Depolarization Field-Induced Photovoltaic Effect in Graphene/α-In₂Se₃/Graphene Heterostructures

The ferroelectric photovoltaic effect (FPVE) enables alternate pathways for energy conversion that are not allowed in centrosymmetric materials. Understanding the dominant mechanism of the FPVE at the ultrathin limit is important for defining the ultimate efficiency. In contrast to the wide band gap conventional thin-film ferroelectrics, 2D α-In₂Se₃ has an ideal band gap of 1.3 eV and enables the fabrication of ultrathin and stable heterostructures, providing the perfect platform to explore FPVE in the nanoscale limit. Here, we study the ferroelectric layer thickness-dependent FPVE in vertical few-layer graphene/α-In₂Se₃/graphene heterostructures. We find that the short-circuit photocurrent is antiparallel to the ferroelectric polarization and increases exponentially with decreasing thickness. We show that the observed behavior is predicted by the depolarization field model, originating from the unscreened bound charges due to the finite density of states in semimetal few-layer graphene. As a result, the heterostructures show enhancement of the power conversion efficiency, reaching 2.56 × 10^-3% under 100 W/cm² in 18 nm thick α-In₂Se₃, approximately 275 times more than the 50 nm thick α-In₂Se₃. These results demonstrate the importance of the depolarization field at the nanoscale and define design principles for the potential of harnessing FPVE at reduced dimension.