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Bulk photovoltaic (BPVE) effect in crystals lacking inversion symmetry offersgreat potential for optoelectronic applications due to its unique propertiessuch as above bandgap photovoltage and switchable photocurrent. Because oftheir large spontaneous polarizations, ferroelectric materials are idealplatforms for studying BPVE. However, identifying the origin of experimentallyobserved photovoltaic response is often challenging due to the entanglementbetween bulk and interface effects, leading to much debate in the field. Thisissue is particularly pronounced in vertical heterostructures, where the twoeffects are comparable. Here we report a crossover between bulk- andinterface-dominant response in vertical BiFeO3 heterostructures when changingthe photon energy. We show that well above-bandgap excitation leads to bulkphotovoltaic response, but band-edge excitation requires interface band bendingto separate the photocarriers. Our findings not only help to clarifycontradicting reports in the literature, but also lay the ground for a deeperunderstanding of ferroelectric photovoltaic effect and its applications invarious devices.

Crossover between bulk and interface photovoltaic mechanisms in ferroelectric vertical heterostructure