal γ′−Fe4N films, Appl. Phys. Express 3, 113003 (2010).
  26. S. Isogami, K. Takanashi, and M. Mizuguchi, Dependence of anomalous Nernst effect on crystal orientation in highly ordered γ′−Fe4N films with anti-perovskite structure, Appl. Phys. Express 10, 073005 (2017).
  27. K. Ito, J. Wang, Y. Shimada, H. Sharma, M. Mizuguchi, and K. Takanashi, Enhancement of the anomalous Nernst effect in epitaxial Fe4N films grown on SrTiO3(001) substrates with oxygen deficient layers, J. Appl. Phys. 132, 133904 (2022).
  28. K. Kabara, M. Tsunoda, and S. Kokado, Anomalous Hall effects in pseudo-single-crystal γ′−Fe4N thin films, AIP Adv. 6, 055801 (2016).
  29. A. Damascelli, Z. Hussain, and Z.-X. Shen, Angle-resolved photoemission studies of the cuprate superconductors, Rev. Mod. Phys. 75, 473 (2003).
  30. K. Kabara, M. Tsunoda, and S. Kokado, Annealing effects on nitrogen site ordering and anisotropic magnetoresistance in pseudo-single-crystal γ′−Fe4N films, Appl. Phys. Express 7, 063003 (2014).
  31. T. Okuda, K. Miyamaoto, H. Miyahara, K. Kuroda, A. Kimura, H. Namatame, and M. Taniguchi, Efficient spin resolved spectroscopy observation machine at Hiroshima Synchrotron Radiation Center, Rev. Sci. Instrum. 82, 103302 (2011).
  32. T. Okuda, K. Miyamoto, A. Kimura, H. Namatame, and M. Taniguchi, A double VLEED spin detector for high-resolution three dimensional spin vectorial analysis of anisotropic Rashba spin splitting, J. Electron Spectrosc. Relat. Phenom. 201, 23 (2015).
  33. T. Okuda and A. Kimura, Spin- and angle-resolved photoemission of strongly spin–orbit coupled systems, J. Phys. Soc. Jpn. 82, 021002 (2013).
  34. See Supplemental Material at https://link.aps.org/supplemental/10.1103/mlcy-gszb for details of the experimental procedures, surface characterization (LEED and Auger electron spectroscopy (AES)), computational methods, and additional orbital-resolved band structure analysis, which includes Refs. [ [31, 32],S1–S4].
  35. S. Isogami, K. Masuda, Y. Miura, N. Rajamanickam, and Y. Sakuraba, Anomalous Hall and Nernst effects in ferrimagnetic Mn4N films: Possible interpretations and prospects for enhancement, Appl. Phys. Lett. 118, 092407 (2021).
  36. S. Isogami, M. Tsunoda, M. Oogane, A. Sakuma, and M. Takahashi, Dependence of magnetic damping on temperature and crystal orientation in epitaxial Fe4N thin films, J. Magn. Soc. Jpn. 38, 162 (2014).
  37. M. Fanciulli, J. Schusser, M.-I. Lee, Z. E. Youbi, O. Heckmann, M. C. Richter, C. Cacho, C. Spezzani, D. Bresteau, J.-F. Hergott, P. D’Oliveira, O. Tcherbakoff, T. Ruchon, J. Minár, and K. Hricovini, Spin, time, and angle resolved photoemission spectroscopy on WTe2, Phys. Rev. Res. 2, 013261 (2020).
  38. M. Schmitt, O. Kirilmaz, S. Chernov, S. Babenkov, D. Vasilyev, O. Fedchenko, K. Medjanik, Y. Matveyev, A. Gloskovskii, C. Schlueter, A. Winkelmann, L. Dudy, H.-J. Elmers, G. Schönhense, M. Sing, and R. Claessen, Bulk spin polarization of magnetite from spin-resolved hard x-ray photoelectron spectroscopy, Phys. Rev. B 104, 045129 (2021).
  39. Y. Wan, L. Wang, K. Kuroda, P. Zhang, K. Koshiishi, M. Suzuki, J. Kim, R. Noguchi, C. Bareille, K. Yaji, A. Harasawa, S. Shin, S.-W. Cheong, A. Fujimori, and T. Kondo, Selective observation of surface and bulk bands in polar WTe2 by laser-based spin- and angle-resolved photoemission spectroscopy, Phys. Rev. B 105, 085421 (2022).
  40. Y. Fukushima, K. Kawaguchi, K. Kuroda, M. Ochi, M. Hirayama, R. Mori, H. Tanaka, A. Harasawa, T. Iimori, Z. Zhao, S. Tani, K. Yaji, S. Shin, F. Komori, Y. Kobayashi, and T. Kondo, Spin-polarized saddle points in the topological surface states of elemental bismuth revealed by pump-probe spin- and angle-resolved photoemission spectroscopy, Phys. Rev. B 110, L041401 (2024).
  41. K. Miyamoto, K. Iori, K. Sakamoto, H. Narita, A. Kimura, M. Taniguchi, S. Qiao, K. Hasegawa, K. Shimada, H. Namatame, and S. Blügel, Spin polarized d surface resonance state of fcc Co/Cu(001), New J. Phys. 10, 125032 (2008).
  42. S. Hüfner, Photoelectron Spectroscopy: Principles and Applications, 3rd ed. (Springer, Berlin, 2003).
  43. J. J. Yeh and I. Lindau, Atomic subshell photoionization cross sections and asymmetry parameters: 1≤Z≤103, At. Data Nucl. Data Tables 32, 1 (1985).
  44. T. Valet and A. Fert, Theory of the perpendicular magnetoresistance in magnetic multilayers, Phys. Rev. B 48, 7099 (1993).
  45. S. Kokado, M. Tsunoda, K. Harigaya, and A. Sakuma, Anisotropic magnetoresistance effects in Fe, Co, Ni, Fe4N, and half-metallic ferromagnet: A systematic analysis, J. Phys. Soc. Jpn. 81, 024705 (2012).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation