Inversion symmetry-breaking-driven charge generation in ferroelectrics upon visible light absorption has become a focal point for light-harvesting applications. Although several light-induced phenomena have been proposed to explain photovoltaic effects in many ferroelectric thin-film systems, photovoltaic mechanisms in ${\mathrm{Bi}}_2{\mathrm{FeCrO}}_6$ (BFCO) films remain elusive. Here, by combining advanced scanning probe techniques capable of locally assessing light-induced charge generation with macroscopic photovoltaic and spectroscopic experiments, we reveal that the photovoltaic effect in this system is strongly influenced by abrupt discontinuities in electronic band structure at the BFCO/substrate interface. In particular, BFCO/Nb-doped ${\mathrm{SrTiO}}_3$ is found to exhibit an interfacial built-in electric field that promotes a dominant p-n junction-like photovoltaic effect, whereas $\mathrm{BFCO}/{\mathrm{La}}_{2/3}{\mathrm{Sr}}_{1/3}{\mathrm{MnO}}_3$ shows no interfacial built-in field, demonstrating instead a bulk photovoltaic effect. These findings suggest that an interfacial electric field can significantly reduce bulk photovoltaic effects. In addition, strong sensitivity to ferroelectric polarization direction is observed, offering a promising approach to controlling photoelectric responses. This study provides clearer insights into the photovoltaic properties of BFCO thin films, suggesting potential applications not only in solar energy harvesting but also in switch-type optoelectronic devices.

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• Electric polarization
• Ferroelectricity
• Optical conductivity
• Optoelectronics
• Photocurrent
• Energy materials
• Ferroelectrics
• Layered semiconductors
• Schottky barriers
• Semiconductor compounds
• Atomic force microscopy
• Epitaxy
• Film deposition