- 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

Pulsed magnetophononics in gapped quantum magnets

B. Demazure1,2,*, M. Krebs3, G. S. Uhrig3, and B. Normand1

  • *Contact author: baptiste.demazure@psi.ch
PDF

Phys. Rev. B 112, 075112 – Published 6 August, 2025

DOI: https://doi.org/10.1103/4ddn-y88c

Abstract

One route to the control of quantum magnetism at ultrafast timescales is magnetophononics, the modulation of magnetic interactions by coherently driven lattice excitations. Theoretical studies of a gapped quantum magnet subject to continuous, single-frequency driving of one strongly coupled phonon mode find intriguing phenomena including mutually repelling phonon-bitriplon excitations and global renormalization of the spin excitation spectrum. Because experiments are performed with ultrashort pulses that contain a wide range of driving frequencies, we investigate phonon-bitriplon physics under pulsed laser driving. We use the equations of motion to compute the transient response of the driven and dissipative spin-phonon system, which we characterize using the phonon displacement, phonon number, and triplon occupations. In the Fourier transforms of each quantity we discover a low-frequency energetic oscillation between the lattice and spin sectors, which is an intrinsically nonequilibrium collective mode, and demonstrate its origin as a beating between mutually repelling composite excitations. We introduce a phonon-bitriplon approximation that captures all the physics of hybridization, collective mode formation, and difference-frequency excitation, and show that sum-frequency phenomena also leave clear signatures in the response. We model the appearance of such magnetophononic phenomena in the strongly coupled spin-chain compound CuGeO3, whose overlapping phonon and spin excitation spectra are well characterized, to deduce the criteria for their possible observation in quantum magnetic materials.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (54)

  1. T. Kampfrath, K. Tanaka, and K. A. Nelson, Resonant and nonresonant control over matter and light by intense terahertz transients, Nat. Photon. 7, 680 (2013).
  2. X. C. Zhang, A. Shkurinov, and Y. Zhang, Extreme terahertz science, Nat. Photon. 11, 16 (2017).
  3. P. Salén, M. Basini, S. Bonetti, J. Hebling, M. Krasilnikov, A. Y. Nikitin, G. Shamuilov, Z. Tibai, V. Zhaunerchyk, and V. Goryashko, Matter manipulation with extreme terahertz light: Progress in the enabling THz technology, Phys. Rep. 836-837, 1 (2019).
  4. A. Cavalleri, Photo-induced superconductivity, Contemp. Phys. 59, 31 (2018).
  5. Y. Murakami, D. Golež, M. Eckstein, and P. Werner, Photo-induced nonequilibrium states in Mott insulators, arXiv:2310.05201.
  6. T. Oka and S. Kitamura, Floquet engineering of quantum materials, Annu. Rev. Condens. Matter Phys. 10, 387 (2019).
  7. A. S. Disa, T. F. Nova, B. Liu, and A. Cavalleri, Engineering crystal structures with light, Nat. Phys. 17, 1087 (2021).
  8. A. de la Torre, D. M. Kennes, M. Claassen, S. Gerber, J. W. McIver, and M. A. Sentef, Nonthermal pathways to ultrafast control in quantum materials, Rev. Mod. Phys. 93, 041002 (2021).
  9. T. Kampfrath, A. Sell, G. Klatt, A. Pashkin, S. Mährlein, T. Dekorsy, M. Wolf, M. Fiebig, A. Leitenstorfer, and R. Huber, Coherent terahertz control of antiferromagnetic spin waves, Nat. Photon. 5, 31 (2011).
  10. T. Kubacka, J. A. Johnson, M. C. Hoffmann, C. Vicario, S. de Jong, P. Beaud, S. Grübel, S.-W. Huang, L. Huber, L. Patthey et al., Large-amplitude spin dynamics driven by a THz pulse in resonance with an electromagnon, Science 343, 1333 (2014).
  11. S. Baierl, M. Hohenleutner, T. Kampfrath, A. K. Zvezdin, A. V. Kimel, R. Huber, and R. V. Mikhaylovskiy, Nonlinear spin control by terahertz-driven anisotropy fields, Nat. Photon. 10, 715 (2016).
  12. J. Lu, X. Li, H. Y. Hwang, B. K. Ofori-Okai, T. Kurihara, T. Suemoto, and K. A. Nelson, Coherent two-dimensional terahertz magnetic resonance spectroscopy of collective spin waves, Phys. Rev. Lett. 118, 207204 (2017).
  13. E. A. Mashkovich, K. A. Grishunin, R. V. Mikhaylovskiy, A. K. Zvezdin, R. V. Pisarev, M. B. Strugatsky, P. C. M. Christianen, T. Rasing, and A. V. Kimel, Terahertz optomagnetism: nonlinear THz excitation of GHz spin waves in antiferromagnetic FeBO3, Phys. Rev. Lett. 123, 157202 (2019).
  14. Y. Behovits, A. L. Chekhov, S. Y. Bodnar, O. Gueckstock, S. Reimers, Y. Lytvynenko, Y. Skourski, M. Wolf, T. S. Seifert, O. Gomonay et al., Terahertz Néel spin-orbit torques drive nonlinear magnon dynamics in antiferromagnetic Mn2Au, Nat. Commun. 14, 6038 (2023).
  15. A. Khudoyberdiev and G. S. Uhrig, Switching of magnetization in quantum antiferromagnets with time-dependent control fields, Phys. Rev. B 109, 174419 (2024).
  16. J. Walowski and M. Münzenberg, Perspective: Ultrafast magnetism and THz spintronics, J. Appl. Phys. 120, 140901 (2016).
  17. P. Němec, M. Fiebig, T. Kampfrath, and A. V. Kimel, Antiferromagnetic opto-spintronics, Nat. Phys. 14, 229 (2018).
  18. P. Pirro, V. I. Vasyuchka, A. A. Serga, and B. Hillebrands, Advances in coherent magnonics, Nat. Rev. Mater. 6, 1114 (2021).
  19. C. Broholm, R. J. Cava, S. A. Kivelson, D. G. Nocera, M. R. Norman, and T. Senthil, Quantum spin liquids, Science 367, eaay0668 (2020).
  20. T. F. Nova, A. Cartella, A. Cantaluppi, M. Först, D. Bossini, R. V. Mikhaylovskiy, A. V. Kimel, R. Merlin, and A. Cavalleri, An effective magnetic field from optically driven phonons, Nat. Phys. 13, 132 (2017).
  21. M. Kozina, M. Fechner, P. Marsik, T. van Driel, J. M. Glownia, C. Bernhard, M. Radovic, D. Zhu, S. Bonetti, U. Staub, and M. C. Hoffmann, Terahertz-driven phonon upconversion in SrTiO3, Nat. Phys. 15, 387 (2019).
  22. M. Fechner, A. Sukhov, L. Chotorlishvili, C. Kenel, J. Berakdar, and N. A. Spaldin, Magnetophononics: Ultrafast spin control through the lattice, Phys. Rev. Mater. 2, 064401 (2018).
  23. D. M. Juraschek, P. Narang, and N. A. Spaldin, Phono-magnetic analogs to opto-magnetic effects, Phys. Rev. Res. 2, 043035 (2020).
  24. M. Yarmohammadi, M. Krebs, G. S. Uhrig, and B. Normand, Strong-coupling magnetophononics: Self-blocking, phonon-bitriplons, and spin-band engineering, Phys. Rev. B 107, 174415 (2023).
  25. F. Giorgianni, B. Wehinger, S. Allenspach, N. Colonna, C. Vicario, P. Puphal, E. Pomjakushina, B. Normand, and C. Rüegg, Ultrafast frustration breaking and magnetophononic driving of singlet excitations in a quantum magnet, Phys. Rev. B 107, 184440 (2023).
  26. A. S. Disa, M. Fechner, T. F. Nova, B. Liu, M. Först, D. Prabhakaran, P. G. Radaelli, and A. Cavalleri, Polarizing an antiferromagnet by optical engineering of the crystal field, Nat. Phys. 16, 937 (2020).
  27. D. Afanasiev, J. R. Hortensius, B. A. Ivanov, A. Sasani, E. Bousquet, Y. M. Blanter, R. V. Mikhaylovskiy, A. V. Kimel, and A. D. Caviglia, Ultrafast control of magnetic interactions via light-driven phonons, Nat. Mater. 20, 607 (2021).
  28. E. A. Mashkovich, K. A. Grishunin, R. M. Dubrovin, A. K. Zvezdin, R. V. Pisarev, and A. V. Kimel, Terahertz light–driven coupling of antiferromagnetic spins to lattice, Science 374, 1608 (2021).
  29. D. Bossini, S. D. Conte, M. Terschanski, G. Springholz, A. Bonanni, K. Deltenre, F. Anders, G. S. Uhrig, G. Cerullo, and M. Cinchetti, Femtosecond phononic coupling to both spins and charges in a room-temperature antiferromagnetic semiconductor, Phys. Rev. B 104, 224424 (2021).
  30. M. Yarmohammadi, C. Meyer, B. Fauseweh, B. Normand, and G. S. Uhrig, Dynamical properties of a driven dissipative dimerized S=1/2 chain, Phys. Rev. B 103, 045132 (2021).
  31. M. Hase, I. Terasaki, and K. Uchinokura, Observation of the spin-Peierls transition in linear Cu2+ (spin-1/2) chains in an inorganic compound CuGeO3, Phys. Rev. Lett. 70, 3651 (1993).
  32. Z. V. Popović, S. D. Dević, V. N. Popov, G. Dhalenne, and A. Revcolevschi, Phonons in CuGeO3 studied using polarized far-infrared and Raman-scattering spectroscopies, Phys. Rev. B 52, 4185 (1995).
  33. M. Braden, B. Hennion, W. Reichardt, G. Dhalenne, and A. Revcolevschi, Spin-phonon coupling in CuGeO3, Phys. Rev. Lett. 80, 3634 (1998).
  34. M. Braden, W. Reichardt, B. Hennion, G. Dhalenne, and A. Revcolevschi, Lattice dynamics of CuGeO3: Inelastic neutron scattering and model calculations, Phys. Rev. B 66, 214417 (2002).
  35. L. P. Regnault, M. Aïn, B. Hennion, G. Dhalenne, and A. Revcolevschi, Inelastic neutron scattering investigation of the spin-Peierls system CuGeO3, Phys. Rev. B 53, 5579 (1996).
  36. G. S. Uhrig, Symmetry and dimension of the dispersion of inorganic spin-Peierls systems, Phys. Rev. Lett. 79, 163 (1997).
  37. S. Sachdev and R. N. Bhatt, Bond-operator representation of quantum spins: Mean-field theory of frustrated quantum Heisenberg antiferromagnets, Phys. Rev. B 41, 9323 (1990).
  38. S. Gopalan, T. M. Rice, and M. Sigrist, Spin ladders with spin gaps: A description of a class of cuprates, Phys. Rev. B 49, 8901 (1994).
  39. B. Normand and C. Rüegg, Complete bond-operator theory of the two-chain spin ladder, Phys. Rev. B 83, 054415 (2011).
  40. H.-P. Breuer and F. Petruccione, The Theory of Open Quantum Systems (Oxford University Press, Oxford, 2007).
  41. U. Weiss, Quantum Dissipative Systems, 5th ed. (World Scientific, Singapore, 2021).
  42. G. Lindblad, On the generators of quantum dynamical semigroups, Commun. Math. Phys. 48, 119 (1976).
  43. D. Giavazzi, F. di Maiolo, and A. Painelli, The fate of molecular excited states: Modeling donor–acceptor dyes, Phys. Chem. Chem. Phys. 24, 5555 (2022).
  44. J. Bezanson, A. Edelman, S. Karpinski, and V. B. Shah, Julia: A fresh approach to numerical computing, SIAM Rev. 59, 65 (2017).
  45. P. Virtanen, R. Gommers, T. E. Oliphant, M. Haberland, T. Reddy, D. Cournapeau, E. Burovski, P. Peterson, W. Weckesser, J. Bright, and SciPy 1.0 Contributors, SciPy 1.0: Fundamental algorithms for scientific computing in Python, Nat. Methods 17, 261 (2020).
  46. C. Gros and R. Werner, Dynamics of the Peierls-active phonon modes in CuGeO3, Phys. Rev. B 58, R14677 (1998).
  47. K. Takehana, T. Takamasu, M. Hase, G. Kido, and K. Uchinokura, Far-infrared spectroscopy in the spin-Peierls compound CuGeO3 under high magnetic fields, Phys. Rev. B 62, 5191 (2000).
  48. L. Spitz, A. Razpopov, S. Biswas, H. Lane, S. E. Nikitin, K. Iida, R. Kajimoto, M. Fujita, M. Arai, M. Mourigal, C. Rüegg, R. Valentí, and B. Normand, Phonon spectrum in the spin-Peierls phase of CuGeO3, arXiv:2507.12409.
  49. C. Knetter and G. S. Uhrig, Triplet dispersion in CuGeO3: Perturbative analysis, Phys. Rev. B 63, 094401 (2001).
  50. R. Werner, C. Gros, and M. Braden, Microscopic spin-phonon coupling constants in CuGeO3, Phys. Rev. B 59, 14356 (1999).
  51. S. Feldkemper and W. Weber, Superexchange via cluster states: Calculation of spin-phonon coupling constants for CuGeO3, Phys. Rev. B 62, 3816 (2000).
  52. C. Rackauckas and Q. Nie, DifferentialEquations.jl–A performant and feature-rich ecosystem for solving differential equations in julia, J. Open Res. Softw. 5, 15 (2017).
  53. A. Liu, Multidimensional terahertz probes of quantum materials, npj Quant. Mater. 10, 18 (2025).
  54. B. Demazure, M. Krebs, G. Uhrig, and B. Normand, Datasets for article "Pulsed magnetophononics in gapped quantum magnets", Zenodo, 2025, https://doi.org/10.5281/zenodo.16269926.

Outline

Information

Phys. Rev. B 112, 075112– Published 6 August, 2025
  • Received 23 April 2025
  • Accepted 23 July 2025
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