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Nonlinear phononics relies on the resonant optical excitation of infrared-active lattice vibrations to coherently induce targeted structural deformations in solids. This form of dynamical crystal-structure design has been applied to control the functional properties of many interesting systems, including magneto-resistive manganites, magnetic materials, superconductors, and ferroelectrics. However, phononics has so far been restricted to protocols in which structural deformations occur locally within the optically excited volume, sometimes resulting in unwanted heating. Here, we extend nonlinear phononics to propagating polaritons, effectively separating in space the optical drive from the functional response. Mid-infrared optical pulses are used to resonantly drive an 18 THz phonon at the surface of ferroelectric LiNbO3. A time-resolved stimulated Raman scattering probe reveals that the ferroelectric polarization is reduced over the entire 50 micron depth of the sample, far beyond the ~ micron depth of the evanescent phonon field. We attribute the bulk response of the ferroelectric polarization to the excitation of a propagating 2.5 THz soft-mode phonon-polariton. For the highest excitation amplitudes, we reach a regime in which the polarization is reversed. In this this non-perturbative regime, we expect that the polariton model evolves into that of a solitonic domain wall that propagates from the surface into the materials at near the speed of light.
Nonlinear interactions between phonon modes govern the behavior of vibrationally highly excited solids and molecules. Here, we demonstrate theoretically that optical cavities can be used to control the redistribution of energy from a highly excited c
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 pr
We grow accustomed to the notion that optical susceptibilities can be treated as a local property of a medium. In the context of nonlinear optics, both Kerr and Raman processes are considered local, meaning that optical fields at one location do not
Recent years witnessed much broader use of Brillouin inelastic light scattering spectroscopy for the investigation of phonons and magnons in novel materials, nanostructures, and devices. Driven by developments in instrumentation and the strong need f
Photon-phonon coupling holds strong potential for sound and temperature control with light, opening new horizons in detector technology, remote sound generation and signal broadcasting. Here, we report on a novel stereoscopic ultralight converter bas