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A coherent phonon-induced hidden quadrupolar ordered state in Ca2RuO4

Author

Listed:
  • Honglie Ning

    (California Institute of Technology
    California Institute of Technology)

  • Omar Mehio

    (California Institute of Technology
    California Institute of Technology)

  • Xinwei Li

    (California Institute of Technology
    California Institute of Technology)

  • Michael Buchhold

    (Universität zu Köln)

  • Mathias Driesse

    (California Institute of Technology
    Humboldt-Universität zu Berlin)

  • Hengdi Zhao

    (University of Colorado)

  • Gang Cao

    (University of Colorado)

  • David Hsieh

    (California Institute of Technology
    California Institute of Technology)

Abstract

Ultrafast laser excitation provides a means to transiently realize long-range ordered electronic states of matter that are hidden in thermal equilibrium. Recently, this approach has unveiled a variety of thermally inaccessible ordered states in strongly correlated materials, including charge density wave, ferroelectric, magnetic, and intertwined charge-orbital ordered states. However, more exotic hidden states exhibiting higher multipolar ordering remain elusive owing to the challenge of directly manipulating and detecting them with light. Here we demonstrate a method to induce a dynamical transition from a thermally allowed to a thermally forbidden spin-orbit entangled quadrupolar ordered state in Ca2RuO4 by coherently exciting a phonon that is strongly coupled to the order parameter. Combining probe photon energy-resolved coherent phonon spectroscopy measurements with model Hamiltonian calculations, we show that the dynamical transition is manifested through anomalies in the temperature, pump excitation fluence, and probe photon energy dependence of the strongly coupled phonon. With this procedure, we introduce a general pathway to uncover hidden multipolar ordered states and to control their re-orientation on ultrashort timescales.

Suggested Citation

  • Honglie Ning & Omar Mehio & Xinwei Li & Michael Buchhold & Mathias Driesse & Hengdi Zhao & Gang Cao & David Hsieh, 2023. "A coherent phonon-induced hidden quadrupolar ordered state in Ca2RuO4," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-44021-4
    DOI: 10.1038/s41467-023-44021-4
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    References listed on IDEAS

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    1. Tianqi Li & Aaron Patz & Leonidas Mouchliadis & Jiaqiang Yan & Thomas A. Lograsso & Ilias E. Perakis & Jigang Wang, 2013. "Femtosecond switching of magnetism via strongly correlated spin–charge quantum excitations," Nature, Nature, vol. 496(7443), pages 69-73, April.
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    3. Jiajun Li & Hugo U. R. Strand & Philipp Werner & Martin Eckstein, 2018. "Theory of photoinduced ultrafast switching to a spin-orbital ordered hidden phase," Nature Communications, Nature, vol. 9(1), pages 1-7, December.
    4. S. Wall & D. Wegkamp & L. Foglia & K. Appavoo & J. Nag & R.F. Haglund & J. Stähler & M. Wolf, 2012. "Ultrafast changes in lattice symmetry probed by coherent phonons," Nature Communications, Nature, vol. 3(1), pages 1-6, January.
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