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Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3

Author

Listed:
  • P. Padmanabhan

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • F. L. Buessen

    (University of Toronto)

  • R. Tutchton

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • K. W. C. Kwock

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory
    Columbia University)

  • S. Gilinsky

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • M. C. Lee

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • M. A. McGuire

    (Materials Science and Technology Division, Oak Ridge National Laboratory)

  • S. R. Singamaneni

    (The University of Texas at El Paso)

  • D. A. Yarotski

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • A. Paramekanti

    (University of Toronto)

  • J.-X. Zhu

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • R. P. Prasankumar

    (Center for Integrated Nanotechnologies, Los Alamos National Laboratory
    Deep Science Fund, Intellectual Ventures)

Abstract

The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI3 is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI3 using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI3 and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

Suggested Citation

  • P. Padmanabhan & F. L. Buessen & R. Tutchton & K. W. C. Kwock & S. Gilinsky & M. C. Lee & M. A. McGuire & S. R. Singamaneni & D. A. Yarotski & A. Paramekanti & J.-X. Zhu & R. P. Prasankumar, 2022. "Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-31786-3
    DOI: 10.1038/s41467-022-31786-3
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    References listed on IDEAS

    as
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