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Optically-Induced Symmetry Breaking via Nonlinear Phononics

MPS-Authors
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Zhang,  J.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Xian,  L. D.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Tancogne-Dejean,  N.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

/persons/resource/persons22028

Rubio,  A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Center for Computational Quantum Physics, Simons Foundation Flatiron Institute;

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Citation

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.


Cite as: http://hdl.handle.net/21.11116/0000-0008-EDA3-5
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.