Phonon-enhanced nonlinearities in hexagonal boron nitride

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 Rubio () and Alexander L. Gaeta ()
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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
Gauri N. Patwardhan: Columbia University, New York
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
Alexander L. Gaeta: Columbia University, New York

Nature Communications, 2023, vol. 14, issue 1, 1-7

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-43501-x

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