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Phonon-enhanced nonlinearities in hexagonal boron nitride

Author

Listed:
  • Jared S. Ginsberg

    (Columbia University, New York)

  • M. Mehdi Jadidi

    (Columbia University, New York)

  • Jin Zhang

    (Max Planck Institute for Structure and Dynamics of Matter and Center for Free-Electron Laser Science)

  • Cecilia Y. Chen

    (Columbia University, New York)

  • Nicolas Tancogne-Dejean

    (Max Planck Institute for Structure and Dynamics of Matter and Center for Free-Electron Laser Science)

  • Sang Hoon Chae

    (Columbia University, New York
    Nanyang Technological University
    Nanyang Technological University)

  • Gauri N. Patwardhan

    (Columbia University, New York
    Cornell University)

  • Lede Xian

    (Max Planck Institute for Structure and Dynamics of Matter and Center for Free-Electron Laser Science)

  • Kenji Watanabe

    (National Institute for Materials Science)

  • Takashi Taniguchi

    (National Institute for Materials Science)

  • James Hone

    (Columbia University, New York)

  • Angel Rubio

    (Max Planck Institute for Structure and Dynamics of Matter and Center for Free-Electron Laser Science
    Simons Foundation Flatiron Institute)

  • Alexander L. Gaeta

    (Columbia University, New York
    Columbia University, New York)

Abstract

Polar crystals can be driven into collective oscillations by optical fields tuned to precise resonance frequencies. As the amplitude of the excited phonon modes increases, novel processes scaling non-linearly with the applied fields begin to contribute to the dynamics of the atomic system. Here we show two such optical nonlinearities that are induced and enhanced by the strong phonon resonance in the van der Waals crystal hexagonal boron nitride (hBN). We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies beyond the third.

Suggested Citation

  • Jared S. Ginsberg & M. Mehdi Jadidi & Jin Zhang & Cecilia Y. Chen & Nicolas Tancogne-Dejean & Sang Hoon Chae & Gauri N. Patwardhan & Lede Xian & Kenji Watanabe & Takashi Taniguchi & James Hone & Angel, 2023. "Phonon-enhanced nonlinearities in hexagonal boron nitride," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43501-x
    DOI: 10.1038/s41467-023-43501-x
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    References listed on IDEAS

    as
    1. A. von Hoegen & R. Mankowsky & M. Fechner & M. Först & A. Cavalleri, 2018. "Probing the interatomic potential of solids with strong-field nonlinear phononics," Nature, Nature, vol. 555(7694), pages 79-82, March.
    2. Ofer Neufeld & Daniel Podolsky & Oren Cohen, 2019. "Floquet group theory and its application to selection rules in harmonic generation," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    3. N. Klemke & N. Tancogne-Dejean & G. M. Rossi & Y. Yang & F. Scheiba & R. E. Mainz & G. Sciacca & A. Rubio & F. X. Kärtner & O. D. Mücke, 2019. "Polarization-state-resolved high-harmonic spectroscopy of solids," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
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