Nonlocal nonlinear phononics

Abstract: 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.