Reversible Optical Control of Polarization in Epitaxial Ferroelectric Thin Films

Abstract Light is an effective tool to probe the polarization and domain distribution in ferroelectric materials passively , that is, non‐invasively, for example, via optical second harmonic generation (SHG). With the emergence of oxide electronics, there is now a strong demand to expand the role of light toward active control of the polarization. In this work, optical control of the ferroelectric polarization is demonstrated in prototypical epitaxial PbZr x Ti 1− x O 3 (PZT)‐based heterostructures. This is accomplished in three steps, using above‐bandgap UV light, while tracking the response of the polarization with optical SHG. First, it is found that UV‐light exposure induces a transient enhancement or suppression of the ferroelectric polarization in films with an upward‐ or downward‐oriented polarization, respectively. This behavior is attributed to a modified charge screening driven by the separation of photoexcited charge carriers at the Schottky interface of the ferroelectric thin film. Second, by taking advantage of this optical handle on electrostatics, remanent optical poling from a pristine multi‐domain into a single‐domain configuration is accomplished. Third, via thermal annealing or engineered electrostatic boundary conditions, a complete reversibility of the optical poling is further achieved. Hence, this work paves the way for the all‐optical control of the spontaneous polarization in ferroelectric thin films.