Electric Field‐Manipulated Optical Chirality in Ferroelectric Vortex Domains

Abstract Manipulating optical chirality via electric fields has garnered considerable attention in the realm of both fundamental physics and practical applications. Chiral ferroelectrics, characterized by their inherent optical chirality and switchable spontaneous polarization, are emerging as a promising platform for electronic‐photonic integrated circuits applications. Unlike organics with chiral carbon centers, integrating chirality into technologically mature inorganic ferroelectrics has posed a long‐standing challenge. Here, the successful introduction of chirality is reported into self‐assembly La‐doped BiFeO₃ nanoislands, which exhibit ferroelectric vortex domains. By employing synergistic experimental techniques with piezoresponse force microscopy and nonlinear optical second‐harmonic generation probes, a clear correlation between chirality and polarization configuration within these ferroelectric nanoislands is established. Furthermore, the deterministic control of ferroelectric vortex domains and chirality is demonstrated by applying electric fields, enabling reversible and nonvolatile generation and elimination of optically chiral signals. These findings significantly expand the repertoire of field‐controllable chiral systems and lay the groundwork for the development of innovative ferroelectric optoelectronic devices.