Light‐Induced Reversible Control of Ferroelectric Polarization in BiFeO3

Manipulation of ferroic order parameters, namely (anti‐)ferromagnetic, ferroelectric, and ferroelastic, by light at room temperature is a fascinating topic in modern solid‐state physics due to potential cross‐fertilization in research fields that are largely decoupled. Here, full optical control, that is, reversible switching, of the ferroelectric/ferroelastic domains in BiFeO₃ thin films at room temperature by the mediation of the tip‐enhanced photovoltaic effect is demonstrated. The enhanced short‐circuit photocurrent density at the tip contact area generates a local electric field well exceeding the coercive field, enabling ferroelectric polarization switching. Interestingly, by tailoring the photocurrent direction, via either tuning the illumination geometry or simply rotating the light polarization, full control of the ferroelectric polarization is achieved. The finding offers a new insight into the interactions between light and ferroic orders, enabling fully optical control of all the ferroic orders at room temperature and providing guidance to design novel optoferroic devices for data storage and sensing.