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  • Letter
  • Open Access

Mid-infrared element-specific selective manipulation of the ultrafast magneto-optical Kerr effect dynamics in the ferrimagnet FeCr2S4

Davide Soranzio1,*, Matteo Savoini1, Fabian Graf1, Rafael T. Winkler1, Abhishek Nag2,3, Hiroki Ueda2,4, Kenya Ohgushi5, Yoshinori Tokura6,7, and Steven L. Johnson1,2,†

  • *Contact author: davideso@phys.ethz.ch
  • †Contact author: johnson@phys.ethz.ch
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Phys. Rev. Research 7, L042025 – Published 27 October, 2025

DOI: https://doi.org/10.1103/zn5y-vgkw

Abstract

FeCr2S4 is a ferrimagnet with two oppositely ordered spin sublattices (Fe and Cr), connected via superexchange interaction, giving a nonzero net magnetic moment. We show, using time-resolved measurements of the magneto-optic Kerr effect, how the magnetic dynamics of the sublattices can be selectively manipulated by resonantly perturbing the Fe sublattice with ultrashort laser pulses. The mid-infrared excitation through intra-atomic Fe d−d transitions triggers markedly slower dynamics in comparison to an off-resonant pumping affecting both of the two sublattices simultaneously. By changing probe wavelength to move in and out of resonance with the Fe d−d transitions, we also show the specific contributions of the Fe sublattice to these dynamics.

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References (36)

  1. S. Blundell, Magnetism in Condensed Matter, Oxford Master Series in Condensed Matter Physics 4 (OUP, Oxford, 2001).
  2. S. K. Kim, G. S. D. Beach, K.-J. Lee, T. Ono, T. Rasing, and H. Yang, Ferrimagnetic spintronics, Nat. Mater. 21, 24 (2022).
  3. H. Wu, F. Groß, B. Dai, D. Lujan, S. A. Razavi, P. Zhang, Y. Liu, K. Sobotkiewich, J. Förster, M. Weigand, G. Schütz, X. Li, J. Gräfe, and K. L. Wang, Ferrimagnetic skyrmions in topological insulator/ferrimagnet heterostructures, Adv. Mater. 32, 2003380 (2020).
  4. C. D. Stanciu, F. Hansteen, A. V. Kimel, A. Kirilyuk, A. Tsukamoto, A. Itoh, and T. Rasing, All-optical magnetic recording with circularly polarized light, Phys. Rev. Lett. 99, 047601 (2007).
  5. R. Ahrenkiel, T. Lee, S. Lyu, and F. Moser, Giant magneto-reflectance of CoCr2S4, Solid State Commun. 12, 1113 (1973).
  6. K. Ohgushi, T. Ogasawara, Y. Okimoto, S. Miyasaka, and Y. Tokura, Gigantic Kerr rotation induced by a d−d transition resonance in MCr2S4 (M = Mn, Fe), Phys. Rev. B 72, 155114 (2005).
  7. K. Ohgushi, Y. Okimoto, T. Ogasawara, S. Miyasaka, and Y. Tokura, Magnetic, optical, and magnetooptical properties of spinel-type ACr2X4 (A = Mn, Fe, Co, Cu, Zn, Cd; X = O, S, Se), J. Phys. Soc. Jpn. 77, 034713 (2008).
  8. V. Kocsis, S. Bordács, J. Deisenhofer, L. F. Kiss, K. Ohgushi, Y. Kaneko, Y. Tokura, and I. Kézsmárki, Strong magneto-optical effects in ACr2O4 (A = Fe, Co) spinel oxides generated by tetrahedrally coordinated transition metal ions, Phys. Rev. B 97, 125140 (2018).
  9. K. Sato and T. Ishibashi, Fundamentals of magneto-optical spectroscopy, Front. Phys. 10, 946515 (2022).
  10. B. Koopmans, M. van Kampen, and W. J. M. de Jonge, Experimental access to femtosecond spin dynamics, J. Phys.: Condens. Matter 15, S723 (2003).
  11. A. R. Khorsand, M. Savoini, A. Kirilyuk, A. V. Kimel, A. Tsukamoto, A. Itoh, and T. Rasing, Element-specific probing of ultrafast spin dynamics in multisublattice magnets with visible light, Phys. Rev. Lett. 110, 107205 (2013).
  12. A. Stupakiewicz, K. Szerenos, D. Afanasiev, A. Kirilyuk, and A. V. Kimel, Ultrafast nonthermal photo-magnetic recording in a transparent medium, Nature (London) 542, 71 (2017).
  13. R. V. Mikhaylovskiy, T. J. Huisman, V. A. Gavrichkov, S. I. Polukeev, S. G. Ovchinnikov, D. Afanasiev, R. V. Pisarev, T. Rasing, and A. V. Kimel, Resonant pumping of d−d crystal field electronic transitions as a mechanism of ultrafast optical control of the exchange interactions in iron oxides, Phys. Rev. Lett. 125, 157201 (2020).
  14. S. Mathias, C. La-O-Vorakiat, P. Grychtol, P. Granitzka, E. Turgut, J. M. Shaw, R. Adam, H. T. Nembach, M. E. Siemens, S. Eich, C. M. Schneider, T. J. Silva, M. Aeschlimann, M. M. Murnane, and H. C. Kapteyn, Probing the timescale of the exchange interaction in a ferromagnetic alloy, Proc. Natl. Acad. Sci. USA 109, 4792 (2012).
  15. E. Riedel, R. Karl, and R. Rackwitz, Mössbauer studies of thiospinels. V. The systems Cu1−xFexMe2S4 (Me = Cr, Rh) and Cu1−xFexCr2(S0.7Se0.3)4, J. Solid State Chem. 40, 255 (1981).
  16. Z. Chen, S. Tan, Z. Yang, and Y. Zhang, Evidence for a non-double-exchange mechanism in FeCr2S4, Phys. Rev. B 59, 11172 (1999).
  17. V. Tsurkan, V. Fritsch, J. Hemberger, H.-A. Krug von Nidda, N. Büttgen, D. Samusi, S. Körner, E.-W. Scheidt, S. Horn, R. Tidecks, and A. Loidl, Orbital fluctuations and orbital order in FeCr2S4, J. Phys. Chem. Solids 66, 2036 (2005).
  18. J. Bertinshaw, C. Ulrich, A. Günther, F. Schrettle, M. Wohlauer, S. Krohns, M. Reehuis, A. J. Studer, M. Avdeev, D. V. Quach, J. R. Groza, V. Tsurkan, A. Loidl, and J. Deisenhofer, FeCr2S4 in magnetic fields: Possible evidence for a multiferroic ground state, Sci. Rep. 4, 6079 (2014).
  19. J. Deisenhofer, F. Mayr, M. Schmidt, A. Loidl, and V. Tsurkan, Infrared-active phonons in the ferrimagnetic and multiferroic phases of FeCr2S4: Evidence for structural distortions, Phys. Rev. B 100, 144428 (2019).
  20. D. Maurer, V. Tsurkan, S. Horn, and R. Tidecks, Ultrasonic study of ferrimagnetic FeCr2S4: Evidence for low temperature structural transformations, J. Appl. Phys. 93, 9173 (2003).
  21. D. M. Evans, O. G. Grendal, L. Prodan, M. Winkler, N. Winterhalter-Stocker, P. Gegenwart, S. Ghara, J. Deisenhofer, I. Kézsmárki, and V. Tsurkan, Resolving structural changes and symmetry lowering in spinel FeCr2S4, Phys. Rev. B 105, 174107 (2022).
  22. L. Liu, Q. Yu, J. Xia, W. Shi, D. Wang, J. Wu, L. Xie, Y. Chen, and L. Jiao, 2D air-stable nonlayered ferrimagnetic FeCr2S4 crystals synthesized via chemical vapor deposition, Adv. Mater. 36, 2401338 (2024).
  23. S. Sarkar, M. De Raychaudhury, I. Dasgupta, and T. Saha-Dasgupta, Electronic structure of FeCr2S4: Evidence of Coulomb enhanced spin-orbit splitting, Phys. Rev. B 80, 201101 (2009).
  24. S. G. Chiuzbăian, S. Brignolo, C. F. Hague, R. Delaunay, M. Guarise, A. Nicolaou, Z. Yang, H. Zhou, and J.-M. Mariot, Spectroscopic evidence for superexchange in the ferrimagnetic spinel FeCr2S4, J. Phys. Chem. C 121, 22369 (2017).
  25. T. Ogasawara, K. Ohgushi, H. Okamoto, and Y. Tokura, Photoinduced dynamics of sublattice magnetization in ferrimagnets: FeCr2S4 and CoCr2S4, J. Phys. Soc. Jpn. 75, 083707 (2006).
  26. K. Momma and F. Izumi, VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data, J. Appl. Crystallogr. 44, 1272 (2011).
  27. R. P. Stapele, J. S. van Wieringen, and P. F. Bongers, Strong anisotropy in the cubic ferrimagnet FeCr2S4, J. Phys. (Paris) 32, 53 (1971).
  28. See Supplemental Material at http://link.aps.org/supplemental/10.1103/zn5y-vgkw for additional details on beam spot sizes, out-of-equilibrium hystereses, Fourier transform of the oscillatory response, ellipticity, and reflectivity dynamics, and which includes Refs. [34, 35, 36].
  29. Z. Vardeny and J. Tauc, Picosecond coherence coupling in the pump and probe technique, Opt. Commun. 39, 396 (1981).
  30. S. T. Cundiff, Coherent spectroscopy of semiconductors, Opt. Express 16, 4639 (2008).
  31. J. Xu, A. Habib, R. Sundararaman, and Y. Ping, Ab initio ultrafast spin dynamics in solids, Phys. Rev. B 104, 184418 (2021).
  32. A. L. Chekhov, Y. Behovits, J. J. F. Heitz, C. Denker, D. A. Reiss, M. Wolf, M. Weinelt, P. W. Brouwer, M. Münzenberg, and T. Kampfrath, Ultrafast demagnetization of iron induced by optical versus terahertz pulses, Phys. Rev. X 11, 041055 (2021).
  33. D. Soranzio, https://doi.org/10.3929/ethz-b-000722091, (2025).
  34. D. Soranzio, M. Peressi, R. J. Cava, F. Parmigiani, and F. Cilento, Ultrafast broadband optical spectroscopy for quantifying subpicometric coherent atomic displacements in WTe2, Phys. Rev. Res. 1, 032033 (2019).
  35. R. Trebino, Frequency-Resolved Optical Gating: The Measurement of Ultrashort Laser Pulses (Springer US, New York, NY, 2000).
  36. M. Jovičević-Klug, P. Jovičević-Klug, J. McCord, and B. Podgornik, Investigation of microstructural attributes of steel surfaces through magneto-optical Kerr effect, J. Mater. Res. Technol. 11, 1245 (2021).

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Phys. Rev. Research 7, L042025– Published 27 October, 2025
  • Received 17 February 2025
  • Accepted 25 September 2025
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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.

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