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  Optically-Induced Symmetry Breaking via Nonlinear Phononics

Ginsberg, J. S., Jadidi, M. M., Zhang, J., Chen, C. Y., Chae, S. H., Patwardhan, G. N., et al. (2021). Optically-Induced Symmetry Breaking via Nonlinear Phononics.

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2107.11959.pdf (Preprint), 2MB
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https://arxiv.org/abs/2107.11959 (Preprint)
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 Creators:
Ginsberg, J. S.1, Author
Jadidi, M. M.1, Author
Zhang, J.2, 3, Author           
Chen, C. Y.4, Author
Chae, S. H.5, Author
Patwardhan, G. N.1, 6, Author
Xian, L. D.2, 3, Author           
Tancogne-Dejean, N.2, 3, Author           
Watanabe, K.7, Author
Taniguchi, T.8, Author
Hone, J.5, Author
Rubio, A.2, 3, 9, Author           
Gaeta, A. L.1, 4, Author
Affiliations:
1Department of Applied Physics and Applied Mathematics, Columbia University, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science, ou_persistent22              
4Department of Electrical Engineering, Columbia University, ou_persistent22              
5Department of Mechanical Engineering, Columbia University, ou_persistent22              
6School of Applied and Engineering Physics, Cornell University, ou_persistent22              
7Research Center for Functional Materials, National Institute for Materials Science, ou_persistent22              
8International Center for Materials Nanoarchitectonics, National Institute for Materials Science, ou_persistent22              
9Center for Computational Quantum Physics, Simons Foundation Flatiron Institute, ou_persistent22              

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Free keywords: Physics, Optics, physics.optics, Condensed Matter, Mesoscale and Nanoscale Physics, cond-mat.mes-hall
 Abstract: Optical nonlinearities in solids reveal information about both the in-plane rotational and out-of-plane inversion symmetries of a crystal. In the van der Waals material hexagonal boron nitride (hBN) both these symmetries and the linear vibrational properties have led to the rich physics of mid-infrared phonon-polaritons. However, the role of strong electron-phonon nonlinearities requires further study. In this work, we investigate both theoretically and experimentally the rich interplay of phonon anharmonicity and symmetry in phonon-polariton mediated nonlinear optics. We show that large enhancements (>30x) of third-harmonic generation occur for incident femtosecond pulses that are resonant with the hBN transverse optical phonons. In addition, we predict and observe large transient sub-picosecond duration second-harmonic signals during resonant excitation, which in equilibrium is forbidden by symmetry. This surprising result indicates that instantaneous crystal inversion symmetry breaking can be optically induced and controlled via phonon interactions by both the power and polarization of the pump laser.

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Language(s): eng - English
 Dates: 2021-07-26
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: No review
 Identifiers: arXiv: 2107.11959
 Degree: -

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