Ultrafast Reversal of the Ferroelectric Polarization

We report on the demonstration of ultrafast optical reversal of the ferroelectric polarization in ${\mathrm{LiNbO}}_3$. Rather than driving the ferroelectric mode directly, we couple to it indirectly by resonant excitation of an auxiliary high-frequency phonon mode with femtosecond midinfrared pulses. Because of strong anharmonic coupling between these modes, the atoms are directionally displaced along the ferroelectric mode and the polarization is transiently reversed, as revealed by time-resolved, phase-sensitive, second-harmonic generation. This reversal can be induced in both directions, a key prerequisite for practical applications.