Control of up-to-down/down-to-up light-induced ferroelectric polarization reversalElectronic supplementary information (ESI) available: Complementary experiments and summary of the lattice parameters of the characterized samples. See DOI: https://doi.org/10.1039/d2mh00644h

Light control of ferroelectric polarization is of interest for the exploitation of ferroelectric thin films in ultrafast data storage and logic functionalities. The rapidly oscillating electric field of light absorbed in a ferroelectric layer can suppress its polarization but cannot selectively reverse its direction. Here we take advantage of the built-in asymmetry at ferroelectric/electrode interfaces to break the up/down symmetry in uniaxial ferroelectrics to promote polarization reversal under illumination. It is shown that appropriate ferroelectric/metal structures allow the direction of the imprint electric field to be selected, which is instrumental for polarization reversal. This ability is further exploited by demonstrating the optical control of the resistance states in a ferroelectric capacitor.