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
  • Editors' Suggestion
  • Letter
  • Open Access

Generation of phonons with angular momentum during ultrafast demagnetization

M. S. Mrudul1,*, Markus Weißenhofer1,2, and Peter M. Oppeneer1,†

  • *Contact author: mrudul.muraleedharan@physics.uu.se
  • †Contact author: peter.oppeneer@physics.uu.se

Phys. Rev. B 112, L180407 – Published 19 November, 2025

DOI: https://doi.org/10.1103/nt8w-47hb

Abstract

A major question in the field of femtosecond laser-induced demagnetization is whereto the angular momentum lost by the electrons is transferred. Recent ultrafast electron diffraction measurements [Tauchert et al., Nature (London) 602, 73 (2022)] suggest that this angular momentum is transferred to the rotational motion of atoms on a sub-picosecond timescale, but a theory confirmation of this proposition has yet to be given. Here, we investigate the coupled electron-nuclear dynamics during ultrafast demagnetization of L10 FePt, using Ehrenfest nuclear dynamics simulations combined with the time-dependent density functional theory (TDDFT) framework. We demonstrate that atomic rotations appear, i.e., the generation of phonons carrying finite angular momentum following ultrafast demagnetization. We further show that both ultrafast demagnetization and the generation of phonons with angular momentum arise from symmetry constraints imposed by the spin-orbit coupling, thus providing insight in spin-phonon interaction at ultrafast timescales.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (67)

  1. E. Beaurepaire, J.-C. Merle, A. Daunois, and J.-Y. Bigot, Ultrafast spin dynamics in ferromagnetic nickel, Phys. Rev. Lett. 76, 4250 (1996).
  2. J. Hohlfeld, E. Matthias, R. Knorren, and K. H. Bennemann, Nonequilibrium magnetization dynamics of nickel, Phys. Rev. Lett. 78, 4861 (1997).
  3. A. Scholl, L. Baumgarten, R. Jacquemin, and W. Eberhardt, Ultrafast spin dynamics of ferromagnetic thin films observed by fs spin-resolved two-photon photoemission, Phys. Rev. Lett. 79, 5146 (1997).
  4. A. Kirilyuk, A. V. Kimel, and T. Rasing, Ultrafast optical manipulation of magnetic order, Rev. Mod. Phys. 82, 2731 (2010).
  5. K. Carva, P. Baláž, and I. Radu, Laser-induced ultrafast magnetic phenomena, in Handbook of Magnetic Materials, edited by E. Brück (Elsevier, Amsterdam, 2017), Vol. 26, pp. 291–463.
  6. G. P. Zhang and W. Hübner, Laser-induced ultrafast demagnetization in ferromagnetic metals, Phys. Rev. Lett. 85, 3025 (2000).
  7. M. Cinchetti, M. Sánchez Albaneda, D. Hoffmann, T. Roth, J.-P. Wüstenberg, M. Krauß, O. Andreyev, H. C. Schneider, M. Bauer, and M. Aeschlimann, Spin-flip processes and ultrafast magnetization dynamics in Co: Unifying the microscopic and macroscopic view of femtosecond magnetism, Phys. Rev. Lett. 97, 177201 (2006).
  8. E. Carpene, E. Mancini, C. Dallera, M. Brenna, E. Puppin, and S. De Silvestri, Dynamics of electron-magnon interaction and ultrafast demagnetization in thin iron films, Phys. Rev. B 78, 174422 (2008).
  9. B. Koopmans, G. Malinowski, F. Dalla Longa, D. Steiauf, M. Fähnle, T. Roth, M. Cinchetti, and M. Aeschlimann, Explaining the paradoxical diversity of ultrafast laser-induced demagnetization, Nat. Mater. 9, 259 (2010).
  10. M. Battiato, K. Carva, and P. M. Oppeneer, Superdiffusive spin transport as a mechanism of ultrafast demagnetization, Phys. Rev. Lett. 105, 027203 (2010).
  11. A. J. Schellekens and B. Koopmans, Comparing ultrafast demagnetization rates between competing models for finite temperature magnetism, Phys. Rev. Lett. 110, 217204 (2013).
  12. B. Y. Mueller, A. Baral, S. Vollmar, M. Cinchetti, M. Aeschlimann, H. Schneider, and B. Rethfeld, Feedback effect during ultrafast demagnetization dynamics in ferromagnets, Phys. Rev. Lett. 111, 167204 (2013).
  13. E. Carpene, H. Hedayat, F. Boschini, and C. Dallera, Ultrafast demagnetization of metals: Collapsed exchange versus collective excitations, Phys. Rev. B 91, 174414 (2015).
  14. K. Krieger, J. K. Dewhurst, P. Elliott, S. Sharma, and E. K. U. Gross, Laser-induced demagnetization at ultrashort time scales: Predictions of TDDFT, J. Chem. Theory Comput. 11, 4870 (2015).
  15. E. Turgut, D. Zusin, D. Legut, K. Carva, R. Knut, J. M. Shaw, C. Chen, Z. Tao, H. T. Nembach, T. J. Silva et al., Stoner versus Heisenberg: Ultrafast exchange reduction and magnon generation during laser-induced demagnetization, Phys. Rev. B 94, 220408 (2016).
  16. S. R. Acharya, V. Turkowski, G. P. Zhang, and T. S. Rahman, Ultrafast electron correlations and memory effects at work: Femtosecond demagnetization in Ni, Phys. Rev. Lett. 125, 017202 (2020).
  17. P. Scheid, Q. Remy, S. Lebègue, G. Malinowski, and S. Mangin, Light induced ultrafast magnetization dynamics in metallic compounds, J. Magn. Magn. Mater. 560, 169596 (2022).
  18. M. Weißenhofer and P. M. Oppeneer, Ultrafast demagnetization through femtosecond generation of non-thermal magnons, Adv. Phys. Res. 4, 2300103 (2024).
  19. A. Einstein and W. J. de Haas, Experimental proof of the existence of Ampère's molecular currents, in Proceedings of the Royal Netherlands Academy of Arts and Sciences (KNAW) (Digital Library, Amsterdam, 1915), Vol. 18, pp. 696–711.
  20. K. Carva, M. Battiato, D. Legut, and P. M. Oppeneer, Ab initio theory of electron-phonon mediated ultrafast spin relaxation of laser-excited hot electrons in transition-metal ferromagnets, Phys. Rev. B 87, 184425 (2013).
  21. T. Griepe and U. Atxitia, Evidence of electron-phonon mediated spin flip as driving mechanism for ultrafast magnetization dynamics in 3d ferromagnets, Phys. Rev. B 107, L100407 (2023).
  22. S. Essert and H. C. Schneider, Electron-phonon scattering dynamics in ferromagnetic metals and their influence on ultrafast demagnetization processes, Phys. Rev. B 84, 224405 (2011).
  23. C. Illg, M. Haag, and M. Fähnle, Ultrafast demagnetization after laser irradiation in transition metals: Ab initio Calculations of the spin-flip electron-phonon scattering with reduced exchange splitting, Phys. Rev. B 88, 214404 (2013).
  24. D. A. Garanin and E. M. Chudnovsky, Angular momentum in spin-phonon processes, Phys. Rev. B 92, 024421 (2015).
  25. J. Holanda, D. Maior, A. Azevedo, and S. Rezende, Detecting the phonon spin in magnon–phonon conversion experiments, Nat. Phys. 14, 500 (2018).
  26. S. Eich, M. Plötzing, M. Rollinger, S. Emmerich, R. Adam, C. Chen, H. C. Kapteyn, M. M. Murnane, L. Plucinski, D. Steil, B. Stadtmüller, M. Cinchetti, M. Aeschlimann, C. M. Schneider, and S. Mathias, Band structure evolution during the ultrafast ferromagnetic-paramagnetic phase transition in cobalt, Sci. Adv. 3, e1602094 (2017).
  27. C. Dornes, Y. Acremann, M. Savoini, M. Kubli, M. J. Neugebauer, E. Abreu, L. Huber, G. Lantz, C. A. F. Vaz, H. Lemke, E. M. Bothschafter, M. Porer, V. Esposito, L. Rettig, M. Buzzi, A. Alberca, Y. W. Windsor, P. Beaud, U. Staub, D. Zhu et al., The ultrafast Einstein–de Haas effect, Nature (London) 565, 209 (2019).
  28. S. R. Tauchert, M. Volkov, D. Ehberger, D. Kazenwadel, M. Evers, H. Lange, A. Donges, A. Book, W. Kreuzpaintner, U. Nowak, and P. Baum, Polarized phonons carry angular momentum in ultrafast demagnetization, Nature (London) 602, 73 (2022).
  29. L. Zhang and Q. Niu, Angular momentum of phonons and the Einstein–de Haas effect, Phys. Rev. Lett. 112, 085503 (2014).
  30. Y. Ren, C. Xiao, D. Saparov, and Q. Niu, Phonon magnetic moment from electronic topological magnetization, Phys. Rev. Lett. 127, 186403 (2021).
  31. D. Shin, H. Hübener, U. De Giovannini, H. Jin, A. Rubio, and N. Park, Phonon-driven spin-floquet magneto-valleytronics in MoS2, Nat. Commun. 9, 638 (2018).
  32. J. Cui, E. V. Boström, M. Ozerov, F. Wu, Q. Jiang, J.-H. Chu, C. Li, F. Liu, X. Xu, A. Rubio, and Q. Zhang, Chirality selective magnon-phonon hybridization and magnon-induced chiral phonons in a layered zigzag antiferromagnet, Nat. Commun. 14, 3396 (2023).
  33. J. Luo, T. Lin, J. Zhang, X. Chen, E. R. Blackert, R. Xu, B. I. Yakobson, and H. Zhu, Large effective magnetic fields from chiral phonons in rare-earth halides, Science 382, 698 (2023).
  34. C. S. Davies, F. G. N. Fennema, A. Tsukamoto, I. Razdolski, A. V. Kimel, and A. Kirilyuk, Phononic switching of magnetization by the ultrafast Barnett effect, Nature (London) 628, 540 (2024).
  35. D. M. Juraschek and N. A. Spaldin, Orbital magnetic moments of phonons, Phys. Rev. Mater. 3, 064405 (2019).
  36. M. Weißenhofer, P. Rieger, M. S. Mrudul, L. Mikadze, U. Nowak, and P. M. Oppeneer, Chiral phonons arising from chirality-selective magnon-phonon coupling, Phys. Rev. Lett. 135, 216701 (1990).
  37. S. De Silvestri Jr., J. Fujimoto, E. Ippen, E. B. Gamble Jr, L. R. Williams, and K. A. Nelson, Femtosecond time-resolved measurements of optic phonon dephasing by impulsive stimulated Raman scattering in α-perylene crystal from 20 to 300 K, Chem. Phys. Lett. 116, 146 (1985).
  38. K. Ishioka, M. Hase, M. Kitajima, and H. Petek, Coherent optical phonons in diamond, Appl. Phys. Lett. 89, 231916 (2006).
  39. G. C. Cho, W. Kütt, and H. Kurz, Subpicosecond time-resolved coherent-phonon oscillations in GaAs, Phys. Rev. Lett. 65, 764 (1990).
  40. A. Melnikov, I. Radu, U. Bovensiepen, O. Krupin, K. Starke, E. Matthias, and M. Wolf, Coherent optical phonons and parametrically coupled magnons induced by femtosecond laser excitation of the Gd (0001) surface, Phys. Rev. Lett. 91, 227403 (2003).
  41. Y. Shinohara, K. Yabana, Y. Kawashita, J.-I. Iwata, T. Otobe, and G. F. Bertsch, Coherent phonon generation in time-dependent density functional theory, Phys. Rev. B 82, 155110 (2010).
  42. M. Hase, K. Ishioka, J. Demsar, K. Ushida, and M. Kitajima, Ultrafast dynamics of coherent optical phonons and nonequilibrium electrons in transition metals, Phys. Rev. B 71, 184301 (2005).
  43. T. Henighan, M. Trigo, S. Bonetti, P. Granitzka, D. Higley, Z. Chen, M. P. Jiang, R. Kukreja, A. Gray, A. H. Reid, E. Jal, M. C. Hoffmann, M. Kozina, S. Song, M. Chollet, D. Zhu, P. F. Xu, J. Jeong, K. Carva, P. Maldonado et al., Generation mechanism of terahertz coherent acoustic phonons in Fe, Phys. Rev. B 93, 220301 (2016).
  44. C. A. Ullrich, Time-Dependent Density-Functional Theory – Concepts and Applications (Oxford University Press, Oxford, 2011).
  45. M. A. L. Marques, N. T. Maitra, F. M. S. Nogueira, E. K. U. Gross, and A. Rubio, Fundamentals of Time-Dependent Density Functional Theory (Springer, Berlin, Heidelberg, 2012), Vol. 837.
  46. J. P. Perdew and A. Zunger, Self-interaction correction to density-functional approximations for many-electron systems, Phys. Rev. B 23, 5048 (1981).
  47. C. Hartwigsen, S. Gœdecker, and J. Hutter, Relativistic separable dual-space Gaussian pseudopotentials from H to Rn, Phys. Rev. B 58, 3641 (1998).
  48. X. Andrade, A. Castro, D. Zueco, J. L. Alonso, P. Echenique, F. Falceto, and A. Rubio, Modified Ehrenfest formalism for efficient large-scale ab initio molecular dynamics, J. Chem. Theory Comput. 5, 728 (2009).
  49. N. Tancogne-Dejean, M. J. T. Oliveira, X. Andrade, H. Appel, C. H. Borca, G. Le Breton, F. Buchholz, A. Castro, S. Corni, A. A. Correa et al., Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems, J. Chem. Phys. 152, 124119 (2020).
  50. P. Maldonado, K. Carva, M. Flammer, and P. M. Oppeneer, Theory of out-of-equilibrium ultrafast relaxation dynamics in metals, Phys. Rev. B 96, 174439 (2017).
  51. P. M. Oppeneer, Magneto-optical spectroscopy in the valence-band energy regime: Relationship to the magnetocrystalline anisotropy, J. Magn. Magn. Mater. 188, 275 (1998).
  52. M. S. Mrudul and P. M. Oppeneer, Ab initio investigation of laser-induced ultrafast demagnetization of L10 FePt: Intensity dependence and importance of electron coherence, Phys. Rev. B 109, 144418 (2024).
  53. P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo et al., quantum espresso: A modular and open-source software project for quantum simulations of materials, J. Phys.: Condens. Matter 21, 395502 (2009).
  54. P. Giannozzi Jr, O. Andreussi, T. Brumme, O. Bunau, M. B. Nardelli, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, M. Cococcioni et al., Advanced capabilities for materials modeling with quantum espresso, J. Phys.: Condens. Matter 29, 465901 (2017).
  55. G. P. Zhang and Y. H. Bai, Laser-induced forces on atoms during ultrafast demagnetization, J. Magn. Magn. Mater. 563, 169885 (2022).
  56. N. Tancogne-Dejean, F. G. Eich, and A. Rubio, Effect of spin-orbit coupling on the high harmonics from the topological Dirac semimetal Na3Bi, npj Comput. Mater. 8, 145 (2022).
  57. M. S. Dresselhaus, G. Dresselhaus, and A. Jorio, Group Theory: Application to the Physics of Condensed Matter (Springer Science & Business Media, Berlin, Heidelberg, 2007).
  58. The space group and magnetic space group of L10 FePt are P4/mmm and P4/mm′m′, respectively. The primed notation (m→m′) indicates that two reflection planes are coupled with the spin-reversal operator.
  59. A. Abedi, N. T. Maitra, and E. K. Gross, Exact factorization of the time-dependent electron-nuclear wave function, Phys. Rev. Lett. 105, 123002 (2010).
  60. Q. Zhang and B. Wu, General approach to quantum-classical hybrid systems and geometric forces, Phys. Rev. Lett. 97, 190401 (2006).
  61. N. Wu, S. Zhang, D. Chen, Y. Wang, and S. Meng, Three-stage ultrafast demagnetization dynamics in a monolayer ferromagnet, Nat. Commun. 15, 2804 (2024).
  62. S. Sharma, S. Shallcross, P. Elliott, and J. K. Dewhurst, Making a case for femto-phono-magnetism with FePt, Sci. Adv. 8, eabq2021 (2022).
  63. C. Strohm, G. L. J. A. Rikken, and P. Wyder, Phenomenological evidence for the phonon Hall effect, Phys. Rev. Lett. 95, 155901 (2005).
  64. L. Zhang and Q. Niu, Chiral phonons at high-symmetry points in monolayer hexagonal lattices, Phys. Rev. Lett. 115, 115502 (2015).
  65. H. Chen, W. Zhang, Q. Niu, and L. Zhang, Chiral phonons in two-dimensional materials, 2D Mater. 6, 012002 (2018).
  66. S. Park and B.-J. Yang, Phonon angular momentum Hall effect, Nano Lett. 20, 7694 (2020).
  67. M. S. Mrudul, M. Weißenhofer, and P. M. Oppeneer, Generation of phonons with angular momentum during ultrafast demagnetization [Data set], Zenodo (2025), https://doi.org/10.5281/zenodo.17522581.

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation